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2026 Volume 37 Issue 7
2026, 37(7): 110975
doi: 10.1016/j.cclet.2025.110975
Abstract:
Synthesis of pseudo-mono-coordinate dysprosium(Ⅲ) single-molecule magnets (SMMs) with strong axiality is challenging. Here, by using very basic alkoxides as axial ligands and ether type neutral ligands as ancillary parts two targeted complexes, [Dy(OtBu)(15-C-5)(THF)2][I3]2 1 and [Dy(1-AdO)(15-C-5)(THF)2][I3]2 2 were successfully isolated. Structurally they possess very short Dy–Oalkoxide bonds (2.016(4) Å for 1 and 2.028(3) Å for 2) and very long Dy–Oether bonds (ranging from 2.427(4) Å to 2.523(4) Å for 1 and 2.416(3) Å to 2.509(3) Å for 2). As such, they are very similar to the diatomic model complex [DyO]+and can be magnetically perceived as pseudo-mono-coordinate Dy(Ⅲ) complexes. Both 1 and 2 exhibit high effective magnetic anisotropy barriers (1054(6) K for 1 and 1028(9) K for 2). Consequently, both 1 and 2 demonstrate high opening hysteresis temperatures, namely 14 K for 1 and 10 K for 2. This study provides a new insight into of pseudo-mono-coordinate mode and further emphasizes the excellent potential of this model for constructing high-performance SMMs.
Synthesis of pseudo-mono-coordinate dysprosium(Ⅲ) single-molecule magnets (SMMs) with strong axiality is challenging. Here, by using very basic alkoxides as axial ligands and ether type neutral ligands as ancillary parts two targeted complexes, [Dy(OtBu)(15-C-5)(THF)2][I3]2 1 and [Dy(1-AdO)(15-C-5)(THF)2][I3]2 2 were successfully isolated. Structurally they possess very short Dy–Oalkoxide bonds (2.016(4) Å for 1 and 2.028(3) Å for 2) and very long Dy–Oether bonds (ranging from 2.427(4) Å to 2.523(4) Å for 1 and 2.416(3) Å to 2.509(3) Å for 2). As such, they are very similar to the diatomic model complex [DyO]+and can be magnetically perceived as pseudo-mono-coordinate Dy(Ⅲ) complexes. Both 1 and 2 exhibit high effective magnetic anisotropy barriers (1054(6) K for 1 and 1028(9) K for 2). Consequently, both 1 and 2 demonstrate high opening hysteresis temperatures, namely 14 K for 1 and 10 K for 2. This study provides a new insight into of pseudo-mono-coordinate mode and further emphasizes the excellent potential of this model for constructing high-performance SMMs.
2026, 37(7): 111037
doi: 10.1016/j.cclet.2025.111037
Abstract:
The design and exploitation of high-property cathode materials and the exploration of their energy storage mechanism have always been research hotspots in the area of zinc-ion hybrid capacitors (ZHCs). In this study, the new RuO2 nanodots/reduced graphene oxide (RuO2 NDs/rGO) composite is designed, and employed as a cathode for ZHC for the first time. Thanks to the synergism of nanoscale design and composite engineering, the RuO2 NDs/rGO//Zn ZHC delivers large specific capacitance (169.5 mAh/g at 0.1 A/g), splendid rate property (74.4 mAh/g at 20 A/g), eminent cyclic property (up to 10,000 cycles), and high energy and power densities (101.7 Wh/kg and 12 kW/kg). Furthermore, systematic kinetic analyses are used to confirm the rapid ion transport kinetics of the RuO2 NDs/rGO//Zn ZHC. More importantly, systematic ex-situ measurements are employed to illustrate its energy storage mechanism of the coexistence of electric double-layer capacitance (physical adsorption/desorption of SO42-) and pseudocapacitance (insertion/extraction of Zn2+ and H+ and chemical adsorption/desorption between Zn2+ and oxygen-containing functional groups). This study not only offers a good strategy for the design and exploitation of high-performance pseudocapacitive cathode for ZHCs, but also proposes an insight into energy storage mechanism of RuO2-based pseudocapacitive cathode.
The design and exploitation of high-property cathode materials and the exploration of their energy storage mechanism have always been research hotspots in the area of zinc-ion hybrid capacitors (ZHCs). In this study, the new RuO2 nanodots/reduced graphene oxide (RuO2 NDs/rGO) composite is designed, and employed as a cathode for ZHC for the first time. Thanks to the synergism of nanoscale design and composite engineering, the RuO2 NDs/rGO//Zn ZHC delivers large specific capacitance (169.5 mAh/g at 0.1 A/g), splendid rate property (74.4 mAh/g at 20 A/g), eminent cyclic property (up to 10,000 cycles), and high energy and power densities (101.7 Wh/kg and 12 kW/kg). Furthermore, systematic kinetic analyses are used to confirm the rapid ion transport kinetics of the RuO2 NDs/rGO//Zn ZHC. More importantly, systematic ex-situ measurements are employed to illustrate its energy storage mechanism of the coexistence of electric double-layer capacitance (physical adsorption/desorption of SO42-) and pseudocapacitance (insertion/extraction of Zn2+ and H+ and chemical adsorption/desorption between Zn2+ and oxygen-containing functional groups). This study not only offers a good strategy for the design and exploitation of high-performance pseudocapacitive cathode for ZHCs, but also proposes an insight into energy storage mechanism of RuO2-based pseudocapacitive cathode.
2026, 37(7): 111079
doi: 10.1016/j.cclet.2025.111079
Abstract:
Ni-rich layered oxides are regarded as one of the most reliable cathode materials for lithium-ion batteries. Modifying the crystal structure through doping with foreign elements and constructing surface coating layers are common modification methods for Ni-rich cathode materials. However, the relationship between the diffusion depth and distribution behavior of foreign elements within the cathode material and the composition of the cathode material has rarely been studied in depth. In this work, by exploring the relationship between element concentration and position in a specially prepared two-substances diffusion couple, the diffusion coefficients between Zr4+ and transition metal elements TMn+ (TM = Ni, Co, Mn; n = 3, 4) were obtained. It was found that the magnitude relationship of their diffusion coefficients is: Zr4+/Mn4+ > Zr4+/Mn3+ > Zr4+/Co3+ > Zr4+/Ni3+. Moreover, through the Arrhenius equation, it was determined that the Zr4+/Mn4+ diffusion couple has the smallest diffusion activation energy of only 0.43 eV, while the Zr4+/Ni3+ diffusion couple has the largest diffusion activation energy, which is 0.63 eV. In addition, this study designed a specific core-shell structure model based on the microscopic morphology of the prepared cathode precursor particles, accurately predicting the distribution differences of Zr4+ in cathode materials with different compositions during the actual sintering process. This work explains the reason for the formation of a Li2ZrO3 secondary phase coating layer on the surface of Ni-rich cathode material particles from the perspective of diffusion kinetics, providing a strong theoretical basis for the future design of high-performance element-modified Ni-rich cathode materials.
Ni-rich layered oxides are regarded as one of the most reliable cathode materials for lithium-ion batteries. Modifying the crystal structure through doping with foreign elements and constructing surface coating layers are common modification methods for Ni-rich cathode materials. However, the relationship between the diffusion depth and distribution behavior of foreign elements within the cathode material and the composition of the cathode material has rarely been studied in depth. In this work, by exploring the relationship between element concentration and position in a specially prepared two-substances diffusion couple, the diffusion coefficients between Zr4+ and transition metal elements TMn+ (TM = Ni, Co, Mn; n = 3, 4) were obtained. It was found that the magnitude relationship of their diffusion coefficients is: Zr4+/Mn4+ > Zr4+/Mn3+ > Zr4+/Co3+ > Zr4+/Ni3+. Moreover, through the Arrhenius equation, it was determined that the Zr4+/Mn4+ diffusion couple has the smallest diffusion activation energy of only 0.43 eV, while the Zr4+/Ni3+ diffusion couple has the largest diffusion activation energy, which is 0.63 eV. In addition, this study designed a specific core-shell structure model based on the microscopic morphology of the prepared cathode precursor particles, accurately predicting the distribution differences of Zr4+ in cathode materials with different compositions during the actual sintering process. This work explains the reason for the formation of a Li2ZrO3 secondary phase coating layer on the surface of Ni-rich cathode material particles from the perspective of diffusion kinetics, providing a strong theoretical basis for the future design of high-performance element-modified Ni-rich cathode materials.
2026, 37(7): 111080
doi: 10.1016/j.cclet.2025.111080
Abstract:
The direct utilization of magnesium (Mg) metal as the anode of Mg batteries is significantly susceptible to passivation in conventional electrolytes, which critically hinders Mg plating and stripping. To address this issue, a synergistic effect of the three-dimensional (3D) scaffolds’ dispersive current strategy and the gradient conductivity artificial layer effectively promotes internal reversible Mg plating and stripping. In this study, we have synthesized 3D magnesiophilic gradient conductivity scaffolds (Sn@Ni), featuring an electronic insulation layer, uniform Mg2+ transport channels, and a high specific surface area, through in situ ion-exchange reactions. It is observed that the plate-like metal chloride insulation provides the necessary potential gradient to prevent electrolyte decomposition and Mg deposition on the surface. Furthermore, the magnesiophilic metal tin (Sn) effectively lowers the nucleation barrier of Mg, enhancing the uniform diffusion of Mg. Additionally, the high specific surface area of the nickel foam skeleton effectively mitigates current density and regulates Mg deposition behavior. As a result, the Sn@Ni 3D gradient conductivity scaffolds exhibit an exceptionally low Mg nucleation overpotential (52 mV) under 500 μA/cm2. Moreover, the Sn@Ni-Mg gradient conductivity anode, produced by plating Mg onto Sn@Ni, demonstrates a symmetric cell capable of sustaining an ultra-long stable reversible cycle exceeding 2800 h (5300 cycles). Full cells with Mo6S8 cathode also show an impressive capacity retention of 95.6% after 500 cycles at 1 C. This breakthrough provides a novel approach to anode design, presenting potential advancements for next-generation Mg batteries.
The direct utilization of magnesium (Mg) metal as the anode of Mg batteries is significantly susceptible to passivation in conventional electrolytes, which critically hinders Mg plating and stripping. To address this issue, a synergistic effect of the three-dimensional (3D) scaffolds’ dispersive current strategy and the gradient conductivity artificial layer effectively promotes internal reversible Mg plating and stripping. In this study, we have synthesized 3D magnesiophilic gradient conductivity scaffolds (Sn@Ni), featuring an electronic insulation layer, uniform Mg2+ transport channels, and a high specific surface area, through in situ ion-exchange reactions. It is observed that the plate-like metal chloride insulation provides the necessary potential gradient to prevent electrolyte decomposition and Mg deposition on the surface. Furthermore, the magnesiophilic metal tin (Sn) effectively lowers the nucleation barrier of Mg, enhancing the uniform diffusion of Mg. Additionally, the high specific surface area of the nickel foam skeleton effectively mitigates current density and regulates Mg deposition behavior. As a result, the Sn@Ni 3D gradient conductivity scaffolds exhibit an exceptionally low Mg nucleation overpotential (52 mV) under 500 μA/cm2. Moreover, the Sn@Ni-Mg gradient conductivity anode, produced by plating Mg onto Sn@Ni, demonstrates a symmetric cell capable of sustaining an ultra-long stable reversible cycle exceeding 2800 h (5300 cycles). Full cells with Mo6S8 cathode also show an impressive capacity retention of 95.6% after 500 cycles at 1 C. This breakthrough provides a novel approach to anode design, presenting potential advancements for next-generation Mg batteries.
2026, 37(7): 111081
doi: 10.1016/j.cclet.2025.111081
Abstract:
perovskite solar cells have attained exceptional power conversion efficiencies, offering a robust material foundation and device design process for the future of photovoltaics. In addition to optimizing perovskite materials for charge-related properties, it is essential to consider spin-related characteristics, as these could prove to be a pivotal factor in enhancing the photoelectric conversion efficiency. In this study, perovskite solar cells featuring various perovskite/transport layer interfaces were engineered to investigate the interfacial spin polarization’s impact on charge extraction. The intensity of charge extraction correlates directly with the interfacial spin polarization. By applying an external electric field, the interfacial spin polarization can be further amplified, thereby enhancing charge extraction. This amplified charge extraction, resulting from increased interfacial spin polarization, can substantially boost the overall photocurrent, thus enabling a high power conversion efficiency.
perovskite solar cells have attained exceptional power conversion efficiencies, offering a robust material foundation and device design process for the future of photovoltaics. In addition to optimizing perovskite materials for charge-related properties, it is essential to consider spin-related characteristics, as these could prove to be a pivotal factor in enhancing the photoelectric conversion efficiency. In this study, perovskite solar cells featuring various perovskite/transport layer interfaces were engineered to investigate the interfacial spin polarization’s impact on charge extraction. The intensity of charge extraction correlates directly with the interfacial spin polarization. By applying an external electric field, the interfacial spin polarization can be further amplified, thereby enhancing charge extraction. This amplified charge extraction, resulting from increased interfacial spin polarization, can substantially boost the overall photocurrent, thus enabling a high power conversion efficiency.
2026, 37(7): 111083
doi: 10.1016/j.cclet.2025.111083
Abstract:
As an indispensable subset of functional materials, quadratic nonlinear optical (NLO) switches have garnered increasing attention owing to their vast potential in next-generation intelligent optoelectronic devices. Despite considerable progress in NLO switches based on solid-state phase transitions, identifying an effective strategy to design high-efficiency NLO switches remains a huge challenge. Herein, we present a molecular engineering approach to develop a high-efficiency lead halide organic-inorganic hybrid NLO switch, (C8H12N)2Pb2Cl6·H2O (NMPTPC). Through the substitution of hydrogen with a methyl group (-CH3) in protonated N-methylaniline, the initial compound (C7H10N)2Pb2Cl6·H2O (NMAPC) transformed into NMPTPC retaining the original space group, which gives rise to a dramatic enhancement of second harmonic generation (SHG) and phase transition temperature. As expected, NMPTPC exhibits high-efficiency modulation of the SHG property (2.6 times that of KH2PO4) and a high phase transition temperature of 372 K. Notably, NMPTPC exhibits a remarkable temperature-dependent SHG behavior, with an impressive "ON/OFF" ratio of approximately 70, underscoring its significant potential as a high-efficient solid-state NLO switch. Based on in-depth crystal structure analysis and theoretical calculations, the modulation of the NLO property is attributed to the asymmetric distortion of the [PbCl6]4− octahedra coupled with π-conjugated aromatic amines with a large dipole moment. This research highlights a promising strategy for advancing the development of high-efficiency NLO switches and provides insights into their applications in next-generation intelligent optoelectronic devices.
As an indispensable subset of functional materials, quadratic nonlinear optical (NLO) switches have garnered increasing attention owing to their vast potential in next-generation intelligent optoelectronic devices. Despite considerable progress in NLO switches based on solid-state phase transitions, identifying an effective strategy to design high-efficiency NLO switches remains a huge challenge. Herein, we present a molecular engineering approach to develop a high-efficiency lead halide organic-inorganic hybrid NLO switch, (C8H12N)2Pb2Cl6·H2O (NMPTPC). Through the substitution of hydrogen with a methyl group (-CH3) in protonated N-methylaniline, the initial compound (C7H10N)2Pb2Cl6·H2O (NMAPC) transformed into NMPTPC retaining the original space group, which gives rise to a dramatic enhancement of second harmonic generation (SHG) and phase transition temperature. As expected, NMPTPC exhibits high-efficiency modulation of the SHG property (2.6 times that of KH2PO4) and a high phase transition temperature of 372 K. Notably, NMPTPC exhibits a remarkable temperature-dependent SHG behavior, with an impressive "ON/OFF" ratio of approximately 70, underscoring its significant potential as a high-efficient solid-state NLO switch. Based on in-depth crystal structure analysis and theoretical calculations, the modulation of the NLO property is attributed to the asymmetric distortion of the [PbCl6]4− octahedra coupled with π-conjugated aromatic amines with a large dipole moment. This research highlights a promising strategy for advancing the development of high-efficiency NLO switches and provides insights into their applications in next-generation intelligent optoelectronic devices.
2026, 37(7): 111110
doi: 10.1016/j.cclet.2025.111110
Abstract:
Poly(ethylene oxide)-based polymer all-solid-state lithium-sulfur batteries (ASSLSBs) have been a prominent direction in new generation of energy storage devices due to their safety, low cost and high specific energy. However, the performance degradation arising from the “shuttle effect” and poor ion transport dynamics limit its further development. Herein, for the first time, we introduce the concepts of adsorption and catalysis into polymer ASSLSBs. By combining S@KB with g-C3N4, the polysulfides shuttling is significantly inhibited. Meanwhile, the kinetic process of the cathode is obviously improved, which is confirmed by in situ electrochemical impedance spectroscopy. The battery with g-C3N4 can provide a high reversible capacity 1078.5 mAh/g, and can be stabilized for 150 cycles with a final Coulombic efficiency of 97.47%, implying a superior electrochemical stability than previously reported. Furthermore, the intrinsic mechanisms of adsorption and catalysis are intensively studied by means of XPS, DFT calculations, and galvanostatic intermittent titration technique. Changes in electrode properties before and after cycling have also been used to study battery stability. Overall, this work will open the door to the novel polymer all-solid-state lithium-sulfur battery design for practical realization of high-energy batteries.
Poly(ethylene oxide)-based polymer all-solid-state lithium-sulfur batteries (ASSLSBs) have been a prominent direction in new generation of energy storage devices due to their safety, low cost and high specific energy. However, the performance degradation arising from the “shuttle effect” and poor ion transport dynamics limit its further development. Herein, for the first time, we introduce the concepts of adsorption and catalysis into polymer ASSLSBs. By combining S@KB with g-C3N4, the polysulfides shuttling is significantly inhibited. Meanwhile, the kinetic process of the cathode is obviously improved, which is confirmed by in situ electrochemical impedance spectroscopy. The battery with g-C3N4 can provide a high reversible capacity 1078.5 mAh/g, and can be stabilized for 150 cycles with a final Coulombic efficiency of 97.47%, implying a superior electrochemical stability than previously reported. Furthermore, the intrinsic mechanisms of adsorption and catalysis are intensively studied by means of XPS, DFT calculations, and galvanostatic intermittent titration technique. Changes in electrode properties before and after cycling have also been used to study battery stability. Overall, this work will open the door to the novel polymer all-solid-state lithium-sulfur battery design for practical realization of high-energy batteries.
2026, 37(7): 111111
doi: 10.1016/j.cclet.2025.111111
Abstract:
Near-infrared (NIR) light offers significant advantages in photocatalytic reactions due to its excellent penetration ability and low phototoxicity. However, the development and utilization of NIR light for efficient photocatalysis continue to encounter several challenges. In this work, we designed and synthesized two stable iron-oxo clusters functionalized with 1, 1-ferrocene dicarboxylic acid (Fcdc), Fe11-Fcdc and BiFe10-Fcdc, both of which can effectively utilize full-spectrum light to realize efficient oxidative coupling reaction of benzylamine (BA) with a product of selectivity over 90% and a conversion up to 97%. Particularly, under the NIR light, Fe11-Fcdc shows significantly better photocatalytic performance (a conversion of 82.3%) than BiFe10-Fcdc (41.0%), which may be responsible for the stronger metal-ligand charge transfer effect in Fe11-Fcdc. This work reports for the first time the study of ferrocene-modified crystalline clusters achieving effective utilization of NIR light.
Near-infrared (NIR) light offers significant advantages in photocatalytic reactions due to its excellent penetration ability and low phototoxicity. However, the development and utilization of NIR light for efficient photocatalysis continue to encounter several challenges. In this work, we designed and synthesized two stable iron-oxo clusters functionalized with 1, 1-ferrocene dicarboxylic acid (Fcdc), Fe11-Fcdc and BiFe10-Fcdc, both of which can effectively utilize full-spectrum light to realize efficient oxidative coupling reaction of benzylamine (BA) with a product of selectivity over 90% and a conversion up to 97%. Particularly, under the NIR light, Fe11-Fcdc shows significantly better photocatalytic performance (a conversion of 82.3%) than BiFe10-Fcdc (41.0%), which may be responsible for the stronger metal-ligand charge transfer effect in Fe11-Fcdc. This work reports for the first time the study of ferrocene-modified crystalline clusters achieving effective utilization of NIR light.
2026, 37(7): 111112
doi: 10.1016/j.cclet.2025.111112
Abstract:
Hard carbon materials are currently the only practical anode materials for commercial sodium-ion battery production, due to their advantages such as high volumetric capacity, low discharge potential, and low production cost. However, hard carbon typically faces issues like low initial Coulombic efficiency (ICE), poor rate performance, and structural instability during cycling, on account of its disordered and porous structure. To address these challenges, this study designs and implements a surface modification strategy to coat hard carbon with a carbon layer derived from the pyrolysis of liquid paraffin. This modified layer significantly reduces the surface defect sites, promotes the ordering of the material's surface structure, and effectively fills the pores of the material. As a result, the ICE of surface-modified hard carbon can be improved from 80% to 90%, with an increased reversible capacity to 310 mAh/g, while also enhancing the rate and cycling performance. This method offers a simple yet efficient approach for structural modification and performance optimization of hard carbon anode materials for developing advanced sodium-ion battery technologies.
Hard carbon materials are currently the only practical anode materials for commercial sodium-ion battery production, due to their advantages such as high volumetric capacity, low discharge potential, and low production cost. However, hard carbon typically faces issues like low initial Coulombic efficiency (ICE), poor rate performance, and structural instability during cycling, on account of its disordered and porous structure. To address these challenges, this study designs and implements a surface modification strategy to coat hard carbon with a carbon layer derived from the pyrolysis of liquid paraffin. This modified layer significantly reduces the surface defect sites, promotes the ordering of the material's surface structure, and effectively fills the pores of the material. As a result, the ICE of surface-modified hard carbon can be improved from 80% to 90%, with an increased reversible capacity to 310 mAh/g, while also enhancing the rate and cycling performance. This method offers a simple yet efficient approach for structural modification and performance optimization of hard carbon anode materials for developing advanced sodium-ion battery technologies.
2026, 37(7): 111113
doi: 10.1016/j.cclet.2025.111113
Abstract:
Argyrodite-based all-solid-state batteries exhibit significant potential as energy storage devices across a wide temperature zone. The Li-ion and electronic conductivities in the cathode mixture is crucial factor in determining the corresponding electrochemical performances. Here, an effective charge carrier distribution is tailored by introducing Li3InCl6 electrolyte with wider voltage stability surrounding the bare LiNi0.7Co0.2Mn0.1O2 to promote ionic conductivity and mixing carbon additives to enhance electronic conductivity. The Li3InCl6@LiNi0.7Co0.2Mn0.1O2/Li5.5PS4.5Cl1.5/Li-In battery exhibits superior electrochemical performance at various C-rates over a wide operating temperature range due to the enhanced charge carrier conducting rates. It delivers high charge/discharge capacities, superior rate capability and exceptional cycling performance. Specifically, the battery delivers initial discharge capacities of 202 mAh/g at 0.2 C and retains a discharge capacity of 162 mAh/g at 2 C with a capacity retention of 91.8% over 500 cycles when cycled at room temperature. Moreover, due to the Li3InCl6 coating layer and the carbon additive in the cathode, it exhibits higher discharge capacities and superior cycling performances when operated at -20 and 60 ℃. This work presents a guideline for fabricating high-performance all-climate solid-state lithium batteries via tailoring the charger carriers conducting pathway in the electrode structure.
Argyrodite-based all-solid-state batteries exhibit significant potential as energy storage devices across a wide temperature zone. The Li-ion and electronic conductivities in the cathode mixture is crucial factor in determining the corresponding electrochemical performances. Here, an effective charge carrier distribution is tailored by introducing Li3InCl6 electrolyte with wider voltage stability surrounding the bare LiNi0.7Co0.2Mn0.1O2 to promote ionic conductivity and mixing carbon additives to enhance electronic conductivity. The Li3InCl6@LiNi0.7Co0.2Mn0.1O2/Li5.5PS4.5Cl1.5/Li-In battery exhibits superior electrochemical performance at various C-rates over a wide operating temperature range due to the enhanced charge carrier conducting rates. It delivers high charge/discharge capacities, superior rate capability and exceptional cycling performance. Specifically, the battery delivers initial discharge capacities of 202 mAh/g at 0.2 C and retains a discharge capacity of 162 mAh/g at 2 C with a capacity retention of 91.8% over 500 cycles when cycled at room temperature. Moreover, due to the Li3InCl6 coating layer and the carbon additive in the cathode, it exhibits higher discharge capacities and superior cycling performances when operated at -20 and 60 ℃. This work presents a guideline for fabricating high-performance all-climate solid-state lithium batteries via tailoring the charger carriers conducting pathway in the electrode structure.
Reviving the ionic conductivity of air-instable solid-state electrolytes via a facile heat treatment
2026, 37(7): 111114
doi: 10.1016/j.cclet.2025.111114
Abstract:
The quest for sustainable and efficient energy storage solutions has led to significant advancements in the field of solid-state batteries, with a particular focus on solid-state electrolytes (SSEs) especially highly ionic conductive sulfide and halide materials. However, the air instability of these SSEs not only limits their mass production but also poses environmental and safety risks. Herein, the damage of humid-air exposure on the structure and electrochemical properties of Li5.5PS4.5Cl0.8Br0.7 and Li3InCl6 is evaluated, and a subsequent heat treatment is proposed and proven effective to recover the damage, whose mechanisms are pinpointed through XRD data with Retvield refinement. For the exposed samples, a lattice contraction occurs as the hydrolysis reaction caused by H2O from humid air severely damages the structure, which impedes lithium-ion transport. After heat treatment, a lattice rearrangement can rebuild sufficient lithium-ion pathway in the material, leading to the greatly improved ionic conductivity. As a result, the treated electrolytes provide greatly promoted ionic conductivity (from 0.95 mS/cm to 1.8 mS/cm for Li3InCl6, from 1.24 S/cm to 7.04 S/cm for Li5.5PS4.5Cl0.8Br0.7). More importantly, ASSBs employed with the treated electrolytes achieve outstanding long-term cycling and rate performance, even guarantee considerable capacity output of ~217 and ~159 mAh/g under extreme conditions of 60 and –20 ℃, illustrating significantly improved electrochemical reaction kinetics and the impressive reliability of the heat treatment method.
The quest for sustainable and efficient energy storage solutions has led to significant advancements in the field of solid-state batteries, with a particular focus on solid-state electrolytes (SSEs) especially highly ionic conductive sulfide and halide materials. However, the air instability of these SSEs not only limits their mass production but also poses environmental and safety risks. Herein, the damage of humid-air exposure on the structure and electrochemical properties of Li5.5PS4.5Cl0.8Br0.7 and Li3InCl6 is evaluated, and a subsequent heat treatment is proposed and proven effective to recover the damage, whose mechanisms are pinpointed through XRD data with Retvield refinement. For the exposed samples, a lattice contraction occurs as the hydrolysis reaction caused by H2O from humid air severely damages the structure, which impedes lithium-ion transport. After heat treatment, a lattice rearrangement can rebuild sufficient lithium-ion pathway in the material, leading to the greatly improved ionic conductivity. As a result, the treated electrolytes provide greatly promoted ionic conductivity (from 0.95 mS/cm to 1.8 mS/cm for Li3InCl6, from 1.24 S/cm to 7.04 S/cm for Li5.5PS4.5Cl0.8Br0.7). More importantly, ASSBs employed with the treated electrolytes achieve outstanding long-term cycling and rate performance, even guarantee considerable capacity output of ~217 and ~159 mAh/g under extreme conditions of 60 and –20 ℃, illustrating significantly improved electrochemical reaction kinetics and the impressive reliability of the heat treatment method.
2026, 37(7): 111115
doi: 10.1016/j.cclet.2025.111115
Abstract:
The development of photosynthetic biological systems (PBSs) presents a promising approach to mitigating global climate change. However, the practical application of PBSs remains hindered by their low product yields. Key determinants of production efficiency include light utilization, electron transfer efficiency, and catalyst stability. To address these challenges, we developed a high-performance Cupriavidus necator/CdS@Au@Poly dimethyl diallyl ammonium chloride (C. necator/CdS@Au@PDDA) biohybrid system for the photocatalytic conversion of CO2 into bioplastic poly(3-hydroxybutyrate) (PHB). The incorporation of Au nanoclusters extends the visible light absorption range and alleviates photocorrosion of CdS, while the PDDA modification enhances electron transfer rates and enables the material to firmly adhere to the bacterial surface. In situ H2 production by CdS@Au@PDDA drives CO2 fixation through bacterial metabolic pathways, achieving a quantum efficiency of 2.76% ± 0.22% and a maximum PHB yield of 53.6 ± 5.2 mg/L, representing the highest yield reported for C. necator-based artificial PBSs. This biohybrid system demonstrates the effective integration of advanced nanomaterials with microbial processes, offering a robust platform for sustainable bioplastic production through carbon-neutral artificial photosynthesis technology and providing a novel perspective for addressing the global challenge of microplastic pollution.
The development of photosynthetic biological systems (PBSs) presents a promising approach to mitigating global climate change. However, the practical application of PBSs remains hindered by their low product yields. Key determinants of production efficiency include light utilization, electron transfer efficiency, and catalyst stability. To address these challenges, we developed a high-performance Cupriavidus necator/CdS@Au@Poly dimethyl diallyl ammonium chloride (C. necator/CdS@Au@PDDA) biohybrid system for the photocatalytic conversion of CO2 into bioplastic poly(3-hydroxybutyrate) (PHB). The incorporation of Au nanoclusters extends the visible light absorption range and alleviates photocorrosion of CdS, while the PDDA modification enhances electron transfer rates and enables the material to firmly adhere to the bacterial surface. In situ H2 production by CdS@Au@PDDA drives CO2 fixation through bacterial metabolic pathways, achieving a quantum efficiency of 2.76% ± 0.22% and a maximum PHB yield of 53.6 ± 5.2 mg/L, representing the highest yield reported for C. necator-based artificial PBSs. This biohybrid system demonstrates the effective integration of advanced nanomaterials with microbial processes, offering a robust platform for sustainable bioplastic production through carbon-neutral artificial photosynthesis technology and providing a novel perspective for addressing the global challenge of microplastic pollution.
2026, 37(7): 111124
doi: 10.1016/j.cclet.2025.111124
Abstract:
The disordered structure plays an essential role in high capacity of hard carbon. However, the lack of universal descriptor for characterizing the structural disorder of hard carbon limit advancements in understanding and optimizing its sodium diffusion performance in sodium ion batteries (SIBs). Herein, fractal dimension (D) revealed by small angle X-ray scattering (SAXS) is identified as a descriptor of hard carbon’s structural disorder under the data-driven methods, correlating it with electrochemical and structural features. Porod’s law, TEM and XRD are used to determine the correlation between D and the microstructure of hard carbon. The results reveal that as D increases, pseudo-graphitic domains decrease and carbon layers become more curved, which result in more closed pores. Meanwhile, the diffusion coefficient in different potential below 0.1 V vs. Na+/Na suggest that D are unfavorable to sodium ions diffusion as the diffusion coefficients decrease with D increase and result in a reduce of slope capacity percentage in SIBs. D are used in analyze the sodium ion storage behavior by ex-situ SAXS, which suggests that carbon layers with larger D have more structural defects as nucleation sites. In addition, theoretical plateau capacity utilization (TCU) is proposed based on D and reveal the accessibility of closed pore of hard carbon. This work provides a foundation for bridging the gap between structural characterization and practical performances, and guiding the structural design of hard carbon with high sodium storage and kinetic performance.
The disordered structure plays an essential role in high capacity of hard carbon. However, the lack of universal descriptor for characterizing the structural disorder of hard carbon limit advancements in understanding and optimizing its sodium diffusion performance in sodium ion batteries (SIBs). Herein, fractal dimension (D) revealed by small angle X-ray scattering (SAXS) is identified as a descriptor of hard carbon’s structural disorder under the data-driven methods, correlating it with electrochemical and structural features. Porod’s law, TEM and XRD are used to determine the correlation between D and the microstructure of hard carbon. The results reveal that as D increases, pseudo-graphitic domains decrease and carbon layers become more curved, which result in more closed pores. Meanwhile, the diffusion coefficient in different potential below 0.1 V vs. Na+/Na suggest that D are unfavorable to sodium ions diffusion as the diffusion coefficients decrease with D increase and result in a reduce of slope capacity percentage in SIBs. D are used in analyze the sodium ion storage behavior by ex-situ SAXS, which suggests that carbon layers with larger D have more structural defects as nucleation sites. In addition, theoretical plateau capacity utilization (TCU) is proposed based on D and reveal the accessibility of closed pore of hard carbon. This work provides a foundation for bridging the gap between structural characterization and practical performances, and guiding the structural design of hard carbon with high sodium storage and kinetic performance.
2026, 37(7): 111125
doi: 10.1016/j.cclet.2025.111125
Abstract:
Silicon/graphite (Si/C) composites, which combine the advantages of Si anodes and commercial graphite anodes, are promising anode materials for high-energy-density lithium-ion batteries (LIBs). Despite experimental and theoretical studies on the electrochemical characteristics of different silicon crystal surfaces, there have been limited investigations on the electrochemical and mechanical properties of Si composite anode materials with different graphite crystal planes, such as the electrode interfaces between Si(111) and graphite (0001), as well as amorphous Si and graphite (1010). In this study, models of Si/C anode interfaces for LIBs were constructed to explore the mechanical-electrochemical-low-temperature performance by density functional theory (DFT) calculations and ab initio molecular dynamics (AIMD) simulations. The calculation results indicate that upon Li intercalation into the graphite (1010) surface, the electrical conductivity, electrochemical adsorption, and interfacial mechanical strength of the Si/C composite are significantly enhanced, with a separation work that is 2.3 times higher than that of Si/C on the graphite (0001) surface. More importantly, AIMD simulations at low temperatures reveal that the interface between graphite (1010) and amorphous Si forms a solid electrolyte interphase (SEI) rich in organic components, which significantly improves the Li-diffusion kinetics. This discovery provides new insights for the design and optimization of Si/C anode materials for low-temperature LIBs.
Silicon/graphite (Si/C) composites, which combine the advantages of Si anodes and commercial graphite anodes, are promising anode materials for high-energy-density lithium-ion batteries (LIBs). Despite experimental and theoretical studies on the electrochemical characteristics of different silicon crystal surfaces, there have been limited investigations on the electrochemical and mechanical properties of Si composite anode materials with different graphite crystal planes, such as the electrode interfaces between Si(111) and graphite (0001), as well as amorphous Si and graphite (1010). In this study, models of Si/C anode interfaces for LIBs were constructed to explore the mechanical-electrochemical-low-temperature performance by density functional theory (DFT) calculations and ab initio molecular dynamics (AIMD) simulations. The calculation results indicate that upon Li intercalation into the graphite (1010) surface, the electrical conductivity, electrochemical adsorption, and interfacial mechanical strength of the Si/C composite are significantly enhanced, with a separation work that is 2.3 times higher than that of Si/C on the graphite (0001) surface. More importantly, AIMD simulations at low temperatures reveal that the interface between graphite (1010) and amorphous Si forms a solid electrolyte interphase (SEI) rich in organic components, which significantly improves the Li-diffusion kinetics. This discovery provides new insights for the design and optimization of Si/C anode materials for low-temperature LIBs.
2026, 37(7): 111126
doi: 10.1016/j.cclet.2025.111126
Abstract:
The oxidative coupling reaction of methane (OCM) process offers a promising pathway for the direct conversion of methane into high value C2 hydrocarbons (C2H6 and C2H4), albeit facing the challenges of harsh reaction conditions and competing overoxidation reaction. Herein, Ba-doped Eu2O3 synthesized via the spray pyrolysis method was employed as highly active dopant catalyst for the methane oxidative coupling reaction. The prepared Eu0.9Ba0.1Ox catalyst showed satisfactory reactivity and stability, with a C2+ product selectivity of 52.4%, a C2+ yield of 16.2%, and a stabilization time of at least 100 h. The incorporation of Ba atoms into Eu2O3 lattice leads to an increased molar ratio of Eu2+/Eu3+ and a higher oxygen vacancies (Ov) concentration. Such modulation of surface electronic state significantly improves the adsorption and activation behavior of oxygen, thereby accelerating the production of reactive oxygen species (O2−). Meanwhile, the acid-base properties of Eu2O3 substrate also undergo obvious alteration with more basic site generation after Ba doping, which is conducive to the stabilization activated oxygen. O2− substances can promote the activation of methane into methyl radicals, and also facilitate the dehydrogenation of ethane into ethylene, thus improving the catalytic activity.
The oxidative coupling reaction of methane (OCM) process offers a promising pathway for the direct conversion of methane into high value C2 hydrocarbons (C2H6 and C2H4), albeit facing the challenges of harsh reaction conditions and competing overoxidation reaction. Herein, Ba-doped Eu2O3 synthesized via the spray pyrolysis method was employed as highly active dopant catalyst for the methane oxidative coupling reaction. The prepared Eu0.9Ba0.1Ox catalyst showed satisfactory reactivity and stability, with a C2+ product selectivity of 52.4%, a C2+ yield of 16.2%, and a stabilization time of at least 100 h. The incorporation of Ba atoms into Eu2O3 lattice leads to an increased molar ratio of Eu2+/Eu3+ and a higher oxygen vacancies (Ov) concentration. Such modulation of surface electronic state significantly improves the adsorption and activation behavior of oxygen, thereby accelerating the production of reactive oxygen species (O2−). Meanwhile, the acid-base properties of Eu2O3 substrate also undergo obvious alteration with more basic site generation after Ba doping, which is conducive to the stabilization activated oxygen. O2− substances can promote the activation of methane into methyl radicals, and also facilitate the dehydrogenation of ethane into ethylene, thus improving the catalytic activity.
2026, 37(7): 111127
doi: 10.1016/j.cclet.2025.111127
Abstract:
Lithium plating and gas evolution during fast charging of graphite-based lithium-ion batteries (LIBs) are among the pivotal challenges contributing to rapid capacity loss. However, the mechanisms underlying gas generation and corresponding mitigation strategies in electrolytes comprising mixed organic molecules and Li salts remain underexplored. Herein, we employed first-principles studies to simulate the lithiation process of electrolytes and predicted gas formation at anode interfaces with Li plating. Our results emphasize the critical role of Li salts in initiating solvent molecule decomposition and the exacerbation of interfacial degradation under conditions of elevated temperature and prolonged annealing, giving rise to the production of CO, C2H4, CH4, and H2, along with a significant increase in SEI's electronic conductivity. Moreover, our computations highlight that ethylene carbonate (EC) in commercial electrolytes is the overarching cause of interface instability and gas evolution. Experimental validations demonstrate that reducing the EC content in electrolytes results in an enhancement of the specific capacity of LiNi0.8Co0.1Mn0.1O2graphite full cells from 158.13 mAh/g to 182.53 mAh/g, and an improvement in capacity retention from 72.0% to 80.4% over 130 cycling at 3 C. This research provides a theoretical framework for designing fast-charging electrolytes with stable interfaces and minimal gas generation.
Lithium plating and gas evolution during fast charging of graphite-based lithium-ion batteries (LIBs) are among the pivotal challenges contributing to rapid capacity loss. However, the mechanisms underlying gas generation and corresponding mitigation strategies in electrolytes comprising mixed organic molecules and Li salts remain underexplored. Herein, we employed first-principles studies to simulate the lithiation process of electrolytes and predicted gas formation at anode interfaces with Li plating. Our results emphasize the critical role of Li salts in initiating solvent molecule decomposition and the exacerbation of interfacial degradation under conditions of elevated temperature and prolonged annealing, giving rise to the production of CO, C2H4, CH4, and H2, along with a significant increase in SEI's electronic conductivity. Moreover, our computations highlight that ethylene carbonate (EC) in commercial electrolytes is the overarching cause of interface instability and gas evolution. Experimental validations demonstrate that reducing the EC content in electrolytes results in an enhancement of the specific capacity of LiNi0.8Co0.1Mn0.1O2graphite full cells from 158.13 mAh/g to 182.53 mAh/g, and an improvement in capacity retention from 72.0% to 80.4% over 130 cycling at 3 C. This research provides a theoretical framework for designing fast-charging electrolytes with stable interfaces and minimal gas generation.
2026, 37(7): 111156
doi: 10.1016/j.cclet.2025.111156
Abstract:
Hard carbon with abundant resources and superior sodium storage performance is the most representative anode material for sodium-ion batteries (SIBs), but suffers from unsatisfied reversible capacity and low initial Coulombic efficiency. Herein, brown coal is employed as the precursor to obtain high-performance hard carbon anode materials with the assistance of pre-oxidation treatment for SIBs. The unique pre-oxidation treatment introduces an abundance of oxygen-containing functional groups to regulate the microstructure of hard carbon anode, achieving a more disordered phase structure for improved sodium storage performance. These enable a high reversible specific capacity of 316.1 mAh/g with an initial Coulombic efficiency of 87.6%, significantly higher than those of 236.5 mAh/g and 71.7% in carbonized pristine brown coal. Meanwhile, the adsorption-insertion-pore filling sodium storage mechanism of brown coal-derived hard carbon is demonstrated by in-situ XRD and Raman. This work emphasizes the role of pre-oxidation treatment on boosting the sodium storage performance of brown coal-derived hard carbon for advanced SIBs.
Hard carbon with abundant resources and superior sodium storage performance is the most representative anode material for sodium-ion batteries (SIBs), but suffers from unsatisfied reversible capacity and low initial Coulombic efficiency. Herein, brown coal is employed as the precursor to obtain high-performance hard carbon anode materials with the assistance of pre-oxidation treatment for SIBs. The unique pre-oxidation treatment introduces an abundance of oxygen-containing functional groups to regulate the microstructure of hard carbon anode, achieving a more disordered phase structure for improved sodium storage performance. These enable a high reversible specific capacity of 316.1 mAh/g with an initial Coulombic efficiency of 87.6%, significantly higher than those of 236.5 mAh/g and 71.7% in carbonized pristine brown coal. Meanwhile, the adsorption-insertion-pore filling sodium storage mechanism of brown coal-derived hard carbon is demonstrated by in-situ XRD and Raman. This work emphasizes the role of pre-oxidation treatment on boosting the sodium storage performance of brown coal-derived hard carbon for advanced SIBs.
2026, 37(7): 111157
doi: 10.1016/j.cclet.2025.111157
Abstract:
The combination of high-nickel cathodes with poly(ethylene oxide) (PEO)-based solid-state electrolytes represents a promising strategy to achieve both high energy density and enhanced safety. However, existing studies predominantly employ LiFePO4 cathodes due to the inherent limitations of PEO-based electrolytes in high-voltage stability. Even with the improved electrochemical stability window (ESW) of PEO-based electrolytes, current implementations still utilize low-nickel-content (≤80%) cathodes. To further enhance the energy density of PEO-based solid-state batteries (SSBs), this work employs high-nickel-content (> 80%) cathodes in conjunction with PEO-based electrolytes. The influence of nickel content in cathode materials (CAMs) on the electrochemical performance of PEO-based SSBs is systematically investigated through a progressive nickel content optimization approach. This study elucidates the intrinsic relationship between the nickel content and the characteristic capacity activation mechanism observed during the initial cycling phases in solid-state battery systems, revealing a nickel-content-dependent electrochemical activation pattern unique to solid-state configurations. Additionally, through a series of detection schemes, the failure mechanism of high-nickel PEO-based SSBs is systematically studied from the cathode/electrolyte interface, electrolyte, and CAM. Particularly, the degree of PEO decomposition is quantitatively analyzed using differential electrochemical mass spectrometry (DEMS) and gel permeation chromatography (GPC). This work reveals the key issues faced when further increasing the nickel content of CAMs, providing insights for targeted modification designs of high-nickel PEO-based solid-state batteries in the future.
The combination of high-nickel cathodes with poly(ethylene oxide) (PEO)-based solid-state electrolytes represents a promising strategy to achieve both high energy density and enhanced safety. However, existing studies predominantly employ LiFePO4 cathodes due to the inherent limitations of PEO-based electrolytes in high-voltage stability. Even with the improved electrochemical stability window (ESW) of PEO-based electrolytes, current implementations still utilize low-nickel-content (≤80%) cathodes. To further enhance the energy density of PEO-based solid-state batteries (SSBs), this work employs high-nickel-content (> 80%) cathodes in conjunction with PEO-based electrolytes. The influence of nickel content in cathode materials (CAMs) on the electrochemical performance of PEO-based SSBs is systematically investigated through a progressive nickel content optimization approach. This study elucidates the intrinsic relationship between the nickel content and the characteristic capacity activation mechanism observed during the initial cycling phases in solid-state battery systems, revealing a nickel-content-dependent electrochemical activation pattern unique to solid-state configurations. Additionally, through a series of detection schemes, the failure mechanism of high-nickel PEO-based SSBs is systematically studied from the cathode/electrolyte interface, electrolyte, and CAM. Particularly, the degree of PEO decomposition is quantitatively analyzed using differential electrochemical mass spectrometry (DEMS) and gel permeation chromatography (GPC). This work reveals the key issues faced when further increasing the nickel content of CAMs, providing insights for targeted modification designs of high-nickel PEO-based solid-state batteries in the future.
2026, 37(7): 111159
doi: 10.1016/j.cclet.2025.111159
Abstract:
Upconversion nanoparticles (UCNPs) have been naturally entangled with surface phonons since their discovery due to their high specific surface area. However, in addition to quenching luminescence at ambient temperatures, surface phonons play a crucial role in activating the dark layer between the sensitizer and the activator to enhance luminescence in thermal environments. Considering that the positive effect of surface phonons may be eliminated under inert cladding, a β-NaGdF4:Yb,Tm@NaYF4@NaGdF4:Yb,Er core-shell-shell upconversion luminescence (UCL) system with two opposite thermo-responsive luminescence behaviors is designed here. The imposition of an inert intermediate shell layer causes the weakening of the blue luminescence of the core Tm ions in the thermal environment, while on the contrary the outermost Er ions realize an effective enhancement of luminescence with the help of surface phonons. In addition, the photoluminescence results show that effective modulation of luminescence color can be achieved by changing the thickness of the inert shell layer, the concentration of Er ions in the activation layer, and the excitation power. Finally, the distinct thermally responsive luminescence behaviors and temperature-dependent color variations enabled moderate temperature sensing and information encryption applications. The maximum relative and absolute sensitivities can be up to 1.62%/K and 0.64%/K from 298 K to 573 K, respectively. These findings provided new insights into optimizing the luminescent properties of fluorides and provided a new platform for the application of multiple properties in a material.
Upconversion nanoparticles (UCNPs) have been naturally entangled with surface phonons since their discovery due to their high specific surface area. However, in addition to quenching luminescence at ambient temperatures, surface phonons play a crucial role in activating the dark layer between the sensitizer and the activator to enhance luminescence in thermal environments. Considering that the positive effect of surface phonons may be eliminated under inert cladding, a β-NaGdF4:Yb,Tm@NaYF4@NaGdF4:Yb,Er core-shell-shell upconversion luminescence (UCL) system with two opposite thermo-responsive luminescence behaviors is designed here. The imposition of an inert intermediate shell layer causes the weakening of the blue luminescence of the core Tm ions in the thermal environment, while on the contrary the outermost Er ions realize an effective enhancement of luminescence with the help of surface phonons. In addition, the photoluminescence results show that effective modulation of luminescence color can be achieved by changing the thickness of the inert shell layer, the concentration of Er ions in the activation layer, and the excitation power. Finally, the distinct thermally responsive luminescence behaviors and temperature-dependent color variations enabled moderate temperature sensing and information encryption applications. The maximum relative and absolute sensitivities can be up to 1.62%/K and 0.64%/K from 298 K to 573 K, respectively. These findings provided new insights into optimizing the luminescent properties of fluorides and provided a new platform for the application of multiple properties in a material.
2026, 37(7): 111176
doi: 10.1016/j.cclet.2025.111176
Abstract:
Chiral hybrid metal halides, known for their exceptional piezoelectric properties, facile synthesis, and design flexibility, have become promising candidates for advanced piezoelectric devices. However, most chiral metal halides contain toxic lead and are predominantly restricted to 1D or 2D structures. In contrast, 0D hybrid piezoelectric materials, despite their lower elastic moduli, remain significantly less explored. Here, we report the synthesis of a pair of lead-free chiral 0D hybrid metal halides, R-(APP)2CoBr4 and S-(APP)2CoBr4 (APP = 2-amino-3-phenylpropan-1-ol). First-principles calculations reveal that S-(APP)2CoBr4 exhibits a noticeable shear piezoelectric coefficient while maintaining a relatively low elastic modulus. Furthermore, S-(APP)2CoBr4/PDMS composite films (PDMS = polydimethylsiloxane) were fabricated and their potential for energy harvesting and human motion sensing was investigated. Under a 2 N applied force, a 15 wt% S-(APP)2CoBr4/PDMS composite film exhibits promising performance, generating an open-circuit voltage of 10.21 V and a short-circuit current of 1.02 µA. Additionally, the low acoustic impedance of S-(APP)2CoBr4 (5.80–6.67 MRayl) and its compatibility with water (1.5 MRayl) facilitate efficient ultrasound transmission in composite devices, ensuring precise localization of ultrasound sources. These findings offer valuable insights into the potential of lead-free 0D hybrid metal halides for advanced electromechanical applications.
Chiral hybrid metal halides, known for their exceptional piezoelectric properties, facile synthesis, and design flexibility, have become promising candidates for advanced piezoelectric devices. However, most chiral metal halides contain toxic lead and are predominantly restricted to 1D or 2D structures. In contrast, 0D hybrid piezoelectric materials, despite their lower elastic moduli, remain significantly less explored. Here, we report the synthesis of a pair of lead-free chiral 0D hybrid metal halides, R-(APP)2CoBr4 and S-(APP)2CoBr4 (APP = 2-amino-3-phenylpropan-1-ol). First-principles calculations reveal that S-(APP)2CoBr4 exhibits a noticeable shear piezoelectric coefficient while maintaining a relatively low elastic modulus. Furthermore, S-(APP)2CoBr4/PDMS composite films (PDMS = polydimethylsiloxane) were fabricated and their potential for energy harvesting and human motion sensing was investigated. Under a 2 N applied force, a 15 wt% S-(APP)2CoBr4/PDMS composite film exhibits promising performance, generating an open-circuit voltage of 10.21 V and a short-circuit current of 1.02 µA. Additionally, the low acoustic impedance of S-(APP)2CoBr4 (5.80–6.67 MRayl) and its compatibility with water (1.5 MRayl) facilitate efficient ultrasound transmission in composite devices, ensuring precise localization of ultrasound sources. These findings offer valuable insights into the potential of lead-free 0D hybrid metal halides for advanced electromechanical applications.
2026, 37(7): 111330
doi: 10.1016/j.cclet.2025.111330
Abstract:
Lithium–sulfur (Li–S) battery is considered as a promising next-generation high-energy-density battery. However, the cycle life of Li–S batteries is severely plagued by the instability of Li metal anodes. Improving Li deposition uniformity can mitigate the formation of inactive Li and the side reactions between Li polysulfides and Li metal anodes. Herein, 1-methyl-1-propylpyrrolidinium bis(fluorosulfonyl)imide (Py13FSI) is proposed as an additive to improve the uniformity of Li deposition in Li–S batteries. At a low concentration, Py13+ exhibits a lower reduction potential than Li ions. Py13+ can be adsorbed and accumulate on the surface protuberances of Li metal anodes, inducing the deposition of Li towards non-tip sites and improving the uniformity of Li deposition. With a high-loading cathode (4.1 mgS/cm2) and an ultrathin Li metal anode (50 µm), the cycle life of Li–S batteries is prolonged from 61 to 120 cycles via Py13FSI additives. Furthermore, a 401 Wh/kg Li–S pouch cell with Py13FSI additives undergoes 14 cycles. This work demonstrates the potential of improving Li deposition uniformity in Li–S batteries by appropriate electrolyte additives.
Lithium–sulfur (Li–S) battery is considered as a promising next-generation high-energy-density battery. However, the cycle life of Li–S batteries is severely plagued by the instability of Li metal anodes. Improving Li deposition uniformity can mitigate the formation of inactive Li and the side reactions between Li polysulfides and Li metal anodes. Herein, 1-methyl-1-propylpyrrolidinium bis(fluorosulfonyl)imide (Py13FSI) is proposed as an additive to improve the uniformity of Li deposition in Li–S batteries. At a low concentration, Py13+ exhibits a lower reduction potential than Li ions. Py13+ can be adsorbed and accumulate on the surface protuberances of Li metal anodes, inducing the deposition of Li towards non-tip sites and improving the uniformity of Li deposition. With a high-loading cathode (4.1 mgS/cm2) and an ultrathin Li metal anode (50 µm), the cycle life of Li–S batteries is prolonged from 61 to 120 cycles via Py13FSI additives. Furthermore, a 401 Wh/kg Li–S pouch cell with Py13FSI additives undergoes 14 cycles. This work demonstrates the potential of improving Li deposition uniformity in Li–S batteries by appropriate electrolyte additives.
2026, 37(7): 111584
doi: 10.1016/j.cclet.2025.111584
Abstract:
A series of highly rearranged labdane diterpenoids featuring previously unreported skeletons, including 9,18-cyclolabdanes (1 and 2), 1,10-seco-9,18-cyclolabdanes (3–5), 7,18-cyclolabdanes (6), and 1,10-seco-1,5-cyclolabdanes (7), along with seven novel labdanes (8–14), two novel halimane diterpenoids (15 and 16), and three known congeners (17–19), were isolated from Chinese liverwort Haplomitrium mnioides. Their structures were unequivocally determined through comprehensive spectroscopic analysis, single-crystal X-ray diffraction and electronic circular dichroism (ECD) calculations. These diverse diterpenoids were biosynthesized through an aldol-type cascade process, using 19 as the starting material, distinguishing them from compounds generated via conventional carbocation rearrangement. Anti-inflammatory assays revealed that haploide O (15) and haplomitrenolide C (17) significantly inhibited the secretion of proinflammatory cytokines interferon-γ (IFN-γ), tumor necrosis factor-α (TNF-α), and interleukin-6 (IL-6) in vitro in concanavalin A (ConA)-induced murine spleen cells.
A series of highly rearranged labdane diterpenoids featuring previously unreported skeletons, including 9,18-cyclolabdanes (1 and 2), 1,10-seco-9,18-cyclolabdanes (3–5), 7,18-cyclolabdanes (6), and 1,10-seco-1,5-cyclolabdanes (7), along with seven novel labdanes (8–14), two novel halimane diterpenoids (15 and 16), and three known congeners (17–19), were isolated from Chinese liverwort Haplomitrium mnioides. Their structures were unequivocally determined through comprehensive spectroscopic analysis, single-crystal X-ray diffraction and electronic circular dichroism (ECD) calculations. These diverse diterpenoids were biosynthesized through an aldol-type cascade process, using 19 as the starting material, distinguishing them from compounds generated via conventional carbocation rearrangement. Anti-inflammatory assays revealed that haploide O (15) and haplomitrenolide C (17) significantly inhibited the secretion of proinflammatory cytokines interferon-γ (IFN-γ), tumor necrosis factor-α (TNF-α), and interleukin-6 (IL-6) in vitro in concanavalin A (ConA)-induced murine spleen cells.
2026, 37(7): 111585
doi: 10.1016/j.cclet.2025.111585
Abstract:
The application of Arsenic trioxide (ATO) has greatly improved the cure rates in patients with acute promyelocytic leukemia (APL) and has shown therapeutic effects in other leukemia types, as evidenced by an increasing number of preclinical trials. However, its clinical application is still limited due to a lack of understanding of the underlying mechanisms. In this report, we have demonstrated that ATO can induce pyroptosis and release damage-associated molecular patterns (DAMPs), such as high mobility group box 1 (HMGB1) and interleukin-1β (IL-1β). DAMPs can activate the immunogenic cell death (ICD) mechanism. Our study elucidated the pivotal role of pyroptosis and demonstrated the activation of the caspase-3/gasdermin E (GSDME) pathway both in vivo and in vitro upon ATO intervention. Proteomic analysis of cell supernatants revealed the release of the ICD-associated molecule HMGB1. Results from both in vitro and in vivo experiments collectively demonstrated that the release of HMGB1 is contingent upon GSDME-mediated pyroptosis. Furthermore, label-free quantitative proteomics in vivo indicated that ATO-induced pyroptosis activates natural killer cells (NKs) and promotes the release of granzyme B (GZMB). Our study is the first to demonstrate the synergistic interplay between pyroptosis and ICD mechanisms during ATO treatment, providing novel insights into the potential of ATO for immunotherapy and synergistic treatment approaches.
The application of Arsenic trioxide (ATO) has greatly improved the cure rates in patients with acute promyelocytic leukemia (APL) and has shown therapeutic effects in other leukemia types, as evidenced by an increasing number of preclinical trials. However, its clinical application is still limited due to a lack of understanding of the underlying mechanisms. In this report, we have demonstrated that ATO can induce pyroptosis and release damage-associated molecular patterns (DAMPs), such as high mobility group box 1 (HMGB1) and interleukin-1β (IL-1β). DAMPs can activate the immunogenic cell death (ICD) mechanism. Our study elucidated the pivotal role of pyroptosis and demonstrated the activation of the caspase-3/gasdermin E (GSDME) pathway both in vivo and in vitro upon ATO intervention. Proteomic analysis of cell supernatants revealed the release of the ICD-associated molecule HMGB1. Results from both in vitro and in vivo experiments collectively demonstrated that the release of HMGB1 is contingent upon GSDME-mediated pyroptosis. Furthermore, label-free quantitative proteomics in vivo indicated that ATO-induced pyroptosis activates natural killer cells (NKs) and promotes the release of granzyme B (GZMB). Our study is the first to demonstrate the synergistic interplay between pyroptosis and ICD mechanisms during ATO treatment, providing novel insights into the potential of ATO for immunotherapy and synergistic treatment approaches.
2026, 37(7): 111586
doi: 10.1016/j.cclet.2025.111586
Abstract:
Multiple myeloma (MM) is the second most common hematological malignancy and still remains incurable. Selinexor (SEL) is the first-in-class exportin 1 (XPO1) inhibitor, and has demonstrated survival benefits in relapsed/refractory MM patients. Despite its therapeutic potential, dose-limiting toxicities frequently compromise SEL’s clinical utility and patients’ quality of life. In this work, to improve therapeutic efficacy and minimize side effects of SEL, we designed the monomethyl poly(ethylene glycol)-poly(ε-caprolactone) (mPEG-PCL) micelle-encapsulated nanoformulation for MM therapy. The mPEG-PCL-SEL micelle exhibited controlled release behavior and showed remarkable cytotoxicity in MM cells. Most importantly, in the orthotopic MM model, this micelle system exhibited impressive therapeutic efficacy at low dosages and significantly prolonged the survival of MM-bearing mice. Moreover, the mPEG-PCL-SEL micelle demonstrated a favorable safety profile with fewer gastrointestinal and constitutional symptoms. And we found that compared with the free-SEL, the mPEG-PCL-SEL micelle maintained the integrity of the intestinal barrier, and was more beneficial to the diversity of the intestinal microbiota, which may be related to the improved gastrointestinal tolerability, making it an effective and safe choice for MM treatment.
Multiple myeloma (MM) is the second most common hematological malignancy and still remains incurable. Selinexor (SEL) is the first-in-class exportin 1 (XPO1) inhibitor, and has demonstrated survival benefits in relapsed/refractory MM patients. Despite its therapeutic potential, dose-limiting toxicities frequently compromise SEL’s clinical utility and patients’ quality of life. In this work, to improve therapeutic efficacy and minimize side effects of SEL, we designed the monomethyl poly(ethylene glycol)-poly(ε-caprolactone) (mPEG-PCL) micelle-encapsulated nanoformulation for MM therapy. The mPEG-PCL-SEL micelle exhibited controlled release behavior and showed remarkable cytotoxicity in MM cells. Most importantly, in the orthotopic MM model, this micelle system exhibited impressive therapeutic efficacy at low dosages and significantly prolonged the survival of MM-bearing mice. Moreover, the mPEG-PCL-SEL micelle demonstrated a favorable safety profile with fewer gastrointestinal and constitutional symptoms. And we found that compared with the free-SEL, the mPEG-PCL-SEL micelle maintained the integrity of the intestinal barrier, and was more beneficial to the diversity of the intestinal microbiota, which may be related to the improved gastrointestinal tolerability, making it an effective and safe choice for MM treatment.
2026, 37(7): 111589
doi: 10.1016/j.cclet.2025.111589
Abstract:
Developing effective strategies to simultaneously suppress tumor thermotolerance and secondary inflammation remains a significant challenge in enhanced photothermal therapy (PTT). In this study, we developed a nitroreductase (NTR)-triggered multifunctional photothermal agent (m-SCy-DCF) by conjugating mitochondria-targeted sulfur-substituted hemicyanine to the anti-inflammatory diclofenac (DCF) through an NTR-cleavable linker. Upon activation in the hypoxic tumor microenvironment, m-SCy-DCF selectively accumulated in mitochondria and generated localized hyperthermia under laser irradiation. This process not only disrupted mitochondrial function but also suppressed the expression of heat shock proteins (HSPs). Simultaneously, the released DCF exerted potent anti-inflammatory effects, effectively reducing the levels of inflammatory cytokines in vivo. This dual suppression of tumor thermotolerance and inflammation induced immunogenic cell death and achieved effective tumor ablation, demonstrating the potential of m-SCy-DCF as a highly promising candidate for enhanced PTT.
Developing effective strategies to simultaneously suppress tumor thermotolerance and secondary inflammation remains a significant challenge in enhanced photothermal therapy (PTT). In this study, we developed a nitroreductase (NTR)-triggered multifunctional photothermal agent (m-SCy-DCF) by conjugating mitochondria-targeted sulfur-substituted hemicyanine to the anti-inflammatory diclofenac (DCF) through an NTR-cleavable linker. Upon activation in the hypoxic tumor microenvironment, m-SCy-DCF selectively accumulated in mitochondria and generated localized hyperthermia under laser irradiation. This process not only disrupted mitochondrial function but also suppressed the expression of heat shock proteins (HSPs). Simultaneously, the released DCF exerted potent anti-inflammatory effects, effectively reducing the levels of inflammatory cytokines in vivo. This dual suppression of tumor thermotolerance and inflammation induced immunogenic cell death and achieved effective tumor ablation, demonstrating the potential of m-SCy-DCF as a highly promising candidate for enhanced PTT.
2026, 37(7): 111641
doi: 10.1016/j.cclet.2025.111641
Abstract:
Macrophage-derived exosomes have demonstrated considerable potential for promoting bone regeneration. This study proposes a novel engineered therapeutic strategy that utilizes carbon monoxide releasing prodrugs (TG-Fe CORMs) to selectively induce M2 macrophage polarization, thereby enhancing the production of M2 macrophage-derived exosomes (CO-M2-Exos). These exosomes have been observed to significantly promote osteogenesis and accelerate alveolar bone regeneration through the microRNA-21/Lhx8 signaling pathway. Notably, these exosomes possess several advantageous characteristics, including their capacity for remarkable regenerative effects, low immunogenicity, and high cellular uptake, which renders them promising cell-free therapy for addressing alveolar bone defects. Moreover, the scalable production of CO-M2-Exos successfully overcomes the significant challenges associated with traditional exosome-based therapies, such as the complexity of cell culture processes, the instability of phenotype, and the low yield of exosome production. This engineered approach offers a reliable, efficient, and cost-effective solution for clinical translation, particularly for promoting alveolar bone regeneration in cases of severe bone atrophy following tooth extraction.
Macrophage-derived exosomes have demonstrated considerable potential for promoting bone regeneration. This study proposes a novel engineered therapeutic strategy that utilizes carbon monoxide releasing prodrugs (TG-Fe CORMs) to selectively induce M2 macrophage polarization, thereby enhancing the production of M2 macrophage-derived exosomes (CO-M2-Exos). These exosomes have been observed to significantly promote osteogenesis and accelerate alveolar bone regeneration through the microRNA-21/Lhx8 signaling pathway. Notably, these exosomes possess several advantageous characteristics, including their capacity for remarkable regenerative effects, low immunogenicity, and high cellular uptake, which renders them promising cell-free therapy for addressing alveolar bone defects. Moreover, the scalable production of CO-M2-Exos successfully overcomes the significant challenges associated with traditional exosome-based therapies, such as the complexity of cell culture processes, the instability of phenotype, and the low yield of exosome production. This engineered approach offers a reliable, efficient, and cost-effective solution for clinical translation, particularly for promoting alveolar bone regeneration in cases of severe bone atrophy following tooth extraction.
2026, 37(7): 111642
doi: 10.1016/j.cclet.2025.111642
Abstract:
Globo-H is a tumor-associated carbohydrate antigen (TACA) that is overexpressed in various cancers, making it a promising target for anticancer vaccine development. However, traditional conjugate vaccines, such as those linked to keyhole limpet hemocyanin (KLH) or cross-reactive material 197 (CRM197), have demonstrated limited clinical efficacy. To address this limitation, we developed an innovative vaccine candidate by conjugating chemoenzymatically synthesized Globo-H to a mutant of bacteriophage Qβ (mQβ) virus-like particle. The resulting mQβ-Globo-H conjugate elicited significantly higher levels of anti-Globo-H IgG antibodies in mice compared to both KLH-Globo-H and CRM197-Globo-H conjugates. Furthermore, the antibodies produced by the mQβ-Globo-H conjugate exhibited strong binding to MCF-7 breast cancer cells and triggered potent complement-dependent cytotoxicity (CDC) against these cancer cells. In contrast, negligible antibody binding and CDC effects were observed against normal MCF-10A breast epithelial cells. This new conjugate vaccine also produced robust humoral responses in rabbits, with the resulting antibodies exhibiting high selectivity for human breast cancer tissues. These findings underscore the clinical translational potential of the mQβ-Globo-H conjugate vaccine.
Globo-H is a tumor-associated carbohydrate antigen (TACA) that is overexpressed in various cancers, making it a promising target for anticancer vaccine development. However, traditional conjugate vaccines, such as those linked to keyhole limpet hemocyanin (KLH) or cross-reactive material 197 (CRM197), have demonstrated limited clinical efficacy. To address this limitation, we developed an innovative vaccine candidate by conjugating chemoenzymatically synthesized Globo-H to a mutant of bacteriophage Qβ (mQβ) virus-like particle. The resulting mQβ-Globo-H conjugate elicited significantly higher levels of anti-Globo-H IgG antibodies in mice compared to both KLH-Globo-H and CRM197-Globo-H conjugates. Furthermore, the antibodies produced by the mQβ-Globo-H conjugate exhibited strong binding to MCF-7 breast cancer cells and triggered potent complement-dependent cytotoxicity (CDC) against these cancer cells. In contrast, negligible antibody binding and CDC effects were observed against normal MCF-10A breast epithelial cells. This new conjugate vaccine also produced robust humoral responses in rabbits, with the resulting antibodies exhibiting high selectivity for human breast cancer tissues. These findings underscore the clinical translational potential of the mQβ-Globo-H conjugate vaccine.
2026, 37(7): 111645
doi: 10.1016/j.cclet.2025.111645
Abstract:
The antioxidant and immune-suppressive microenvironment of tumors has severely limited the efficacy of photodynamic therapy (PDT). To overcome these limitations, we proposed a novel nanoparticle (PEG-PFc/Hyp) that combined hypericin (Hyp) and ferrocene for synergistic anti-tumor therapy within a single system. Briefly, the optimum PEG114-PLL10 was reacted with ferrocene by the carboxylic acid N-succinimidyl ester(ferrocene-NHS), and the subsequent Hyp encapsulated in the above fabricated amphiphilic polymer. When under light irradiation, Hyp generated abundant reactive oxygen species (ROS) that synergized with •OH produced by ferrocene, leading to disrupted redox balance, amplified lethal lipid peroxidation (LPO) and inducing significant ferroptosis. Furthermore, the ferrocene could greatly alleviate hypoxia via O2 production, thereby cascaded enhancing the ROS production efficiency of PDT. As a result, the cascade augmented ROS level, alongside the glutathione (GSH) depletion in tumor cells, caused effective immunogenic cell death (ICD) and potent anti-tumor response. It turned out that the PDT-ferroptosis-ICD strategy enabled significant oxidative damage and tumor cell immunogenicity, offering great potential in cancer immunotherapy.
The antioxidant and immune-suppressive microenvironment of tumors has severely limited the efficacy of photodynamic therapy (PDT). To overcome these limitations, we proposed a novel nanoparticle (PEG-PFc/Hyp) that combined hypericin (Hyp) and ferrocene for synergistic anti-tumor therapy within a single system. Briefly, the optimum PEG114-PLL10 was reacted with ferrocene by the carboxylic acid N-succinimidyl ester(ferrocene-NHS), and the subsequent Hyp encapsulated in the above fabricated amphiphilic polymer. When under light irradiation, Hyp generated abundant reactive oxygen species (ROS) that synergized with •OH produced by ferrocene, leading to disrupted redox balance, amplified lethal lipid peroxidation (LPO) and inducing significant ferroptosis. Furthermore, the ferrocene could greatly alleviate hypoxia via O2 production, thereby cascaded enhancing the ROS production efficiency of PDT. As a result, the cascade augmented ROS level, alongside the glutathione (GSH) depletion in tumor cells, caused effective immunogenic cell death (ICD) and potent anti-tumor response. It turned out that the PDT-ferroptosis-ICD strategy enabled significant oxidative damage and tumor cell immunogenicity, offering great potential in cancer immunotherapy.
2026, 37(7): 111655
doi: 10.1016/j.cclet.2025.111655
Abstract:
Copper dysregulation is a critical factor in tumorigenesis and cancer therapy, underscoring the need for in vivo Cu(Ⅰ) imaging in tumors to elucidate its pathological roles. However, developing molecular probes for high-sensitivity and high-resolution in vivo Cu(Ⅰ) imaging remains a significant challenge. Herein, we report a covalently targeted small-molecule probe for dual-modality fluorescence and photoacoustic (PA) imaging of Cu(Ⅰ) in tumors. This probe exhibits highly selective near-infrared fluorescence enhancement and a ratiometric PA response upon coordination with Cu(Ⅰ). Furthermore, it enables precise tumor targeting and sustained imaging through specific recognition and covalent anchoring to the neutral cholesterol ester hydrolase 1 (NCEH1) protein. In vivo experiments demonstrate its capability for dynamic tracking of Cu(Ⅰ) in tumors with high sensitivity via fluorescence imaging and micro resolution via ratiometric PA imaging. We anticipate this Cu(Ⅰ)-responsive dual-modality probe with targeted anchoring capabilities will be a powerful tool for investigating Cu(Ⅰ) dynamics and transport in tumors, thereby deepening our understanding of pathological roles of Cu(Ⅰ) in cancer biology.
Copper dysregulation is a critical factor in tumorigenesis and cancer therapy, underscoring the need for in vivo Cu(Ⅰ) imaging in tumors to elucidate its pathological roles. However, developing molecular probes for high-sensitivity and high-resolution in vivo Cu(Ⅰ) imaging remains a significant challenge. Herein, we report a covalently targeted small-molecule probe for dual-modality fluorescence and photoacoustic (PA) imaging of Cu(Ⅰ) in tumors. This probe exhibits highly selective near-infrared fluorescence enhancement and a ratiometric PA response upon coordination with Cu(Ⅰ). Furthermore, it enables precise tumor targeting and sustained imaging through specific recognition and covalent anchoring to the neutral cholesterol ester hydrolase 1 (NCEH1) protein. In vivo experiments demonstrate its capability for dynamic tracking of Cu(Ⅰ) in tumors with high sensitivity via fluorescence imaging and micro resolution via ratiometric PA imaging. We anticipate this Cu(Ⅰ)-responsive dual-modality probe with targeted anchoring capabilities will be a powerful tool for investigating Cu(Ⅰ) dynamics and transport in tumors, thereby deepening our understanding of pathological roles of Cu(Ⅰ) in cancer biology.
2026, 37(7): 111666
doi: 10.1016/j.cclet.2025.111666
Abstract:
Excessive and prolonged inflammatory monocyte activity accelerates left ventricular remodeling after myocardial infarction (MI). After myocardial reperfusion, the CCL2/CCR2 axis is considered to be a key chemokine axis that initiates and modulates tissue inflammatory damage. Effectively blocking the CCL2/CCR2 axis can reduce the chemotaxis of inflammatory monocytes to the infarct area, which has important therapeutic value for the repair of myocardium after reperfusion injury (MI/R). Here, we propose a nanoparticle carrying CCL2 silencing short interfering RNA (siRNA), which is prepared by coating a lipid hybrid CCR2-overexprssion macrophage cell membrane on a siRNA-loaded mesoporous silica nanoparticle. The overexpression of CCR2 and adhesion factors on the macrophage membrane improves its targeting ability, directing nanoparticle to the myocardial infarction area of MI/R-induced mice, the overexpress CCR2 in the macrophage cell membrane also adsorb more CCL2. Then by fusing with the cell membrane, siRNA is released into the injured endothelial cells cytoplasm, silencing the expression of CCL2. In vivo administration of the formula blocked CCL2/CCR2 axis, reduce the chemotaxis of inflammatory cells, regulate the immune microenvironment, further decreasing myocardial infarction area and improving cardiac function. Targeted block of CCL2/CCR2 axis represent a new therapeutic intervention for inflammatory disease.
Excessive and prolonged inflammatory monocyte activity accelerates left ventricular remodeling after myocardial infarction (MI). After myocardial reperfusion, the CCL2/CCR2 axis is considered to be a key chemokine axis that initiates and modulates tissue inflammatory damage. Effectively blocking the CCL2/CCR2 axis can reduce the chemotaxis of inflammatory monocytes to the infarct area, which has important therapeutic value for the repair of myocardium after reperfusion injury (MI/R). Here, we propose a nanoparticle carrying CCL2 silencing short interfering RNA (siRNA), which is prepared by coating a lipid hybrid CCR2-overexprssion macrophage cell membrane on a siRNA-loaded mesoporous silica nanoparticle. The overexpression of CCR2 and adhesion factors on the macrophage membrane improves its targeting ability, directing nanoparticle to the myocardial infarction area of MI/R-induced mice, the overexpress CCR2 in the macrophage cell membrane also adsorb more CCL2. Then by fusing with the cell membrane, siRNA is released into the injured endothelial cells cytoplasm, silencing the expression of CCL2. In vivo administration of the formula blocked CCL2/CCR2 axis, reduce the chemotaxis of inflammatory cells, regulate the immune microenvironment, further decreasing myocardial infarction area and improving cardiac function. Targeted block of CCL2/CCR2 axis represent a new therapeutic intervention for inflammatory disease.
2026, 37(7): 111680
doi: 10.1016/j.cclet.2025.111680
Abstract:
Among various smart drug delivery systems (DDSs), redox-responsive systems have emerged as promising platforms for tumor therapy. Herein, we successfully fabricated a tumor microenvironment dual redox-responsive nanoparticle platform (DTX@Cys-0E NPs) assembled from an L-cystine-based biodegradable polymer (Cys-0E) for efficient delivery of docetaxel (DTX). The engineered Cys-0E features a unique structure containing both disulfide bonds and peroxalate ester bonds, synthesized via a one-step reaction. Notably, the strategic incorporation of 6-o-palmitoyl ascorbic acid (PA) not only enhances the stability of DTX@Cys-0E NPs but also generates tumor-specific H2O2. This PA-mediated H2O2 production triggers the degradation of the peroxalate ester bond, followed by CO2 generation, which ultimately results in DTX-controlled release. Simultaneously, the disulfide bonds in Cys-0E react with high concentrations of glutathione (GSH) in tumor cells, increasing the reactive oxygen species (ROS) level, and further facilitating drug release. Both in vitro and in vivo experiment results show that, once DTX@Cys-0E NPs are enriched into tumor cells, the rapid degradation of Cys-0E triggered by these stimuli leads to a burst release of DTX, inducing tumor cell apoptosis and exhibiting significantly better tumor inhibition compared to free DTX. In summary, this novel dual redox-responsive nano platform holds great promise as a controlled drug release system for cancer therapy.
Among various smart drug delivery systems (DDSs), redox-responsive systems have emerged as promising platforms for tumor therapy. Herein, we successfully fabricated a tumor microenvironment dual redox-responsive nanoparticle platform (DTX@Cys-0E NPs) assembled from an L-cystine-based biodegradable polymer (Cys-0E) for efficient delivery of docetaxel (DTX). The engineered Cys-0E features a unique structure containing both disulfide bonds and peroxalate ester bonds, synthesized via a one-step reaction. Notably, the strategic incorporation of 6-o-palmitoyl ascorbic acid (PA) not only enhances the stability of DTX@Cys-0E NPs but also generates tumor-specific H2O2. This PA-mediated H2O2 production triggers the degradation of the peroxalate ester bond, followed by CO2 generation, which ultimately results in DTX-controlled release. Simultaneously, the disulfide bonds in Cys-0E react with high concentrations of glutathione (GSH) in tumor cells, increasing the reactive oxygen species (ROS) level, and further facilitating drug release. Both in vitro and in vivo experiment results show that, once DTX@Cys-0E NPs are enriched into tumor cells, the rapid degradation of Cys-0E triggered by these stimuli leads to a burst release of DTX, inducing tumor cell apoptosis and exhibiting significantly better tumor inhibition compared to free DTX. In summary, this novel dual redox-responsive nano platform holds great promise as a controlled drug release system for cancer therapy.
2026, 37(7): 111692
doi: 10.1016/j.cclet.2025.111692
Abstract:
Ferroptosis, a form of programmed cell death driven by iron-dependent lipid peroxidation (LPO), has emerged as a promising therapeutic strategy for cancer. However, challenges such as uncontrolled iron delivery, insufficient ferroptosis induction efficiency, and off-target drug leakage limit its applications. To address these limitations, we developed a biomimetic nanoplatform (Fe-DTX@M) integrating cancer cell membrane-camouflaged Fe-based metallacycles with the chemotherapeutic drug docetaxel (DTX), which synergistically amplifies ferroptosis and apoptosis for precise and effective cervical cancer therapy. The membrane camouflage enabled highly efficient tumor-specific accumulation, achieving a 5.4-fold increase compared to non-targeted controls, and reduced systemic toxicity. Within tumors, Fe2+/Fe3+ cycles attributed to Fe-based metallacycle drove Fenton reactions to convert H2O2 into •OH, inducing LPO, while Fe3+-mediated glutathione depletion inhibited GPX4, amplifying ferroptosis with 2.4-fold malondialdehyde (MDA) increase. Acid-triggered DTX release of nanoplatform further promoted apoptosis, thereby enhancing therapeutic efficacy. Furthermore, Fe-DTX@M exhibited excellent long-term biocompatibility and safety in normal mice over 30 days post-intravenous injection. This combination of biomimetic metallacycles-induced ferroptosis and chemotherapy-induced apoptosis may provide a new paradigm for achieving effective cancer therapy.
Ferroptosis, a form of programmed cell death driven by iron-dependent lipid peroxidation (LPO), has emerged as a promising therapeutic strategy for cancer. However, challenges such as uncontrolled iron delivery, insufficient ferroptosis induction efficiency, and off-target drug leakage limit its applications. To address these limitations, we developed a biomimetic nanoplatform (Fe-DTX@M) integrating cancer cell membrane-camouflaged Fe-based metallacycles with the chemotherapeutic drug docetaxel (DTX), which synergistically amplifies ferroptosis and apoptosis for precise and effective cervical cancer therapy. The membrane camouflage enabled highly efficient tumor-specific accumulation, achieving a 5.4-fold increase compared to non-targeted controls, and reduced systemic toxicity. Within tumors, Fe2+/Fe3+ cycles attributed to Fe-based metallacycle drove Fenton reactions to convert H2O2 into •OH, inducing LPO, while Fe3+-mediated glutathione depletion inhibited GPX4, amplifying ferroptosis with 2.4-fold malondialdehyde (MDA) increase. Acid-triggered DTX release of nanoplatform further promoted apoptosis, thereby enhancing therapeutic efficacy. Furthermore, Fe-DTX@M exhibited excellent long-term biocompatibility and safety in normal mice over 30 days post-intravenous injection. This combination of biomimetic metallacycles-induced ferroptosis and chemotherapy-induced apoptosis may provide a new paradigm for achieving effective cancer therapy.
2026, 37(7): 111694
doi: 10.1016/j.cclet.2025.111694
Abstract:
Prodrug nanoassemblies (NPs) have attracted much attention in improving the selectivity of chemotherapy drugs, while most of them suffer from poor targeting efficiency. Biotin, a well-known tumor-targeting ligand, can greatly enhance tumor accumulation. Herein, we construct the biotinylated prodrug (Biotin-PTX) by connecting paclitaxel (PTX) to biotin via a disulfide bond, enabling the prodrug to self-assemble into nanoparticles (Biotin-PTX NPs). However, the pure NPs are observed to be rapidly cleared without polyethylene glycol (PEG) modifying, while excessive PEG can compromise their targeting efficiency, suggesting that it is crucial to optimize the amount of PEG. On this basis, the effect of distearoyl phosphatidylethanolamine-polyethylene glycol2000 (DSPE-PEG2k) ratios (0%, 5%, 10%, 20%, 40% and 60%, WPEG/Wprodrug+PEG) on their performance have been investigated. The results provide evidence that Biotin-PTX NPs containing 20% DSPE-PEG2k (20% NPs) can significantly improve colloidal stability and tumor-targeting efficiency. Moreover, 20% NPs exhibits good antitumor efficacy and safety compared with Taxol, Abraxane and Prodrug Sol. This work highlights the key role of moderate PEGylation in regulating the therapeutic performance of targeting NPs, offering a new way of thinking for tumor-targeting treatment.
Prodrug nanoassemblies (NPs) have attracted much attention in improving the selectivity of chemotherapy drugs, while most of them suffer from poor targeting efficiency. Biotin, a well-known tumor-targeting ligand, can greatly enhance tumor accumulation. Herein, we construct the biotinylated prodrug (Biotin-PTX) by connecting paclitaxel (PTX) to biotin via a disulfide bond, enabling the prodrug to self-assemble into nanoparticles (Biotin-PTX NPs). However, the pure NPs are observed to be rapidly cleared without polyethylene glycol (PEG) modifying, while excessive PEG can compromise their targeting efficiency, suggesting that it is crucial to optimize the amount of PEG. On this basis, the effect of distearoyl phosphatidylethanolamine-polyethylene glycol2000 (DSPE-PEG2k) ratios (0%, 5%, 10%, 20%, 40% and 60%, WPEG/Wprodrug+PEG) on their performance have been investigated. The results provide evidence that Biotin-PTX NPs containing 20% DSPE-PEG2k (20% NPs) can significantly improve colloidal stability and tumor-targeting efficiency. Moreover, 20% NPs exhibits good antitumor efficacy and safety compared with Taxol, Abraxane and Prodrug Sol. This work highlights the key role of moderate PEGylation in regulating the therapeutic performance of targeting NPs, offering a new way of thinking for tumor-targeting treatment.
2026, 37(7): 111714
doi: 10.1016/j.cclet.2025.111714
Abstract:
Age-related macular degeneration (AMD) represents a primary cause of vision loss in the elderly population. Reactive oxygen species (ROS) generation constitutes a pivotal pathogenesis mechanism in AMD. Berberine (BBR) shows therapeutic potential for dry AMD through its ability to mitigate cellular senescence and oxidative stress. However, BBR’s low transmembrane permeability severely limits corneal penetration via topic administration, creating an urgent need for novel posterior segment delivery strategies. In this study, we employed biocompatible ionic liquids (ILs) to enhance BBR permeation for posterior AMD treatment. Our approach features ocular surface pretreatment with ILs followed by topical administration of BBR solution. Comprehensive in vitro and in vivo safety assessments confirmed the biocompatibility of monoethanolamine-based IL (Mea-ILs) as ocular penetration enhancers. Trans-monolayer experiments using human corneal epithelial cells (HCECs) demonstrated that ILs enhance paracellular permeability, potentially through tight junction modulation. In vivo studies utilizing a sodium iodate-induced dry AMD mouse model revealed that pretreatment with the [monoethanolamine][citric acid] ([Mea][Ci]) IL significantly potentiated BBR's therapeutic efficacy. These findings not only expand pharmaceutical applications of ILs but also establish a safe, efficient strategy for noninvasive dry AMD therapy with BBR. Furthermore, this work provides critical insights for developing advanced penetration enhancers for posterior ocular drug delivery.
Age-related macular degeneration (AMD) represents a primary cause of vision loss in the elderly population. Reactive oxygen species (ROS) generation constitutes a pivotal pathogenesis mechanism in AMD. Berberine (BBR) shows therapeutic potential for dry AMD through its ability to mitigate cellular senescence and oxidative stress. However, BBR’s low transmembrane permeability severely limits corneal penetration via topic administration, creating an urgent need for novel posterior segment delivery strategies. In this study, we employed biocompatible ionic liquids (ILs) to enhance BBR permeation for posterior AMD treatment. Our approach features ocular surface pretreatment with ILs followed by topical administration of BBR solution. Comprehensive in vitro and in vivo safety assessments confirmed the biocompatibility of monoethanolamine-based IL (Mea-ILs) as ocular penetration enhancers. Trans-monolayer experiments using human corneal epithelial cells (HCECs) demonstrated that ILs enhance paracellular permeability, potentially through tight junction modulation. In vivo studies utilizing a sodium iodate-induced dry AMD mouse model revealed that pretreatment with the [monoethanolamine][citric acid] ([Mea][Ci]) IL significantly potentiated BBR's therapeutic efficacy. These findings not only expand pharmaceutical applications of ILs but also establish a safe, efficient strategy for noninvasive dry AMD therapy with BBR. Furthermore, this work provides critical insights for developing advanced penetration enhancers for posterior ocular drug delivery.
2026, 37(7): 111722
doi: 10.1016/j.cclet.2025.111722
Abstract:
Acute respiratory distress syndrome (ARDS) is one of the diseases with a significant mortality rate due to respiratory failure. Yet, malignant microenvironment (MM) composed mainly of inflammatory cytokines (IC) and reactive oxygen species (ROS) limit the therapeutic effect. Herein we construct the nanoparticles (NPs) BSA-MnO2@Tan-IIA/PSLs (BMTPLs) to disrupt the vicious cycle between IC and ROS by suppressing IC production and scavenging ROS, which effectively remodels the MM of ARDS. The BMTPLs composed of the water-dispersible BSA-MnO2 (BM) and phosphatidylserine (PS)-consisting lipid shell containing lipophilic tanshinone IIA (Tan-IIA). After phagocytosed by activated macrophages (M1) in an efferocytosis-like manner originating from the PS effect, the released Tan-IIA inhibit NF-κB pathway and further suppresses the secretion of IC. Concurrently, BM scavenging ROS alleviates the oxidative stress microenvironment, which deeply enhances the anti-inflammation effect of Tan-IIA. Moreover, the low-level ROS and down-regulation IC promote the transformation from pro-inflammatory M1 to anti-inflammatory M2 contributing to restoring tissue homeostasis. The results in vitro and in vivo indicate that the MM of ARDS can be effectively remodeled by BMTPLs, which holds great potential for ARDS treatment.
Acute respiratory distress syndrome (ARDS) is one of the diseases with a significant mortality rate due to respiratory failure. Yet, malignant microenvironment (MM) composed mainly of inflammatory cytokines (IC) and reactive oxygen species (ROS) limit the therapeutic effect. Herein we construct the nanoparticles (NPs) BSA-MnO2@Tan-IIA/PSLs (BMTPLs) to disrupt the vicious cycle between IC and ROS by suppressing IC production and scavenging ROS, which effectively remodels the MM of ARDS. The BMTPLs composed of the water-dispersible BSA-MnO2 (BM) and phosphatidylserine (PS)-consisting lipid shell containing lipophilic tanshinone IIA (Tan-IIA). After phagocytosed by activated macrophages (M1) in an efferocytosis-like manner originating from the PS effect, the released Tan-IIA inhibit NF-κB pathway and further suppresses the secretion of IC. Concurrently, BM scavenging ROS alleviates the oxidative stress microenvironment, which deeply enhances the anti-inflammation effect of Tan-IIA. Moreover, the low-level ROS and down-regulation IC promote the transformation from pro-inflammatory M1 to anti-inflammatory M2 contributing to restoring tissue homeostasis. The results in vitro and in vivo indicate that the MM of ARDS can be effectively remodeled by BMTPLs, which holds great potential for ARDS treatment.
2026, 37(7): 111727
doi: 10.1016/j.cclet.2025.111727
Abstract:
Ulcerative colitis (UC) is a chronic inflammatory bowel disease featured by dysregulated immune responses and compromised intestinal barrier function. Current therapies often suffer from limited efficacy and systemic side effects due to non-specific drug distribution. Here, we developed macrophage membrane-camouflaged nanovesicles (mcNVs) for targeted delivery of emodin (Emo) to inflamed colon tissues. The biomimetic nanovesicles were fabricated by fusing J774A.1 macrophage membranes with Emo-loaded liposomes, inheriting the parent cells' chemotactic homing capabilities while maintaining excellent drug loading and colloidal stability. Systematic characterization confirmed successful membrane integration, as evidenced by transmission electron microscope (TEM) imaging, particle size, and ζ potential analyses. In vitro studies demonstrated favorable sustained release and enhanced cellular uptake of Emo-loaded mcNVs (Emo-mcNVs) compared to conventional liposomes. In a sodium dextran sulfate (DSS)-induced murine colitis model, Emo-mcNVs exhibited superior colon-targeting capability through chemokine gradient recognition (C-C motif chemokine ligand (CCL)2/3/5), resulting in significantly improved therapeutic outcomes versus free Emo and 5-aminosalicylic acid controls. Treatment with Emo-mcNVs attenuated disease severity (reduced disease activity index (DAI) score), preserved the colon architecture, and decreased pro-inflammatory cytokines (tumor necrosis factor α (TNF-α), interleukin 1β (IL-1β), IL-6). Biodistribution studies using multimodal imaging confirmed specific accumulation in the inflamed colon tissue with minimal systemic exposure. This study presents a novel biohybrid delivery system that leverages the pathophysiology of UC for targeted therapy, offering a promising translational approach for inflammatory bowel diseases.
Ulcerative colitis (UC) is a chronic inflammatory bowel disease featured by dysregulated immune responses and compromised intestinal barrier function. Current therapies often suffer from limited efficacy and systemic side effects due to non-specific drug distribution. Here, we developed macrophage membrane-camouflaged nanovesicles (mcNVs) for targeted delivery of emodin (Emo) to inflamed colon tissues. The biomimetic nanovesicles were fabricated by fusing J774A.1 macrophage membranes with Emo-loaded liposomes, inheriting the parent cells' chemotactic homing capabilities while maintaining excellent drug loading and colloidal stability. Systematic characterization confirmed successful membrane integration, as evidenced by transmission electron microscope (TEM) imaging, particle size, and ζ potential analyses. In vitro studies demonstrated favorable sustained release and enhanced cellular uptake of Emo-loaded mcNVs (Emo-mcNVs) compared to conventional liposomes. In a sodium dextran sulfate (DSS)-induced murine colitis model, Emo-mcNVs exhibited superior colon-targeting capability through chemokine gradient recognition (C-C motif chemokine ligand (CCL)2/3/5), resulting in significantly improved therapeutic outcomes versus free Emo and 5-aminosalicylic acid controls. Treatment with Emo-mcNVs attenuated disease severity (reduced disease activity index (DAI) score), preserved the colon architecture, and decreased pro-inflammatory cytokines (tumor necrosis factor α (TNF-α), interleukin 1β (IL-1β), IL-6). Biodistribution studies using multimodal imaging confirmed specific accumulation in the inflamed colon tissue with minimal systemic exposure. This study presents a novel biohybrid delivery system that leverages the pathophysiology of UC for targeted therapy, offering a promising translational approach for inflammatory bowel diseases.
2026, 37(7): 111744
doi: 10.1016/j.cclet.2025.111744
Abstract:
Phosgene, a highly toxic chemical warfare agent and industrial hazard, poses significant environmental and health risks, necessitating the development of rapid and reliable detection methods. Herein, we present a novel near infrared Ⅱ (NIR-Ⅱ) fluorescent probe based on silicon rhodamine and an o-phenylenediamine-responsive group for the sensitive and selective detection of phosgene. In the presence of phosgene, it generates a distinct color change and lights up NIR-Ⅱ (900 nm) emission, enabling both naked-eye visualization and fluorescence in vivo analysis. The probe shows rapid exceptional selectivity for phosgene and achieves rapid detection in solutions, gases, and soils. Notably, we successfully utilize this probe for in vivo imaging in Arabidopsis thaliana, enabling high signal-to-noise ratio real-time monitoring of phosgene within plant systems with minimal interference from autofluorescence. This work advances the design of reaction-based NIR-Ⅱ probes for hazardous chemical monitoring, combining simple operation, high sensitivity, and broad applicability, thereby contributing to environmental safety and sustainability.
Phosgene, a highly toxic chemical warfare agent and industrial hazard, poses significant environmental and health risks, necessitating the development of rapid and reliable detection methods. Herein, we present a novel near infrared Ⅱ (NIR-Ⅱ) fluorescent probe based on silicon rhodamine and an o-phenylenediamine-responsive group for the sensitive and selective detection of phosgene. In the presence of phosgene, it generates a distinct color change and lights up NIR-Ⅱ (900 nm) emission, enabling both naked-eye visualization and fluorescence in vivo analysis. The probe shows rapid exceptional selectivity for phosgene and achieves rapid detection in solutions, gases, and soils. Notably, we successfully utilize this probe for in vivo imaging in Arabidopsis thaliana, enabling high signal-to-noise ratio real-time monitoring of phosgene within plant systems with minimal interference from autofluorescence. This work advances the design of reaction-based NIR-Ⅱ probes for hazardous chemical monitoring, combining simple operation, high sensitivity, and broad applicability, thereby contributing to environmental safety and sustainability.
2026, 37(7): 111745
doi: 10.1016/j.cclet.2025.111745
Abstract:
Nitric oxide (NO), a significant signaling molecule, plays essential roles in diverse physiological and pathological processes including cell senescence. Lysosomes are recognized as pivotal subcellular organelles of cellular senescence, whereas the influence of senescence on lysosomal NO homeostasis remains poorly understood. To explore the potential association between cellular senescence and alterations in lysosomal NO levels, herein, we developed FL-O1, a novel ratiometric fluorescent probe specifically designed for lysosomal NO detection. The probe selectively reacts with NO through the recognition unit of o-phenylenediamine, forming an extended conjugated system that generates a distinct ratiometric optical signal with exceptional sensitivity (detection limit = 95 nmol/L). FL-O1 exhibits versatile applications in both in vitro and in vivo contexts. It successfully visualizes exogenous and endogenous NO dynamics in live zebrafish models and enables specific monitoring of lysosomal NO levels in cellular systems. Importantly, the probe was utilized to quantitatively evaluate NO levels in senescent states of cancer and healthy cells. The results revealed two key insights: (1) Senescent cells consistently maintain higher NO concentrations compared to their non-senescent counterparts, and (2) senescent healthy cells exhibit elevated NO levels relative to senescent cancer cells. This innovative small-molecule probe represents a significant advancement in lysosomal NO imaging technology. Its unique design and capabilities provide a powerful tool for investigating the role of lysosomal NO in cellular senescence, potentially uncovering novel mechanistic insights and facilitating the development of targeted therapeutic strategies for senescence-related disorders.
Nitric oxide (NO), a significant signaling molecule, plays essential roles in diverse physiological and pathological processes including cell senescence. Lysosomes are recognized as pivotal subcellular organelles of cellular senescence, whereas the influence of senescence on lysosomal NO homeostasis remains poorly understood. To explore the potential association between cellular senescence and alterations in lysosomal NO levels, herein, we developed FL-O1, a novel ratiometric fluorescent probe specifically designed for lysosomal NO detection. The probe selectively reacts with NO through the recognition unit of o-phenylenediamine, forming an extended conjugated system that generates a distinct ratiometric optical signal with exceptional sensitivity (detection limit = 95 nmol/L). FL-O1 exhibits versatile applications in both in vitro and in vivo contexts. It successfully visualizes exogenous and endogenous NO dynamics in live zebrafish models and enables specific monitoring of lysosomal NO levels in cellular systems. Importantly, the probe was utilized to quantitatively evaluate NO levels in senescent states of cancer and healthy cells. The results revealed two key insights: (1) Senescent cells consistently maintain higher NO concentrations compared to their non-senescent counterparts, and (2) senescent healthy cells exhibit elevated NO levels relative to senescent cancer cells. This innovative small-molecule probe represents a significant advancement in lysosomal NO imaging technology. Its unique design and capabilities provide a powerful tool for investigating the role of lysosomal NO in cellular senescence, potentially uncovering novel mechanistic insights and facilitating the development of targeted therapeutic strategies for senescence-related disorders.
2026, 37(7): 111748
doi: 10.1016/j.cclet.2025.111748
Abstract:
Extracellular vesicles (EVs), mainly comprising microvesicles (MiV) and exosomes (Exo), were successfully isolated from normal human embryonic kidney cells (HEK293T) and demonstrated specific uptake by human tongue squamous cell carcinoma cells (SCC-9). Initial mechanistic investigations revealed that both MiV and Exo were mainly internalized via endocytic pathways and predominantly relied on the surface proteins of SCC-9 cells for specific uptake. Furthermore, Exo, with better stability and uptake efficiency, were chosen as the carriers of the clinical drug cisplatin (CDDP) for the treatment of tongue cancer. Comprehensive in vitro and in vivo evaluations demonstrated that the Exo-CDDP system exhibited remarkable biocompatibility, mitigated drug-related toxicity and minimized CDDP efflux from tumor cells, and displayed potent anti-tumor efficacy. These findings collectively indicated that HEK293T-derived Exo represent a highly promising drug delivery platform for tongue cancer therapy, while simultaneously offering innovative ideas for the development of versatile Exo-based therapeutic delivery systems.
Extracellular vesicles (EVs), mainly comprising microvesicles (MiV) and exosomes (Exo), were successfully isolated from normal human embryonic kidney cells (HEK293T) and demonstrated specific uptake by human tongue squamous cell carcinoma cells (SCC-9). Initial mechanistic investigations revealed that both MiV and Exo were mainly internalized via endocytic pathways and predominantly relied on the surface proteins of SCC-9 cells for specific uptake. Furthermore, Exo, with better stability and uptake efficiency, were chosen as the carriers of the clinical drug cisplatin (CDDP) for the treatment of tongue cancer. Comprehensive in vitro and in vivo evaluations demonstrated that the Exo-CDDP system exhibited remarkable biocompatibility, mitigated drug-related toxicity and minimized CDDP efflux from tumor cells, and displayed potent anti-tumor efficacy. These findings collectively indicated that HEK293T-derived Exo represent a highly promising drug delivery platform for tongue cancer therapy, while simultaneously offering innovative ideas for the development of versatile Exo-based therapeutic delivery systems.
2026, 37(7): 111749
doi: 10.1016/j.cclet.2025.111749
Abstract:
Core-shell capsules are excellent carriers, showing good performances in cargo protection and controlled release. However, the controlled encapsulation of solid particles in capsules remains a great challenge, severely limiting their widespread applications. Here, a millifluidic system assisted by periodic vibrations is developed to precisely control the preparation of particle-loaded capsules. A high-frequency low-amplitude vibration is applied to prevent the jamming of solid particles by shaking and a low-frequency high-amplitude vibration is applied to synchronize the feeding of solid particles and the emulsification of capsules by generating a periodic flow pulse. The phase diagrams of particle-loaded capsules are systematically investigated with respect to various experimental parameters to provide guidances for the controlled preparation process. The developed millifluidic system offers a versatile platform to precisely prepare core-shell capsules loaded with different sizes, types and numbers of particles. The prepared particle-loaded capsules possess good biocompatibility, monodispersity, mechanical strength, storage stability and controlled release, paving the way for their widespread applications.
Core-shell capsules are excellent carriers, showing good performances in cargo protection and controlled release. However, the controlled encapsulation of solid particles in capsules remains a great challenge, severely limiting their widespread applications. Here, a millifluidic system assisted by periodic vibrations is developed to precisely control the preparation of particle-loaded capsules. A high-frequency low-amplitude vibration is applied to prevent the jamming of solid particles by shaking and a low-frequency high-amplitude vibration is applied to synchronize the feeding of solid particles and the emulsification of capsules by generating a periodic flow pulse. The phase diagrams of particle-loaded capsules are systematically investigated with respect to various experimental parameters to provide guidances for the controlled preparation process. The developed millifluidic system offers a versatile platform to precisely prepare core-shell capsules loaded with different sizes, types and numbers of particles. The prepared particle-loaded capsules possess good biocompatibility, monodispersity, mechanical strength, storage stability and controlled release, paving the way for their widespread applications.
2026, 37(7): 111750
doi: 10.1016/j.cclet.2025.111750
Abstract:
Cysteine (Cys), as a key precursor of glutathione (GSH) and an essential component of the thiol antioxidant system, plays a dual role in the pathological progression of Alzheimer’s disease (AD): it participates in antioxidant defense mechanisms while also potentially exacerbating neurological damage through metabolic dysregulation. Investigating the dynamic regulatory mechanisms of Cys in AD progression serves as a critical bridge linking oxidative stress, metabolic dysregulation, and neurodegenerative degeneration. High-resolution in vivo imaging of Cys dynamics in AD brains remains an unmet need. In view of the instability of the fluorescent probe of acrylyl group and the lack of specificity for Cys. This work introduced chlorine atoms into the probe structure, and achieved dual modifications: (1) Converting the nucleophilic addition mechanism into an SN2 substitution; (2) modulating the conjugation effects between the formyl group and the three-position double bond. In this way, the stability of the probe, the high specificity of Cys, and the crossing of the blood-brain barrier are addressed. Through in situ imaging in AD models, we have demonstrated a pathological reduction in Cys levels during AD. Furthermore, as Cys serves as the core molecule in the regulation of ferroptosis, it was found that ferroptosis can mediate the down-regulation of Cys in AD through ferroptosis inducers and inhibitors. This study is not only to reveal the core pathological mechanism of AD, but to provide theoretical basis and technical support for early diagnosis, targeted therapy and personalized medicine.
Cysteine (Cys), as a key precursor of glutathione (GSH) and an essential component of the thiol antioxidant system, plays a dual role in the pathological progression of Alzheimer’s disease (AD): it participates in antioxidant defense mechanisms while also potentially exacerbating neurological damage through metabolic dysregulation. Investigating the dynamic regulatory mechanisms of Cys in AD progression serves as a critical bridge linking oxidative stress, metabolic dysregulation, and neurodegenerative degeneration. High-resolution in vivo imaging of Cys dynamics in AD brains remains an unmet need. In view of the instability of the fluorescent probe of acrylyl group and the lack of specificity for Cys. This work introduced chlorine atoms into the probe structure, and achieved dual modifications: (1) Converting the nucleophilic addition mechanism into an SN2 substitution; (2) modulating the conjugation effects between the formyl group and the three-position double bond. In this way, the stability of the probe, the high specificity of Cys, and the crossing of the blood-brain barrier are addressed. Through in situ imaging in AD models, we have demonstrated a pathological reduction in Cys levels during AD. Furthermore, as Cys serves as the core molecule in the regulation of ferroptosis, it was found that ferroptosis can mediate the down-regulation of Cys in AD through ferroptosis inducers and inhibitors. This study is not only to reveal the core pathological mechanism of AD, but to provide theoretical basis and technical support for early diagnosis, targeted therapy and personalized medicine.
2026, 37(7): 111775
doi: 10.1016/j.cclet.2025.111775
Abstract:
Polymer dielectric capacitors are crucial for advanced power electronics but are often limited by the trade-off among energy density, efficiency, and thermal stability under high electric fields. To overcome these challenges, we propose a multiscale chemical configuration design strategy by constructing a ternary composite comprising high glass transition temperature fluorene polyester (FPE), polyetherimide (PEI), and high-aspect-ratio γ-Al2O3 nanosheets (AO NS). At the molecular scale, the structural compatibility between FPE and PEI enables homogeneous blending, while the incorporation of PEI increases free volume, enhances dipolar mobility, and preserves low dielectric loss. At the nanoscale, AO NS act as ceramic barriers to suppress charge injection, raise interfacial polarization, and stabilize the local electric field. At the device level, this hierarchical design leads to synergistic improvements in dielectric properties, insulation, and energy storage performance. As a result, the optimized composite achieves excellent high-temperature energy-storage capability, characterized by a high energy density of 5.51 J/cm3 with above 80% efficiency at 150 ℃ and 550 MV/m. This study paves a practical and scalable path toward high-performance polymer dielectrics for reliable energy storage under extreme thermal and electrical conditions.
Polymer dielectric capacitors are crucial for advanced power electronics but are often limited by the trade-off among energy density, efficiency, and thermal stability under high electric fields. To overcome these challenges, we propose a multiscale chemical configuration design strategy by constructing a ternary composite comprising high glass transition temperature fluorene polyester (FPE), polyetherimide (PEI), and high-aspect-ratio γ-Al2O3 nanosheets (AO NS). At the molecular scale, the structural compatibility between FPE and PEI enables homogeneous blending, while the incorporation of PEI increases free volume, enhances dipolar mobility, and preserves low dielectric loss. At the nanoscale, AO NS act as ceramic barriers to suppress charge injection, raise interfacial polarization, and stabilize the local electric field. At the device level, this hierarchical design leads to synergistic improvements in dielectric properties, insulation, and energy storage performance. As a result, the optimized composite achieves excellent high-temperature energy-storage capability, characterized by a high energy density of 5.51 J/cm3 with above 80% efficiency at 150 ℃ and 550 MV/m. This study paves a practical and scalable path toward high-performance polymer dielectrics for reliable energy storage under extreme thermal and electrical conditions.
2026, 37(7): 111798
doi: 10.1016/j.cclet.2025.111798
Abstract:
Biomolecular self-assembly systems form the cornerstone of biological structures, in which the interactions between carbohydrates and proteins play a crucial role in many life processes. This has driven the development of biomimetic carbohydrate-protein supramolecular assemblies (BCPSAs), which show great potential in biomedical research. We successfully constructed a novel supramolecular hybrid nanocarrier with pH responsiveness and targeting capabilities based on specific interactions between carbohydrates and proteins. This system self-assembles into nanoparticles CA@MP5 in water through the specific binding of mannose clusters on glycosylated pillar[5]arene MP5 with lectin Con A. Additionally, through a host-guest assembly strategy with the synthesized β-d-galactopyranosyl pyridine derivative G, it complexes within the MP5 cavity to form a "double-sweet" supramolecular glyco-nanoprotein (CA@MP5⊃G). This system shows high affinity for the asialoglycoprotein receptor (ASGPR) on HepG2 liver cancer cells. In vitro, the doxorubicin (DOX)-loaded micelles (DCA@MP5⊃G) release drug effectively in acidic environments and significantly inhibit HepG2 cell growth, with reduced toxicity toward normal cells. In vivo, the nanocarrier targets tumors effectively, reducing systemic toxicity and inhibiting tumor growth. This study offers a novel construction strategy for drug delivery systems based on carbohydrate-protein interactions in anti-tumor applications, which is significant for enhancing therapeutic efficacy.
Biomolecular self-assembly systems form the cornerstone of biological structures, in which the interactions between carbohydrates and proteins play a crucial role in many life processes. This has driven the development of biomimetic carbohydrate-protein supramolecular assemblies (BCPSAs), which show great potential in biomedical research. We successfully constructed a novel supramolecular hybrid nanocarrier with pH responsiveness and targeting capabilities based on specific interactions between carbohydrates and proteins. This system self-assembles into nanoparticles CA@MP5 in water through the specific binding of mannose clusters on glycosylated pillar[5]arene MP5 with lectin Con A. Additionally, through a host-guest assembly strategy with the synthesized β-d-galactopyranosyl pyridine derivative G, it complexes within the MP5 cavity to form a "double-sweet" supramolecular glyco-nanoprotein (CA@MP5⊃G). This system shows high affinity for the asialoglycoprotein receptor (ASGPR) on HepG2 liver cancer cells. In vitro, the doxorubicin (DOX)-loaded micelles (DCA@MP5⊃G) release drug effectively in acidic environments and significantly inhibit HepG2 cell growth, with reduced toxicity toward normal cells. In vivo, the nanocarrier targets tumors effectively, reducing systemic toxicity and inhibiting tumor growth. This study offers a novel construction strategy for drug delivery systems based on carbohydrate-protein interactions in anti-tumor applications, which is significant for enhancing therapeutic efficacy.
2026, 37(7): 111816
doi: 10.1016/j.cclet.2025.111816
Abstract:
Achieving efficient and sustainable hydrogen production from methanol electrolysis requires significant advances in catalyst design. In this study, we present a novel strategy where nickel selenide, featuring distinct crystal phases, anchors on mesoporous hollow carbon spheres to synergistically enhance the activity of Pt for methanol-assisted water splitting reactions. The heterostructured NiSe/NiSe2 nanosheets modulate the electronic structure of Pt, positioning it closer to an optimal thermodynamic state, and creating a highly oxophilic environment that accelerates charge transfer and optimizes the adsorption and desorption of reaction intermediates. The engineered hybrid catalyst exhibits exceptional enhancements in both mass and specific activity for methanol oxidation, significantly outperforming commercial catalysts. In addition, the catalyst exhibits a high electroactive surface area, an abundance of active sites, fast catalytic kinetics, and excellent stability. Notably, a methanol electrolyzer utilizing this catalyst achieves a current density of 10 mA/cm2 at only 0.67 V, a remarkable 1.08 V reduction compared to the voltage required for conventional water electrolysis (1.75 V). This work provides a transformative strategy for designing high-performance electrocatalysts, offering new pathways for more efficient and sustainable hydrogen production through methanol electrolysis.
Achieving efficient and sustainable hydrogen production from methanol electrolysis requires significant advances in catalyst design. In this study, we present a novel strategy where nickel selenide, featuring distinct crystal phases, anchors on mesoporous hollow carbon spheres to synergistically enhance the activity of Pt for methanol-assisted water splitting reactions. The heterostructured NiSe/NiSe2 nanosheets modulate the electronic structure of Pt, positioning it closer to an optimal thermodynamic state, and creating a highly oxophilic environment that accelerates charge transfer and optimizes the adsorption and desorption of reaction intermediates. The engineered hybrid catalyst exhibits exceptional enhancements in both mass and specific activity for methanol oxidation, significantly outperforming commercial catalysts. In addition, the catalyst exhibits a high electroactive surface area, an abundance of active sites, fast catalytic kinetics, and excellent stability. Notably, a methanol electrolyzer utilizing this catalyst achieves a current density of 10 mA/cm2 at only 0.67 V, a remarkable 1.08 V reduction compared to the voltage required for conventional water electrolysis (1.75 V). This work provides a transformative strategy for designing high-performance electrocatalysts, offering new pathways for more efficient and sustainable hydrogen production through methanol electrolysis.
2026, 37(7): 111819
doi: 10.1016/j.cclet.2025.111819
Abstract:
Alkylated arenes, which are prevalent molecular building blocks, are widely applicable across various scientific domains. However, regioselectively alkylating arenes often poses significant challenges, despite their apparent simplicities. Herein, we report the first examples of substrate-controlled photocatalyzed regiodivergent alkylations of aromatic nitriles. The judicious choice of alkyl halide facilitated selection of mechanistically divergent processes. The two reaction manifolds, an ipso-substitution path that proceeds via radical coupling and a Friedel−Crafts-type C–H alkylation via quantum mechanical tunneling, enabled selective access to regioisomeric alkylated arenes. Mechanistic investigations combined with density functional theory (DFT) calculations shed light on the origin of this regioselectivity switch. Remarkably, this process exhibited superior efficiencies, reactivities, and synthetic utilities, and can be performed on the gram scale.
Alkylated arenes, which are prevalent molecular building blocks, are widely applicable across various scientific domains. However, regioselectively alkylating arenes often poses significant challenges, despite their apparent simplicities. Herein, we report the first examples of substrate-controlled photocatalyzed regiodivergent alkylations of aromatic nitriles. The judicious choice of alkyl halide facilitated selection of mechanistically divergent processes. The two reaction manifolds, an ipso-substitution path that proceeds via radical coupling and a Friedel−Crafts-type C–H alkylation via quantum mechanical tunneling, enabled selective access to regioisomeric alkylated arenes. Mechanistic investigations combined with density functional theory (DFT) calculations shed light on the origin of this regioselectivity switch. Remarkably, this process exhibited superior efficiencies, reactivities, and synthetic utilities, and can be performed on the gram scale.
2026, 37(7): 111820
doi: 10.1016/j.cclet.2025.111820
Abstract:
The potential use of ammonia (NH3) as a hydrogen energy carrier has generated significant interest in developing efficient catalysts for producing NH3 under mild conditions. The main obstacles for NH3 synthesis are the activation of the N≡N bond and the desorption of NH3 from the catalyst surface. Here, we report the use of C60 to overcome these challenges. Through electron transfer, migration, and feedback between C60 and Ru, there is a balance of electronic density at the Ru active sites and a shift in the d-band center. This simultaneously satisfies the electronic requirements for enhancing N2 activation while weakening NH3 adsorption, thereby circumventing the bottlenecks in NH3 synthesis under mild conditions. Meanwhile, anchoring of C60 accelerates hydrogen spillover and enhances the exchangeability of hydrogen species in the ZrH2 support, as well as expose a greater number of B5 sites of Ru entities, resulting in the co-optimization of hydrogen migration and nitrogen activation. As a consequence, the NH3 synthesis rate of the C60-Ru/ZrH2 catalyst is approximately twice that of the Ru/ZrH2 catalyst at 400 ℃ and 1 MPa. This study shows that doping C60 represents a fundamentally different approach compared to traditional promoters for catalytic NH3 synthesis. We anticipate that this strategy may be generalized to generate widespread interest in the catalysis of NH3 synthesis.
The potential use of ammonia (NH3) as a hydrogen energy carrier has generated significant interest in developing efficient catalysts for producing NH3 under mild conditions. The main obstacles for NH3 synthesis are the activation of the N≡N bond and the desorption of NH3 from the catalyst surface. Here, we report the use of C60 to overcome these challenges. Through electron transfer, migration, and feedback between C60 and Ru, there is a balance of electronic density at the Ru active sites and a shift in the d-band center. This simultaneously satisfies the electronic requirements for enhancing N2 activation while weakening NH3 adsorption, thereby circumventing the bottlenecks in NH3 synthesis under mild conditions. Meanwhile, anchoring of C60 accelerates hydrogen spillover and enhances the exchangeability of hydrogen species in the ZrH2 support, as well as expose a greater number of B5 sites of Ru entities, resulting in the co-optimization of hydrogen migration and nitrogen activation. As a consequence, the NH3 synthesis rate of the C60-Ru/ZrH2 catalyst is approximately twice that of the Ru/ZrH2 catalyst at 400 ℃ and 1 MPa. This study shows that doping C60 represents a fundamentally different approach compared to traditional promoters for catalytic NH3 synthesis. We anticipate that this strategy may be generalized to generate widespread interest in the catalysis of NH3 synthesis.
2026, 37(7): 111821
doi: 10.1016/j.cclet.2025.111821
Abstract:
Mechanistic studies of the transmetalation of the trifluoromethyl group from an ionic Cu(Ⅰ) complex Q+[Cu(CF3)2]− to a well-defined chlorinated Cu(Ⅲ) complex trans-[Cu(CF3)2(Cl)(CH2CN)]−Q+ was reported. The combined experimental and computational results including kinetics of the process, reactions in the presence of excess chloride salt, or radical scavengers such as TEMPO or 1, 1-diphenylethene (DPE), 1, 4-dinitrobenzene (DNB), strongly support a concerted metathesis pathway.
Mechanistic studies of the transmetalation of the trifluoromethyl group from an ionic Cu(Ⅰ) complex Q+[Cu(CF3)2]− to a well-defined chlorinated Cu(Ⅲ) complex trans-[Cu(CF3)2(Cl)(CH2CN)]−Q+ was reported. The combined experimental and computational results including kinetics of the process, reactions in the presence of excess chloride salt, or radical scavengers such as TEMPO or 1, 1-diphenylethene (DPE), 1, 4-dinitrobenzene (DNB), strongly support a concerted metathesis pathway.
2026, 37(7): 111822
doi: 10.1016/j.cclet.2025.111822
Abstract:
The etiology and pathogenesis of Parkinson's disease (PD) are complex, and its precise pathology remains poorly defined. Emerging evidence suggest that the dysregulation of intracellular copper ion (Cu2+) is tightly associated with PD progression. However, the dynamic interplay between Cu2+ and different stages of PD progression is not fully understood yet. In this study, we developed four Cu2+ fluorescent sensors and evaluated their blood-brain barrier (BBB) penetration efficiency. Among them, PD-Cu-3 exhibited a 62.15% BBB penetration ability and was successfully utilized for real-time monitoring of Cu2+ fluctuations in PD model cells and mice. We first observed an initial increase in Cu2+ level during the early phase PD model cells, followed by a decline in prolonged conditions due to ATP7A-mediated intracellular Cu2+ efflux. Furthermore, in vivo imaging results from PD model mice and brain slices revealed Cu2+ fluctuations across different PD stages, with an elevation in the acute stage and a subsequent reduction in the subacute stage. This study not only provided a new insight into Cu2+ metabolism in PD progression but also help understanding of PD pathology and searching potential therapeutic approaches.
The etiology and pathogenesis of Parkinson's disease (PD) are complex, and its precise pathology remains poorly defined. Emerging evidence suggest that the dysregulation of intracellular copper ion (Cu2+) is tightly associated with PD progression. However, the dynamic interplay between Cu2+ and different stages of PD progression is not fully understood yet. In this study, we developed four Cu2+ fluorescent sensors and evaluated their blood-brain barrier (BBB) penetration efficiency. Among them, PD-Cu-3 exhibited a 62.15% BBB penetration ability and was successfully utilized for real-time monitoring of Cu2+ fluctuations in PD model cells and mice. We first observed an initial increase in Cu2+ level during the early phase PD model cells, followed by a decline in prolonged conditions due to ATP7A-mediated intracellular Cu2+ efflux. Furthermore, in vivo imaging results from PD model mice and brain slices revealed Cu2+ fluctuations across different PD stages, with an elevation in the acute stage and a subsequent reduction in the subacute stage. This study not only provided a new insight into Cu2+ metabolism in PD progression but also help understanding of PD pathology and searching potential therapeutic approaches.
2026, 37(7): 111823
doi: 10.1016/j.cclet.2025.111823
Abstract:
Switchable chirality in confined environments is central to biological regulation, yet artificial systems enabling reversible chirality control remain challenging. Herein, we report a redox-responsive supramolecular chirality system constructed from phenylalanine-modified viologen (d/l-PheVio⋅2Br) and cucurbit[8]uril (CB[8]) in aqueous solution. The formation of 1:1 host-guest complex triggers pronounced chirality amplification, evident from characteristic induced circular dichroism (ICD) signals. Upon chemical reduction, these ICD signals vanish abruptly, replaced by unusual CD signals from viologen radical cations, demonstrating chirality transfer enabled by the confined environment. The redox-switchable process exhibits exceptional reversibility and repeatability over multiple cycles. These findings deepen our understanding of supramolecular chirality arising from host-guest complexation in confined spaces at the molecular level, offering new perspectives for designing stimuli-responsive chiral materials.
Switchable chirality in confined environments is central to biological regulation, yet artificial systems enabling reversible chirality control remain challenging. Herein, we report a redox-responsive supramolecular chirality system constructed from phenylalanine-modified viologen (d/l-PheVio⋅2Br) and cucurbit[8]uril (CB[8]) in aqueous solution. The formation of 1:1 host-guest complex triggers pronounced chirality amplification, evident from characteristic induced circular dichroism (ICD) signals. Upon chemical reduction, these ICD signals vanish abruptly, replaced by unusual CD signals from viologen radical cations, demonstrating chirality transfer enabled by the confined environment. The redox-switchable process exhibits exceptional reversibility and repeatability over multiple cycles. These findings deepen our understanding of supramolecular chirality arising from host-guest complexation in confined spaces at the molecular level, offering new perspectives for designing stimuli-responsive chiral materials.
2026, 37(7): 111833
doi: 10.1016/j.cclet.2025.111833
Abstract:
Ultra-thick electrodes (UTEs) hold great promise for high-energy-density lithium-ion batteries (LIBs), yet the practical application is hindered by challenges in precise fabrication and reaction kinetics modification. In this contribution, a solvent-free processing method is introduced to tailor UTEs through layer-by-layer fabrication with positive, uniform, and negative gradient porosity from the separator side to the current collector side, denoted as P-UTEs, U-UTEs, and N-UTEs. In contrast to conventional slurry coating, the proposed solvent-free approach effectively circumvents capillary stress, thereby facilitating the fabrication of crack-free UTEs (> 300 µm) while simultaneously mitigating environmental toxicity concerns. The three-layer N-UTEs (> 220 µm) with a gradient porosity of (~34%, ~31%, ~27%) deliver an exceeding areal capacity over 5 mAh/cm2 at 0.29 mA/cm2 and a high-capacity retention over 62% at 2.9 mA/cm2, indicating a favorable balance between the areal capacity and the high-rate behavior. Detailed mechanistic simulations reveal that the multi-center reaction pathways enabled by enhanced ionic accessibility in N-UTEs significantly improve reaction kinetics. This work offers new insights into the gradient porosity tailoring for high-areal-capacity and high-rate UTEs for the next generation LIBs.
Ultra-thick electrodes (UTEs) hold great promise for high-energy-density lithium-ion batteries (LIBs), yet the practical application is hindered by challenges in precise fabrication and reaction kinetics modification. In this contribution, a solvent-free processing method is introduced to tailor UTEs through layer-by-layer fabrication with positive, uniform, and negative gradient porosity from the separator side to the current collector side, denoted as P-UTEs, U-UTEs, and N-UTEs. In contrast to conventional slurry coating, the proposed solvent-free approach effectively circumvents capillary stress, thereby facilitating the fabrication of crack-free UTEs (> 300 µm) while simultaneously mitigating environmental toxicity concerns. The three-layer N-UTEs (> 220 µm) with a gradient porosity of (~34%, ~31%, ~27%) deliver an exceeding areal capacity over 5 mAh/cm2 at 0.29 mA/cm2 and a high-capacity retention over 62% at 2.9 mA/cm2, indicating a favorable balance between the areal capacity and the high-rate behavior. Detailed mechanistic simulations reveal that the multi-center reaction pathways enabled by enhanced ionic accessibility in N-UTEs significantly improve reaction kinetics. This work offers new insights into the gradient porosity tailoring for high-areal-capacity and high-rate UTEs for the next generation LIBs.
2026, 37(7): 111849
doi: 10.1016/j.cclet.2025.111849
Abstract:
Developing metal matrix composites with low thermal expansion yet high thermal conductivity (λ) has been an ongoing effort in electronic packaging materials due to the growing demand for high-power applications. However, progress has been hindered by the insufficient thermal expansion suppression of conventional low thermal expansion reinforcements or the low λ of negative thermal expansion reinforcements. In this study, this challenge is overcome via a multiphase design strategy using ZrW2O8 and SiC to co-reinforce the aluminum matrix composites. This approach simultaneously combines the advantages of the ZrW2O8 for controlling the coefficient of thermal expansion (CTE) and SiC for improving λ. A controlled CTE-λ balance (6.22–9.7 × 10–6 K-1, 63.1–131.1 W/mK) can be obtained by varying the volume ratio of ZrW2O8 to SiC. The CTE of this composite is significantly lower than that of the 50 vol% SiC/Al composite, while its CTE is approximately equal to that of the 45 vol% ZrW2O8/Al composite but with a twofold increase in λ. The good thermal performance of this composite can be attributed to the strong interfacial interactions of SiC and the tailored variation in CTE. Furthermore, simulation and experimental results revealed that the residual stress can be effectively relieved through this strategy. This work presents a straightforward structural design and an effective pathway to manufacture composites with excellent integrated properties.
Developing metal matrix composites with low thermal expansion yet high thermal conductivity (λ) has been an ongoing effort in electronic packaging materials due to the growing demand for high-power applications. However, progress has been hindered by the insufficient thermal expansion suppression of conventional low thermal expansion reinforcements or the low λ of negative thermal expansion reinforcements. In this study, this challenge is overcome via a multiphase design strategy using ZrW2O8 and SiC to co-reinforce the aluminum matrix composites. This approach simultaneously combines the advantages of the ZrW2O8 for controlling the coefficient of thermal expansion (CTE) and SiC for improving λ. A controlled CTE-λ balance (6.22–9.7 × 10–6 K-1, 63.1–131.1 W/mK) can be obtained by varying the volume ratio of ZrW2O8 to SiC. The CTE of this composite is significantly lower than that of the 50 vol% SiC/Al composite, while its CTE is approximately equal to that of the 45 vol% ZrW2O8/Al composite but with a twofold increase in λ. The good thermal performance of this composite can be attributed to the strong interfacial interactions of SiC and the tailored variation in CTE. Furthermore, simulation and experimental results revealed that the residual stress can be effectively relieved through this strategy. This work presents a straightforward structural design and an effective pathway to manufacture composites with excellent integrated properties.
2026, 37(7): 111922
doi: 10.1016/j.cclet.2025.111922
Abstract:
α-d-Fructofuranoside derivatives are prevalent in natural products, exhibiting diverse bioactivities. Herein, a stereoselective glycosylation method for synthesizing α-d-fructofuranosides using fructofuranosyl fluorides as donors is described. Glycosylation of 1,3,4,6-tetra-O-benzoyl-2-d-fructofuranosyl fluoride, promoted by tris(pentafluorophenyl)borane, proved highly effective, yielding glycosylation products in high yields (up to 98%) with primary alcohols, thiols, N- and C-nucleophiles. Furthermore, β-(2→6) cyclodisaccharide di-d-fructose-2,6′:6,2′-dianhydride (DFA Ⅳ), a disaccharide enzymatically derived from levan, was chemically synthesized through orthogonal glycosylation reactions and hydrogen-bond-mediated aglycone delivery involving thioglycosides and glycosyl fluorides for the first time.
α-d-Fructofuranoside derivatives are prevalent in natural products, exhibiting diverse bioactivities. Herein, a stereoselective glycosylation method for synthesizing α-d-fructofuranosides using fructofuranosyl fluorides as donors is described. Glycosylation of 1,3,4,6-tetra-O-benzoyl-2-d-fructofuranosyl fluoride, promoted by tris(pentafluorophenyl)borane, proved highly effective, yielding glycosylation products in high yields (up to 98%) with primary alcohols, thiols, N- and C-nucleophiles. Furthermore, β-(2→6) cyclodisaccharide di-d-fructose-2,6′:6,2′-dianhydride (DFA Ⅳ), a disaccharide enzymatically derived from levan, was chemically synthesized through orthogonal glycosylation reactions and hydrogen-bond-mediated aglycone delivery involving thioglycosides and glycosyl fluorides for the first time.
2026, 37(7): 111939
doi: 10.1016/j.cclet.2025.111939
Abstract:
The carbon-centered radical induced C‒C bond cleavage in strained cyclopropane is a well-known process. However, achieving similar transformations in unstrained rings is still challenging. Herein, a novel inexpensive Cu-catalyzed strategy for the carbon-centered radical-mediated ring-opening/amination or esterification cascade of unstrained α-haloalkyl cycloketone derivatives is presented. Differ from the classical Dowd-Beckwith ring expansion reaction, a ring opening cascade occurred successfully under a simple copper/base catalytic system, yielding useful distal unsaturated amides and esters in good to excellent yields. Mechanistic studies and DFT calculations indicate that the halogen-bonding interaction between halide and base is crucial for the activation of the C‒Br bond. Furthermore, the formation of a bicyclic Cu-complex via bi-dentate coordination, including O–Cu–•CH2, seems to be a crucial factor that promotes ring opening rather than the conventional ring expansion. This work would not only bring new vitality for the radical-mediated C‒C bond cleavage, but also highlight the potential of protocol for synthesizing bioactive molecules.
The carbon-centered radical induced C‒C bond cleavage in strained cyclopropane is a well-known process. However, achieving similar transformations in unstrained rings is still challenging. Herein, a novel inexpensive Cu-catalyzed strategy for the carbon-centered radical-mediated ring-opening/amination or esterification cascade of unstrained α-haloalkyl cycloketone derivatives is presented. Differ from the classical Dowd-Beckwith ring expansion reaction, a ring opening cascade occurred successfully under a simple copper/base catalytic system, yielding useful distal unsaturated amides and esters in good to excellent yields. Mechanistic studies and DFT calculations indicate that the halogen-bonding interaction between halide and base is crucial for the activation of the C‒Br bond. Furthermore, the formation of a bicyclic Cu-complex via bi-dentate coordination, including O–Cu–•CH2, seems to be a crucial factor that promotes ring opening rather than the conventional ring expansion. This work would not only bring new vitality for the radical-mediated C‒C bond cleavage, but also highlight the potential of protocol for synthesizing bioactive molecules.
2026, 37(7): 111940
doi: 10.1016/j.cclet.2025.111940
Abstract:
gem–Difluorovinyl compounds and silicon-containing compounds are valuable structural units in organic and medicinal chemistry. However, they are mostly found separately in most compounds. In this study, we present a photocatalytic approach for the synthesis of gem–difluorovinylsilanes, using readily accessible silylboronic pinacol esters as reagents. Through a radical transfer strategy, this method overcomes the limitation of their high oxidation potential. Biological assays further confirmed that several target compounds exhibited moderate to potent antifungal activity against plant pathogens, including Botrytis cinerea, Setosphaeria turcica and Rhizoctonia solani.
gem–Difluorovinyl compounds and silicon-containing compounds are valuable structural units in organic and medicinal chemistry. However, they are mostly found separately in most compounds. In this study, we present a photocatalytic approach for the synthesis of gem–difluorovinylsilanes, using readily accessible silylboronic pinacol esters as reagents. Through a radical transfer strategy, this method overcomes the limitation of their high oxidation potential. Biological assays further confirmed that several target compounds exhibited moderate to potent antifungal activity against plant pathogens, including Botrytis cinerea, Setosphaeria turcica and Rhizoctonia solani.
2026, 37(7): 111941
doi: 10.1016/j.cclet.2025.111941
Abstract:
The stereodivergent coupling via photoredox/transition metal catalysis has emerged as a powerful tool to construct diverse alkenes in both E and Z configurations. Despite well-established catalytic systems involving late transition metals, the early transition metal catalyzed stereodivergent synthesis of alkenes still remains underdeveloped. Herein in this work, a stereodivergent reductive C(sp2)-C(sp3) coupling between cycloketone oximes and vinyl halides has been achieved by tunable photoredox/Ti dual catalysis, providing a facile access to a broad scope of cyano-substituted (fluoro)alkenes with high efficiency and controlled E/Z selectivity. Several products exhibited promising antifungal activities.
The stereodivergent coupling via photoredox/transition metal catalysis has emerged as a powerful tool to construct diverse alkenes in both E and Z configurations. Despite well-established catalytic systems involving late transition metals, the early transition metal catalyzed stereodivergent synthesis of alkenes still remains underdeveloped. Herein in this work, a stereodivergent reductive C(sp2)-C(sp3) coupling between cycloketone oximes and vinyl halides has been achieved by tunable photoredox/Ti dual catalysis, providing a facile access to a broad scope of cyano-substituted (fluoro)alkenes with high efficiency and controlled E/Z selectivity. Several products exhibited promising antifungal activities.
2026, 37(7): 111943
doi: 10.1016/j.cclet.2025.111943
Abstract:
Functionalized C−N atropisomers has become more and more attractive and found wide applications in natural products, drug molecules, as well as in chiral ligands. As a complement to asymmetric de novo ring formation and cross C−N coupling methods, the resolution approach demonstrates uniquely advantageous, which can progressively introduce the key functional groups and generate enantiomeric excess. Herein, we have developed an enzymatic tool for the construction of difunctionalized C−N atropisomers via lipase-catalyzed desymmetrization and kinetic resolution of N-naphthol-carbazoles. Acetylacetone was found as an efficient proton donor under the catalysis of LPL311-polyester. The enantioselective deacylation process has exhibited good functional group tolerance to produce enantioenriched C−N atropisomers with good to excellent enantioselectivity, in which the pre-installed hydroxyl functionality on the naphthene ring and the hydroxyl functionality on the carbazole ring generated after hydrolysis together provide feasibility for subsequent transformations.
Functionalized C−N atropisomers has become more and more attractive and found wide applications in natural products, drug molecules, as well as in chiral ligands. As a complement to asymmetric de novo ring formation and cross C−N coupling methods, the resolution approach demonstrates uniquely advantageous, which can progressively introduce the key functional groups and generate enantiomeric excess. Herein, we have developed an enzymatic tool for the construction of difunctionalized C−N atropisomers via lipase-catalyzed desymmetrization and kinetic resolution of N-naphthol-carbazoles. Acetylacetone was found as an efficient proton donor under the catalysis of LPL311-polyester. The enantioselective deacylation process has exhibited good functional group tolerance to produce enantioenriched C−N atropisomers with good to excellent enantioselectivity, in which the pre-installed hydroxyl functionality on the naphthene ring and the hydroxyl functionality on the carbazole ring generated after hydrolysis together provide feasibility for subsequent transformations.
2026, 37(7): 111948
doi: 10.1016/j.cclet.2025.111948
Abstract:
The pathological protein α-synuclein (α-Syn) aggregates are considered a key toxic substance responsible for the degeneration of dopaminergic neurons in Parkinson's disease (PD). Clearing these pathological aggregates can potentially control PD progression at its source. However, conventional drug delivery systems face significant challenges, including the blood-brain barrier (BBB) and lack of tissue-specific targeting. To address this, we developed a core-shell hybrid system, named RExo-si-TN-T10, for the co-delivery of triptolide (T10) and small interfering RNA targeting α-Syn (siSNCA). This system comprises two components: an outer shell of exosomes (RExo) derived from BV2 microglial cells and modified with rabies virus glycoprotein peptide (RVG), and an inner core of a nanomicelle composed of phenylboronic acid derivatives: 4-Nitrophenyl 4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl) benzyl carbonate (NBC) and trimethyl chitosan (TMC) for co-delivering gene and small-molecule drugs. Furthermore, we utilized cellular nanoporation (CNP) technology to significantly enhance exosome yield and transfection efficiency. This innovative nano-scavenger effectively eliminates α-Syn aggregates and reduces their cytotoxic effects in PD-affected neurons. Following treatment with RExo-si-TN-T10, we observed significant improvement in the motor behavior of PD mice. Our findings suggest that RExo-si-TN-T10 holds promise as a therapeutic platform for PD.
The pathological protein α-synuclein (α-Syn) aggregates are considered a key toxic substance responsible for the degeneration of dopaminergic neurons in Parkinson's disease (PD). Clearing these pathological aggregates can potentially control PD progression at its source. However, conventional drug delivery systems face significant challenges, including the blood-brain barrier (BBB) and lack of tissue-specific targeting. To address this, we developed a core-shell hybrid system, named RExo-si-TN-T10, for the co-delivery of triptolide (T10) and small interfering RNA targeting α-Syn (siSNCA). This system comprises two components: an outer shell of exosomes (RExo) derived from BV2 microglial cells and modified with rabies virus glycoprotein peptide (RVG), and an inner core of a nanomicelle composed of phenylboronic acid derivatives: 4-Nitrophenyl 4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl) benzyl carbonate (NBC) and trimethyl chitosan (TMC) for co-delivering gene and small-molecule drugs. Furthermore, we utilized cellular nanoporation (CNP) technology to significantly enhance exosome yield and transfection efficiency. This innovative nano-scavenger effectively eliminates α-Syn aggregates and reduces their cytotoxic effects in PD-affected neurons. Following treatment with RExo-si-TN-T10, we observed significant improvement in the motor behavior of PD mice. Our findings suggest that RExo-si-TN-T10 holds promise as a therapeutic platform for PD.
2026, 37(7): 111961
doi: 10.1016/j.cclet.2025.111961
Abstract:
The fentanyl (Fen) analogs-related drug crisis is a global focus that has badly affected social stability. In view of multitudinous overdose deaths, there is a great need for a portable and sensitive analytical approach that can quickly discriminate these dangerous recreational substances. Herein, an extended biphenarene-based fluorescence displacement sensor assay was constructed by integrating two reporter pairs, where terphen[3]arene sulfate and quaterphen[3]arene sulfate act as receptors, and rhodamine 123 acts as the optimal indicator. The formed supramolecular assay was able to completely classify four analogs, including Fen, 3-methylfentanyl, sufentanil and remifentanil in aqueous phosphate buffered saline, artificial urine, mouse plasma, or even real urine sample from model mice. Moreover, mixed samples containing different proportions of cocaine, heroin and ketamine could also be discriminated with 100% accuracy.
The fentanyl (Fen) analogs-related drug crisis is a global focus that has badly affected social stability. In view of multitudinous overdose deaths, there is a great need for a portable and sensitive analytical approach that can quickly discriminate these dangerous recreational substances. Herein, an extended biphenarene-based fluorescence displacement sensor assay was constructed by integrating two reporter pairs, where terphen[3]arene sulfate and quaterphen[3]arene sulfate act as receptors, and rhodamine 123 acts as the optimal indicator. The formed supramolecular assay was able to completely classify four analogs, including Fen, 3-methylfentanyl, sufentanil and remifentanil in aqueous phosphate buffered saline, artificial urine, mouse plasma, or even real urine sample from model mice. Moreover, mixed samples containing different proportions of cocaine, heroin and ketamine could also be discriminated with 100% accuracy.
2026, 37(7): 111962
doi: 10.1016/j.cclet.2025.111962
Abstract:
In this paper, a novel multicolor-responsive fluorescent probe for the rapid and sensitive detection of persulfate ions (S2O82-), KT@Q[8], is constructed via host-guest interactions between cucurbit[8]uril (Q[8]) and 3,6-bis[4-(4-bromophenyl)pyridinium]-carbazole dichloride (KT). Upon interaction with S2O82-, the KT@Q[8] probe exhibits a fluorescence emission blue shift concurrent with a fluorescence color transition gradually from yellow to green. Notably, the probe demonstrates high selectivity for S2O82- even in the presence of competing anions and sulphur-containing metal salts, achieving a detection limit of 0.38 μmol/L. When integrated with smartphone-based RGB analysis, this probe enables rapid visual quantification of S2O82- without requiring sophisticated instrumentation, and can be effectively used to detect S2O82- in tap water, lake water, honey, and white wine. Furthermore, machine learning algorithms enhanced predictive accuracy during data analysis. Overall, this work not only advances a practical approach for persulfate monitoring but also expands the application range of cucurbituril-based fluorescence supramolecular assemblies.
In this paper, a novel multicolor-responsive fluorescent probe for the rapid and sensitive detection of persulfate ions (S2O82-), KT@Q[8], is constructed via host-guest interactions between cucurbit[8]uril (Q[8]) and 3,6-bis[4-(4-bromophenyl)pyridinium]-carbazole dichloride (KT). Upon interaction with S2O82-, the KT@Q[8] probe exhibits a fluorescence emission blue shift concurrent with a fluorescence color transition gradually from yellow to green. Notably, the probe demonstrates high selectivity for S2O82- even in the presence of competing anions and sulphur-containing metal salts, achieving a detection limit of 0.38 μmol/L. When integrated with smartphone-based RGB analysis, this probe enables rapid visual quantification of S2O82- without requiring sophisticated instrumentation, and can be effectively used to detect S2O82- in tap water, lake water, honey, and white wine. Furthermore, machine learning algorithms enhanced predictive accuracy during data analysis. Overall, this work not only advances a practical approach for persulfate monitoring but also expands the application range of cucurbituril-based fluorescence supramolecular assemblies.
Hierarchical confinement achieving cascade phosphorescence resonance energy transfer and application
2026, 37(7): 111964
doi: 10.1016/j.cclet.2025.111964
Abstract:
Herein, we report morphology and luminescence tunable supramolecule containing tetracation 6-bromoisoquinoline modified tetraphenylbenzene (TQ), cucurbit[8]uril (CB[8]), β-cyclodextrin grafted hyaluronic acid (HACD), and two dyes (SR101, Cy5), which can lead to cascade efficient phosphorescence resonance energy transfer (PRET) through multi-scale supramolecular space confinement to achieve longlived multi-wavelength emission, especially near-infrared (NIR) luminescence. The initial unit TQ was assembled to form a green phosphorescent 3D supramolecular organic framework (SOF) under the activation of CB[8] confinement and then co-assembled with polysaccharide HACD to form phosphorescence extended long-lifetime (670.3 μs) 3D nanoparticles. This hierarchical confinement boosted phosphorescence supramolecule can act as the donor to achieve efficient energy transfer from phosphor to the dye SR101, giving long-lived luminescence at 615 nm, which can be employed as a transit depot and further encapsulate secondary acceptor Cy5, achieving efficient delayed NIR fluorescence at 680 nm, and was used as phosphorescence logic gate and NIR imaging reagent.
Herein, we report morphology and luminescence tunable supramolecule containing tetracation 6-bromoisoquinoline modified tetraphenylbenzene (TQ), cucurbit[8]uril (CB[8]), β-cyclodextrin grafted hyaluronic acid (HACD), and two dyes (SR101, Cy5), which can lead to cascade efficient phosphorescence resonance energy transfer (PRET) through multi-scale supramolecular space confinement to achieve longlived multi-wavelength emission, especially near-infrared (NIR) luminescence. The initial unit TQ was assembled to form a green phosphorescent 3D supramolecular organic framework (SOF) under the activation of CB[8] confinement and then co-assembled with polysaccharide HACD to form phosphorescence extended long-lifetime (670.3 μs) 3D nanoparticles. This hierarchical confinement boosted phosphorescence supramolecule can act as the donor to achieve efficient energy transfer from phosphor to the dye SR101, giving long-lived luminescence at 615 nm, which can be employed as a transit depot and further encapsulate secondary acceptor Cy5, achieving efficient delayed NIR fluorescence at 680 nm, and was used as phosphorescence logic gate and NIR imaging reagent.
2026, 37(7): 111965
doi: 10.1016/j.cclet.2025.111965
Abstract:
Balsalazide disodium is an effective drug for alleviating ulcerative colitis. It slowly releases 5-aminosalicylic acid in the intestine. The traditional synthesis methods of balsalazide disodium exhibit high risk, high pollution and low efficiency concern. Thus, we innovatively develop a four-step route for the large-scale production of balsalazide disodium in continuous flow. In this work, methyl 3-aminopropionate hydrochloride was subjected to acylation and hydrolysis reactions to obtain the nitro intermediate with a selectivity of 99.55%. Micro-hydrogenation reactor filled with Raney Ni catalyzed three-phase reaction improves conversion and selectivity. In the diazotization and azo coupling reactions, the optimal equivalents of salicylic acid and base were determined. With the aid of response surface methodology, the influences of reaction temperature and residence time on yield were systematically investigated. Under the optimum conditions, the experimental yields coincided with the predicted yields. Compared to batch experiments, the continuous process achieved a total yield of 66.1% and a purity of 99.63% in 13.1 min.
Balsalazide disodium is an effective drug for alleviating ulcerative colitis. It slowly releases 5-aminosalicylic acid in the intestine. The traditional synthesis methods of balsalazide disodium exhibit high risk, high pollution and low efficiency concern. Thus, we innovatively develop a four-step route for the large-scale production of balsalazide disodium in continuous flow. In this work, methyl 3-aminopropionate hydrochloride was subjected to acylation and hydrolysis reactions to obtain the nitro intermediate with a selectivity of 99.55%. Micro-hydrogenation reactor filled with Raney Ni catalyzed three-phase reaction improves conversion and selectivity. In the diazotization and azo coupling reactions, the optimal equivalents of salicylic acid and base were determined. With the aid of response surface methodology, the influences of reaction temperature and residence time on yield were systematically investigated. Under the optimum conditions, the experimental yields coincided with the predicted yields. Compared to batch experiments, the continuous process achieved a total yield of 66.1% and a purity of 99.63% in 13.1 min.
2026, 37(7): 111966
doi: 10.1016/j.cclet.2025.111966
Abstract:
Efficient macrocycle synthesis remains a persistently pursued objective in supramolecular chemistry. In this work, a series of chiral macrocycles (TBCHMs) incorporating Tröger's base were synthesized via imine condensation reactions from Tröger's base (TB) aldehyde derivatives and cyclohexane-1,2-diamines (CHDA). Gram-scale quantities of crystalline macrocycles were directly obtained during the process of their reaction. Precise modulation of macrocycle structural morphology was achieved by varying the chiral configuration of the components. Notably, chiral self-sorting was realized in these reaction systems, driven by the energy difference between diastereomers and their selective precipitation as crystals. This work might open up new insights for the modular preparation of chiral macrocycles based on dynamic covalent chemistry (DCC).
Efficient macrocycle synthesis remains a persistently pursued objective in supramolecular chemistry. In this work, a series of chiral macrocycles (TBCHMs) incorporating Tröger's base were synthesized via imine condensation reactions from Tröger's base (TB) aldehyde derivatives and cyclohexane-1,2-diamines (CHDA). Gram-scale quantities of crystalline macrocycles were directly obtained during the process of their reaction. Precise modulation of macrocycle structural morphology was achieved by varying the chiral configuration of the components. Notably, chiral self-sorting was realized in these reaction systems, driven by the energy difference between diastereomers and their selective precipitation as crystals. This work might open up new insights for the modular preparation of chiral macrocycles based on dynamic covalent chemistry (DCC).
2026, 37(7): 111967
doi: 10.1016/j.cclet.2025.111967
Abstract:
Multi-resonance thermally activated delayed fluorescence (MR-TADF) materials have attracted growing interest for their potential to achieve high color purity and efficiency in organic light-emitting diode (OLED) applications. However, their key performance parameters, including photoluminescence wavelength (PL), full width at half-maximum (FWHM), and photoluminescence quantum yield (PLQY), are highly structure-dependent, presenting challenges for high-throughput screening and efficient design. In this work, we propose a structure-aware ensemble learning model (BNML) that integrates molecular access system (MACCS) fingerprints, fingerprint2 (FP2) fingerprints, and molecular descriptors (MDs) to predict photophysical properties of MR-TADF materials. The model shows strong regression performance under small-data (415) conditions and achieves nearly 100% prediction accuracy (100%, 100%, and 96%, respectively) within a specific range of values. By incorporating SHapley Additive exPlanations (SHAP) analysis, the model reveals interpretable contributions of donor fragments and π-conjugation to the predicted properties. Guided by this analysis, fifteen novel MR-TADF compounds were designed, among which seven were successfully synthesized and validated, showing strong agreement with the predicted values (accuracy: predict/true, 21/20). This work provides a reliable strategy for intelligent design and rapid evaluation of MR-TADF compounds, offering a new approach for structure-property modeling in complex emission systems.
Multi-resonance thermally activated delayed fluorescence (MR-TADF) materials have attracted growing interest for their potential to achieve high color purity and efficiency in organic light-emitting diode (OLED) applications. However, their key performance parameters, including photoluminescence wavelength (PL), full width at half-maximum (FWHM), and photoluminescence quantum yield (PLQY), are highly structure-dependent, presenting challenges for high-throughput screening and efficient design. In this work, we propose a structure-aware ensemble learning model (BNML) that integrates molecular access system (MACCS) fingerprints, fingerprint2 (FP2) fingerprints, and molecular descriptors (MDs) to predict photophysical properties of MR-TADF materials. The model shows strong regression performance under small-data (415) conditions and achieves nearly 100% prediction accuracy (100%, 100%, and 96%, respectively) within a specific range of values. By incorporating SHapley Additive exPlanations (SHAP) analysis, the model reveals interpretable contributions of donor fragments and π-conjugation to the predicted properties. Guided by this analysis, fifteen novel MR-TADF compounds were designed, among which seven were successfully synthesized and validated, showing strong agreement with the predicted values (accuracy: predict/true, 21/20). This work provides a reliable strategy for intelligent design and rapid evaluation of MR-TADF compounds, offering a new approach for structure-property modeling in complex emission systems.
2026, 37(7): 112000
doi: 10.1016/j.cclet.2025.112000
Abstract:
Multi-substituted pyrrolidine and piperidine N-heterocycles are the top scaffolds of clinical drugs, but syntheses of these scaffolds are far from trivial. Herein, we report a highly enantioselective protocol for the synthesis of 5- and 6-membered cyclic nitrones via Pd-catalyzed cyclization coupling of alkenyl oximes with aryl, alkenyl and alkynyl (pseudo)halides enabled by chiral sulfonamidephosphine (SadPhos) ligands. These cyclic nitrones products, besides their significance per ser, can be facilely converted to multi-substituted pyrrolidines and piperidines by simple operations. This study also represents the first example of two-component catalytic asymmetric synthesis of cyclic nitrones and provides important insights for further development of enantioselective heterocyclization reaction and processes involving multiple selectivity issues.
Multi-substituted pyrrolidine and piperidine N-heterocycles are the top scaffolds of clinical drugs, but syntheses of these scaffolds are far from trivial. Herein, we report a highly enantioselective protocol for the synthesis of 5- and 6-membered cyclic nitrones via Pd-catalyzed cyclization coupling of alkenyl oximes with aryl, alkenyl and alkynyl (pseudo)halides enabled by chiral sulfonamidephosphine (SadPhos) ligands. These cyclic nitrones products, besides their significance per ser, can be facilely converted to multi-substituted pyrrolidines and piperidines by simple operations. This study also represents the first example of two-component catalytic asymmetric synthesis of cyclic nitrones and provides important insights for further development of enantioselective heterocyclization reaction and processes involving multiple selectivity issues.
2026, 37(7): 112118
doi: 10.1016/j.cclet.2025.112118
Abstract:
At present, electromagnetic wave absorbing materials provide an effective solution to the electromagnetic pollution generated by electronic devices. However, materials with a single function can no longer meet practical requirements. Therefore, reduced graphene oxide/Fe3O4 composites were prepared via a combined process involving sol-gel, click chemistry reaction (thiol-ene reaction), and reduction. The results demonstrated that Fe3O4 was covalently grafted onto graphene oxide (GO), which significantly influenced the morphology, electrical conductivity, and electromagnetic wave absorption performance of the composite. When the mass ratio of GO to modified Fe3O4 was 1:1, the composite G2-Fe exhibited optimal impedance matching and the best electromagnetic wave absorption performance. The minimum reflection loss (RLmin) reached -42.0 dB at 4.91 GHz. When the thickness was 2.0 mm, the maximum effective absorption bandwidth (RL < -10 dB) was 4.85 GHz. Moreover, the composite also displayed excellent thermal conductivity and corrosion resistance. The thermal conductivity of the composite material was maintained above 1.486 W m-1 K-1. In a 3.5 wt% saline solution, the composite showed a low corrosion current (3.07 × 10–5 A) and a high corrosion potential (-0.110 V). This study not only achieved structural regulation of the composite through covalent grafting of modified Fe3O4 on GO, but also offered valuable insights for the design of multifunctional materials integrating electromagnetic wave absorption, thermal conduction, and corrosion resistance properties.
At present, electromagnetic wave absorbing materials provide an effective solution to the electromagnetic pollution generated by electronic devices. However, materials with a single function can no longer meet practical requirements. Therefore, reduced graphene oxide/Fe3O4 composites were prepared via a combined process involving sol-gel, click chemistry reaction (thiol-ene reaction), and reduction. The results demonstrated that Fe3O4 was covalently grafted onto graphene oxide (GO), which significantly influenced the morphology, electrical conductivity, and electromagnetic wave absorption performance of the composite. When the mass ratio of GO to modified Fe3O4 was 1:1, the composite G2-Fe exhibited optimal impedance matching and the best electromagnetic wave absorption performance. The minimum reflection loss (RLmin) reached -42.0 dB at 4.91 GHz. When the thickness was 2.0 mm, the maximum effective absorption bandwidth (RL < -10 dB) was 4.85 GHz. Moreover, the composite also displayed excellent thermal conductivity and corrosion resistance. The thermal conductivity of the composite material was maintained above 1.486 W m-1 K-1. In a 3.5 wt% saline solution, the composite showed a low corrosion current (3.07 × 10–5 A) and a high corrosion potential (-0.110 V). This study not only achieved structural regulation of the composite through covalent grafting of modified Fe3O4 on GO, but also offered valuable insights for the design of multifunctional materials integrating electromagnetic wave absorption, thermal conduction, and corrosion resistance properties.
2026, 37(7): 112134
doi: 10.1016/j.cclet.2025.112134
Abstract:
Bergenin (BG), a bioactive coumarin derivative, suffers from poor solubility and low oral bioavailability, restricting its clinical potential. To overcome these limitations, we developed a lipid prodrug strategy by conjugating BG with bioactive fatty acids of different chain lengths (6C, 12C, 18C) via ester bonds, formulating the conjugates into solid lipid nanoparticles (SLNs), and systematically investigating the structure–activity relationship. Fatty acid conjugation not only enhanced lipophilicity, lipid matrix compatibility, and enzymatic stability but also imparted distinct biological effects that shaped oral absorption. Stearic acids (18C) conferred strong resistance to enzymatic hydrolysis, whereas lauric acid (12C) offered the most favorable balance in improving drug loading, stability, and membrane permeability. Pharmacokinetic studies in rats demonstrated that 12C-BG SLNs achieved the greatest enhancement in oral bioavailability, with an 8.6-fold increase over BG-SLNs and more than 40-fold improvement relative to reported suspensions and phospholipid solid dispersions. Mechanistic studies indicated that absorption was primarily driven by prodrug monomers released during intestinal lipolysis, with a minor contribution from undigested nanoparticles, and moreover the fatty acid chain length strongly influenced cellular permeability and systemic exposure. Collectively, these results underscore the critical role of bioactive fatty acids as conjugating groups in modulating prodrug fate and highlight a promising platform for enhancing the oral delivery of poorly soluble phytochemicals.
Bergenin (BG), a bioactive coumarin derivative, suffers from poor solubility and low oral bioavailability, restricting its clinical potential. To overcome these limitations, we developed a lipid prodrug strategy by conjugating BG with bioactive fatty acids of different chain lengths (6C, 12C, 18C) via ester bonds, formulating the conjugates into solid lipid nanoparticles (SLNs), and systematically investigating the structure–activity relationship. Fatty acid conjugation not only enhanced lipophilicity, lipid matrix compatibility, and enzymatic stability but also imparted distinct biological effects that shaped oral absorption. Stearic acids (18C) conferred strong resistance to enzymatic hydrolysis, whereas lauric acid (12C) offered the most favorable balance in improving drug loading, stability, and membrane permeability. Pharmacokinetic studies in rats demonstrated that 12C-BG SLNs achieved the greatest enhancement in oral bioavailability, with an 8.6-fold increase over BG-SLNs and more than 40-fold improvement relative to reported suspensions and phospholipid solid dispersions. Mechanistic studies indicated that absorption was primarily driven by prodrug monomers released during intestinal lipolysis, with a minor contribution from undigested nanoparticles, and moreover the fatty acid chain length strongly influenced cellular permeability and systemic exposure. Collectively, these results underscore the critical role of bioactive fatty acids as conjugating groups in modulating prodrug fate and highlight a promising platform for enhancing the oral delivery of poorly soluble phytochemicals.
2026, 37(7): 112150
doi: 10.1016/j.cclet.2025.112150
Abstract:
Tandem CO2 electroreduction integrated with carbonylation reactions offers a promising pathway for transforming greenhouse gases into valuable chemical products. The development of efficient CO2–to–CO electrocatalysts operational across wide potential ranges is crucial to address renewable energy fluctuations and facilitate integrated cascade systems. Herein, a Ni single–atom catalyst (SAC) with sulfur doping in the second shell of Ni–N4 is reported. In situ measurements and theoretical calculations demonstrate that the incorporation S atoms not only modulates the electronic configuration of Ni active sites but also enhances H2O adsorption, enabling rapid CO2 hydrogenation into *COOH intermediates even at high potentials. Consequently, the Ni–N–S/CNS catalyst achieves a Faradaic efficiency for CO2–to–CO (FECO) of 99.3% at –0.7 VRHE and maintains over 90% across pH–universal conditions with ultrawide potential windows: 1400 mV (from –0.3 VRHE to –1.7 VRHE) in alkaline media, 1200 mV (from –0.7 VRHE to –1.9 VRHE) in neutral conditions, and 1000 mV (from –1.3 VRHE to –2.3 VRHE) in acidic environments. Remarkably, this catalyst enables the tandem CO2RR and N–alkylaniline carbonylation process for synthesizing o–aminobenzoates and isatoic anhydrides with high yield. Our findings demonstrate an electrothermo–catalytic tandem strategy for cost–effective CO2 conversion and synthesis of high valuable fine chemicals, thereby broadening the scope of its utilization.
Tandem CO2 electroreduction integrated with carbonylation reactions offers a promising pathway for transforming greenhouse gases into valuable chemical products. The development of efficient CO2–to–CO electrocatalysts operational across wide potential ranges is crucial to address renewable energy fluctuations and facilitate integrated cascade systems. Herein, a Ni single–atom catalyst (SAC) with sulfur doping in the second shell of Ni–N4 is reported. In situ measurements and theoretical calculations demonstrate that the incorporation S atoms not only modulates the electronic configuration of Ni active sites but also enhances H2O adsorption, enabling rapid CO2 hydrogenation into *COOH intermediates even at high potentials. Consequently, the Ni–N–S/CNS catalyst achieves a Faradaic efficiency for CO2–to–CO (FECO) of 99.3% at –0.7 VRHE and maintains over 90% across pH–universal conditions with ultrawide potential windows: 1400 mV (from –0.3 VRHE to –1.7 VRHE) in alkaline media, 1200 mV (from –0.7 VRHE to –1.9 VRHE) in neutral conditions, and 1000 mV (from –1.3 VRHE to –2.3 VRHE) in acidic environments. Remarkably, this catalyst enables the tandem CO2RR and N–alkylaniline carbonylation process for synthesizing o–aminobenzoates and isatoic anhydrides with high yield. Our findings demonstrate an electrothermo–catalytic tandem strategy for cost–effective CO2 conversion and synthesis of high valuable fine chemicals, thereby broadening the scope of its utilization.
2026, 37(7): 112153
doi: 10.1016/j.cclet.2025.112153
Abstract:
Catalytic oxidation of H2S at room temperature has been regarded as a promising method for removing malodorous H2S pollution. However, most of the existing research has primarily focused on developing catalysts with high sulfur capacity, i.e., high elemental sulfur selectivity, which was unfavored for the catalyst regeneration. The present work prioritizes efficient water wash regeneration as a key objective. A series of activated carbon fibers (ACFs) was synthesized using a synergistic strategy of "nitrogen doping-plasma defect engineering". The certain amount of nitrogen species ensured a certain level of sulfur capacity. The plasma defect engineering can result in the enhancement of surface acidity and defect density, which worked together to make the catalyst with high sulfate selectivity. The O2-plasma modified NH3-ACF-O10 catalyst achieved the best catalytic performance with appropriate sulfur capacity (0.21 g/g) and highest sulfate selectivity (85.40%). Importantly, it can be easily regenerated by water wash, and almost 83.33% sulfur capacity can be recovered. Besides, superoxide radicals (O2•-) were identified as the primary reactive oxygen species for the reaction. And the reaction obeyed a Langmuir-Hinshelwood (L-H) like mechanism, i.e., the reaction was proceeded via chemisorbed H2S and O2•-, which was adsorbed and activated by defect.
Catalytic oxidation of H2S at room temperature has been regarded as a promising method for removing malodorous H2S pollution. However, most of the existing research has primarily focused on developing catalysts with high sulfur capacity, i.e., high elemental sulfur selectivity, which was unfavored for the catalyst regeneration. The present work prioritizes efficient water wash regeneration as a key objective. A series of activated carbon fibers (ACFs) was synthesized using a synergistic strategy of "nitrogen doping-plasma defect engineering". The certain amount of nitrogen species ensured a certain level of sulfur capacity. The plasma defect engineering can result in the enhancement of surface acidity and defect density, which worked together to make the catalyst with high sulfate selectivity. The O2-plasma modified NH3-ACF-O10 catalyst achieved the best catalytic performance with appropriate sulfur capacity (0.21 g/g) and highest sulfate selectivity (85.40%). Importantly, it can be easily regenerated by water wash, and almost 83.33% sulfur capacity can be recovered. Besides, superoxide radicals (O2•-) were identified as the primary reactive oxygen species for the reaction. And the reaction obeyed a Langmuir-Hinshelwood (L-H) like mechanism, i.e., the reaction was proceeded via chemisorbed H2S and O2•-, which was adsorbed and activated by defect.
2026, 37(7): 112158
doi: 10.1016/j.cclet.2025.112158
Abstract:
Rare–earth–based perovskite materials, due to their low cost and tunable structure, have been regarded as a promising platform for photoinduced molecular oxygen activation. However, a comprehensive understanding and precise regulation of the surface reconstruction of the active phase in perovskite oxides during molecular oxygen activation remain highly challenging tasks. Herein, a refined A–site management strategy is proposed for perovskite oxides, which provides power for molecular oxygen activation by adjusting the electronic structure of B–site elements. Comprehensive experimental results reveal that the enhanced photocatalytic mechanism is attributed to the substitution of holmium (Ho) at the atomic level, which facilitates an increase in the valence state of iron and shifts the center of the d–band to a more positive energy level, thereby promoting O2 adsorption. Additionally, theoretical calculations demonstrate that the Ho 4f orbital overlaps with the Fe 3d and O 2p orbitals near the Fermi level, significantly enhancing charge transfer between oxygen and metal, thereby facilitating the conversion of oxygen into highly reactive oxygen species. Therefore, the optimized La0.97Ho0.03FeO3 (LHFO) exhibits greatly enhanced catalytic performance for molecular oxygen activation, and the degradation rate constant of tetracycline is 9.5 times higher than LaFeO3, representing one of the most efficient and robust RE–based perovskites.
Rare–earth–based perovskite materials, due to their low cost and tunable structure, have been regarded as a promising platform for photoinduced molecular oxygen activation. However, a comprehensive understanding and precise regulation of the surface reconstruction of the active phase in perovskite oxides during molecular oxygen activation remain highly challenging tasks. Herein, a refined A–site management strategy is proposed for perovskite oxides, which provides power for molecular oxygen activation by adjusting the electronic structure of B–site elements. Comprehensive experimental results reveal that the enhanced photocatalytic mechanism is attributed to the substitution of holmium (Ho) at the atomic level, which facilitates an increase in the valence state of iron and shifts the center of the d–band to a more positive energy level, thereby promoting O2 adsorption. Additionally, theoretical calculations demonstrate that the Ho 4f orbital overlaps with the Fe 3d and O 2p orbitals near the Fermi level, significantly enhancing charge transfer between oxygen and metal, thereby facilitating the conversion of oxygen into highly reactive oxygen species. Therefore, the optimized La0.97Ho0.03FeO3 (LHFO) exhibits greatly enhanced catalytic performance for molecular oxygen activation, and the degradation rate constant of tetracycline is 9.5 times higher than LaFeO3, representing one of the most efficient and robust RE–based perovskites.
2026, 37(7): 112159
doi: 10.1016/j.cclet.2025.112159
Abstract:
Achieving point-of-care detection of neutrophil gelatinase-associated lipocalin (NGAL) contributes to the early diagnosis and treatment of acute kidney injury (AKI), but the lack of highly sensitive and long-term stable detection methods is a major challenge. In this work, tetrahedral DNA (tDNA)-functionalized large-sized upconversion nanoparticles (t-UCNP300) were synthesized with high luminescence intensity. Leveraging the dual effects of surface charge density and the rigid structure of tDNA, the developed t-UCNP300 exhibited long-term stability for over 60 days after being stored in phosphate buffer at 25 ℃ and pH 7.4, with no obvious aggregation and only slight luminescence attenuation. By using this developed t-UCNP300, a luminescent lateral flow immunoassay (LFIA) strip was developed for point-of-care detection of NGAL, with a detection linearity range of 2.00–250 ng/mL and limit of detection (LOD) of 1.00 ± 0.07 ng/mL (S/N = 3). Taking advantage of the developed LFIA strip for NGAL with high selectivity and a rapid response time of < 5 min, it was successfully applied for the determination of NGAL in artificial urine samples.
Achieving point-of-care detection of neutrophil gelatinase-associated lipocalin (NGAL) contributes to the early diagnosis and treatment of acute kidney injury (AKI), but the lack of highly sensitive and long-term stable detection methods is a major challenge. In this work, tetrahedral DNA (tDNA)-functionalized large-sized upconversion nanoparticles (t-UCNP300) were synthesized with high luminescence intensity. Leveraging the dual effects of surface charge density and the rigid structure of tDNA, the developed t-UCNP300 exhibited long-term stability for over 60 days after being stored in phosphate buffer at 25 ℃ and pH 7.4, with no obvious aggregation and only slight luminescence attenuation. By using this developed t-UCNP300, a luminescent lateral flow immunoassay (LFIA) strip was developed for point-of-care detection of NGAL, with a detection linearity range of 2.00–250 ng/mL and limit of detection (LOD) of 1.00 ± 0.07 ng/mL (S/N = 3). Taking advantage of the developed LFIA strip for NGAL with high selectivity and a rapid response time of < 5 min, it was successfully applied for the determination of NGAL in artificial urine samples.
2026, 37(7): 112161
doi: 10.1016/j.cclet.2025.112161
Abstract:
Understanding the nucleation, growth and structural phase transitions process during the preparation of nanomaterials is crucial for the targeted design and controllable preparation of nanomaterials with specific structures and properties. Herein, a “solid phase transition” behavior is first found in the semiconductor C3N4 material during the conversion process from amorphous bulk C3N4 to high crystallinity C3N4 nanosheets, which usually exists in the process of metals or alloys conversion. A unique C3N4 nanosheet structure with uniform size distribution is successfully synthesized with a simple two-step calcination method, which is totally different from the traditional irregular nanosheets exfoliated from the bulk C3N4. This C3N4 nanosheets also possess high crystallinity and it helps to promote the migration of charge carriers during the catalytic process. By precisely exploring the synthesis process, a new “solid phase transition” mechanism is introduced to help understand the atoms recrystallize and grow to form the uniform high crystallinity nanosheets. The high yield (86%) of this strategy also overcomes the problem of low efficiency in preparing C3N4 nanosheets. Besides, the advantages of this uniform high crystallinity C3N4 nanosheets result in superior long-term stability in 100 CV cycles during the electrochemiluminescence (ECL) test, which is particularly superior to conventional C3N4 nanosheets.
Understanding the nucleation, growth and structural phase transitions process during the preparation of nanomaterials is crucial for the targeted design and controllable preparation of nanomaterials with specific structures and properties. Herein, a “solid phase transition” behavior is first found in the semiconductor C3N4 material during the conversion process from amorphous bulk C3N4 to high crystallinity C3N4 nanosheets, which usually exists in the process of metals or alloys conversion. A unique C3N4 nanosheet structure with uniform size distribution is successfully synthesized with a simple two-step calcination method, which is totally different from the traditional irregular nanosheets exfoliated from the bulk C3N4. This C3N4 nanosheets also possess high crystallinity and it helps to promote the migration of charge carriers during the catalytic process. By precisely exploring the synthesis process, a new “solid phase transition” mechanism is introduced to help understand the atoms recrystallize and grow to form the uniform high crystallinity nanosheets. The high yield (86%) of this strategy also overcomes the problem of low efficiency in preparing C3N4 nanosheets. Besides, the advantages of this uniform high crystallinity C3N4 nanosheets result in superior long-term stability in 100 CV cycles during the electrochemiluminescence (ECL) test, which is particularly superior to conventional C3N4 nanosheets.
2026, 37(7): 112169
doi: 10.1016/j.cclet.2025.112169
Abstract:
Electroactive quinone-based compounds have shown great potential as lithium-ion batteries cathodes due to their high capacity, environmental friendliness, and low cost. However, their practical application is severely hindered by high solubility in aprotic electrolytes and low electronic conductivity. Herein, we skillfully utilized the two-dimensional MXene Ti2C2 as a host material to anchor benzoquinone skeleton by a simple coordination chemical reaction, obtaining the composite cathode materials (T@M). Significantly, the MXene not only stabilizes the benzoquinone framework but also shortens ion/electron diffusion pathways. As a result, the T@M cathode delivers a high discharge specific capacity of 300.1 mAh/g at 0.05 A/g and retains 70% of its capacity after 3000 cycles at 1 A/g. This work provides an effective strategy for developing high-performance organic electrodes for rechargeable batteries.
Electroactive quinone-based compounds have shown great potential as lithium-ion batteries cathodes due to their high capacity, environmental friendliness, and low cost. However, their practical application is severely hindered by high solubility in aprotic electrolytes and low electronic conductivity. Herein, we skillfully utilized the two-dimensional MXene Ti2C2 as a host material to anchor benzoquinone skeleton by a simple coordination chemical reaction, obtaining the composite cathode materials (T@M). Significantly, the MXene not only stabilizes the benzoquinone framework but also shortens ion/electron diffusion pathways. As a result, the T@M cathode delivers a high discharge specific capacity of 300.1 mAh/g at 0.05 A/g and retains 70% of its capacity after 3000 cycles at 1 A/g. This work provides an effective strategy for developing high-performance organic electrodes for rechargeable batteries.
2026, 37(7): 112175
doi: 10.1016/j.cclet.2025.112175
Abstract:
Marine atmospheric aerosols are pivotal components of the global aerosol system, which can significantly influence global climate and human health. Perfluoroalkyl carboxylic acids (PFCAs), persistent emerging contaminants, exhibit pronounced enrichment in sea spray aerosols (SSAs). However, current gas-particle partitioning models underestimate their particulate-phase ratios in polluted atmospheres. Here, we elucidate the interfacial chemistry driving the enrichment of PFCAs in SSAs under anthropogenic impacts. Through Born-Oppenheimer molecular dynamics simulations, we demonstrated that TFA, a representative of PFCAs, exhibited activity at gas-liquid interfaces. The carbonyl oxygen of TFA protrudes beyond hydration layers, which facilitates collisions with gaseous SO3. Interfacial water molecules can promote simultaneous TFA deprotonation and SO3 collision and then the formation of trifluoroacetic acid sulfuric anhydride ions (TFASA-) and hydronium ions (H3O+). TFASA- displays superior hygroscopicity over precursors, enhancing the growth potential of SSAs to form cloud condensation nuclei (CCN). Given the continuous accumulation of PFCAs in marine environment, the interfacial chemical reactions between PFCAs and reactive pollutants (e.g., SO3) in marine atmospheres need urgent focus to understand the influence of PFCAs on marine particulate matter pollution and global climate.
Marine atmospheric aerosols are pivotal components of the global aerosol system, which can significantly influence global climate and human health. Perfluoroalkyl carboxylic acids (PFCAs), persistent emerging contaminants, exhibit pronounced enrichment in sea spray aerosols (SSAs). However, current gas-particle partitioning models underestimate their particulate-phase ratios in polluted atmospheres. Here, we elucidate the interfacial chemistry driving the enrichment of PFCAs in SSAs under anthropogenic impacts. Through Born-Oppenheimer molecular dynamics simulations, we demonstrated that TFA, a representative of PFCAs, exhibited activity at gas-liquid interfaces. The carbonyl oxygen of TFA protrudes beyond hydration layers, which facilitates collisions with gaseous SO3. Interfacial water molecules can promote simultaneous TFA deprotonation and SO3 collision and then the formation of trifluoroacetic acid sulfuric anhydride ions (TFASA-) and hydronium ions (H3O+). TFASA- displays superior hygroscopicity over precursors, enhancing the growth potential of SSAs to form cloud condensation nuclei (CCN). Given the continuous accumulation of PFCAs in marine environment, the interfacial chemical reactions between PFCAs and reactive pollutants (e.g., SO3) in marine atmospheres need urgent focus to understand the influence of PFCAs on marine particulate matter pollution and global climate.
2026, 37(7): 112193
doi: 10.1016/j.cclet.2025.112193
Abstract:
The heterogeneous electro-Fenton (HEF) technology is a promising yet challenging approach for organic pollutant degradation. It is urgent to develop a catalyst for both highly efficient H2O2 and hydroxyl radical (•OH) generation with low energy consumption at neutral conditions. This study presents a bifunctional catalyst (CoPc/OCNTs/FeOF) synthesized by ultrasonic anchoring of FeOF onto cobalt phthalocyanine-modified oxidized carbon nanotubes. The catalyst demonstrated synergistic effects, achieving a 2.94-fold enhancement in H2O2 generation and a 3.85-fold increase in •OH yield compared to its individual components (CoPc/OCNTs and FeOF). At pH 6, the CoPc/OCNTs/FeOF cathode enabled nearly complete phenol removal within 90 min, with a high kinetic rate constant (k) of 0.04848 min-1, driven by cooperative oxidation from singlet oxygen (1O2) and •OH. The system exhibited exceptional stability, inorganic ion tolerance, and broad applicability to real wastewaters, achieving 82.0% total organic carbon (TOC) removal for phenol wastewater at a low energy consumption of 21.9 kWh kg-1 COD-1. Moreover, sodium alginate-immobilized microalgae hydrogel was integrated into the HEF system to supply O2 in situ for the 2e- oxygen reduction reaction (ORR), eliminating energy-intensive mechanical aeration. Subsequent microalgal cultivation further removed 90.6% of total nitrogen and 82.8% of total phosphorus, showcasing a sustainable dual-function strategy for pollutant degradation and nutrient recovery. This work advances the design of efficient HEF catalysts and highlights the potential of microalgae-coupled systems for sustainable wastewater treatment.
The heterogeneous electro-Fenton (HEF) technology is a promising yet challenging approach for organic pollutant degradation. It is urgent to develop a catalyst for both highly efficient H2O2 and hydroxyl radical (•OH) generation with low energy consumption at neutral conditions. This study presents a bifunctional catalyst (CoPc/OCNTs/FeOF) synthesized by ultrasonic anchoring of FeOF onto cobalt phthalocyanine-modified oxidized carbon nanotubes. The catalyst demonstrated synergistic effects, achieving a 2.94-fold enhancement in H2O2 generation and a 3.85-fold increase in •OH yield compared to its individual components (CoPc/OCNTs and FeOF). At pH 6, the CoPc/OCNTs/FeOF cathode enabled nearly complete phenol removal within 90 min, with a high kinetic rate constant (k) of 0.04848 min-1, driven by cooperative oxidation from singlet oxygen (1O2) and •OH. The system exhibited exceptional stability, inorganic ion tolerance, and broad applicability to real wastewaters, achieving 82.0% total organic carbon (TOC) removal for phenol wastewater at a low energy consumption of 21.9 kWh kg-1 COD-1. Moreover, sodium alginate-immobilized microalgae hydrogel was integrated into the HEF system to supply O2 in situ for the 2e- oxygen reduction reaction (ORR), eliminating energy-intensive mechanical aeration. Subsequent microalgal cultivation further removed 90.6% of total nitrogen and 82.8% of total phosphorus, showcasing a sustainable dual-function strategy for pollutant degradation and nutrient recovery. This work advances the design of efficient HEF catalysts and highlights the potential of microalgae-coupled systems for sustainable wastewater treatment.
2026, 37(7): 112196
doi: 10.1016/j.cclet.2025.112196
Abstract:
To reduce the pollution of waste heat to the environment and achieve Sustainable Development Goals, recovering and utilizing of low-grade heat is critical. Although various thermal conversion technologies have been extensively developed, research on thermal energy storage materials with dynamically adjustable properties for diverse applications is still lacking. Herein, hydrated salt hydrogel with switchable stiffness and tunable thermal performance was fabricated by simply incorporating sodium acetate trihydrate into hydrogel network. Hydrated salt hydrogel displayed adjustable thermal performance (maximum heat release temperature from 53 ℃ to 20 ℃; enthalpy value from 0 to 179 J/g) by regulated sodium acetate trihydrate concentration of hydrogels. Moreover, the control of variable mechanical strength (0.03–5.21 MPa) and toughness (0.02–420.58 MPa) was accomplished. The study further demonstrates the promising application of hydrated salt hydrogel in thermal management for electronics and controllable soft-rigid coupling thermoelectric devices, opening new opportunities in waste heat recovery and achieving Sustainable Development Goals.
To reduce the pollution of waste heat to the environment and achieve Sustainable Development Goals, recovering and utilizing of low-grade heat is critical. Although various thermal conversion technologies have been extensively developed, research on thermal energy storage materials with dynamically adjustable properties for diverse applications is still lacking. Herein, hydrated salt hydrogel with switchable stiffness and tunable thermal performance was fabricated by simply incorporating sodium acetate trihydrate into hydrogel network. Hydrated salt hydrogel displayed adjustable thermal performance (maximum heat release temperature from 53 ℃ to 20 ℃; enthalpy value from 0 to 179 J/g) by regulated sodium acetate trihydrate concentration of hydrogels. Moreover, the control of variable mechanical strength (0.03–5.21 MPa) and toughness (0.02–420.58 MPa) was accomplished. The study further demonstrates the promising application of hydrated salt hydrogel in thermal management for electronics and controllable soft-rigid coupling thermoelectric devices, opening new opportunities in waste heat recovery and achieving Sustainable Development Goals.
2026, 37(7): 112207
doi: 10.1016/j.cclet.2025.112207
Abstract:
Alkaline anion exchange membrane water electrolysis (AEMWE) is a low-cost and sustainable technology for hydrogen production. This study presents the development of high-performance anion exchange membrane (AEM) and ionomers based on quaternized poly(diphenyl carbazole) with rigid ether-bond-free aryl backbone and flexible multination strings in the side chains. The optimized molecular architecture induces pronounced microphase separation, enabling high hydroxide conductivity (159.3 mS/cm at 80 ℃) and exceptional alkaline stability (1 mol/L KOH at 80 ℃, retains 97.5% ionic conductivity and 88.6% tensile strength after 1800 h). By implementing an anode water-fed/cathode water-free configuration and regulating the structure and content of ionomers at anode and cathode electrodes, the AEMWE performance was significantly improved from 1.9 A/cm2 to 4.2 A/cm2 at 2 V (a 2.2-fold increase) using 1 mol/L KOH solution as the electrolyte. Under pure water conditions, the electrolyzer still achieved an excellent electrolysis performance of 1.8 A/cm2 at 2 V. Furthermore, the fabricated AEMWE exhibited an outstanding in-situ durability with a low voltage degradation rate of 0.17 mV/h during a continuous operation of 1185 h at a current density of 0.5 A/cm2.
Alkaline anion exchange membrane water electrolysis (AEMWE) is a low-cost and sustainable technology for hydrogen production. This study presents the development of high-performance anion exchange membrane (AEM) and ionomers based on quaternized poly(diphenyl carbazole) with rigid ether-bond-free aryl backbone and flexible multination strings in the side chains. The optimized molecular architecture induces pronounced microphase separation, enabling high hydroxide conductivity (159.3 mS/cm at 80 ℃) and exceptional alkaline stability (1 mol/L KOH at 80 ℃, retains 97.5% ionic conductivity and 88.6% tensile strength after 1800 h). By implementing an anode water-fed/cathode water-free configuration and regulating the structure and content of ionomers at anode and cathode electrodes, the AEMWE performance was significantly improved from 1.9 A/cm2 to 4.2 A/cm2 at 2 V (a 2.2-fold increase) using 1 mol/L KOH solution as the electrolyte. Under pure water conditions, the electrolyzer still achieved an excellent electrolysis performance of 1.8 A/cm2 at 2 V. Furthermore, the fabricated AEMWE exhibited an outstanding in-situ durability with a low voltage degradation rate of 0.17 mV/h during a continuous operation of 1185 h at a current density of 0.5 A/cm2.
2026, 37(7): 112209
doi: 10.1016/j.cclet.2025.112209
Abstract:
The treatment of nitrogen-contained refractory organic wastewater faces challenges due to complex composition and high toxicity. While microscale zero-valent iron (mZVI) based processes enable simultaneous removal of organic contaminants and nitrate (NO3−-N), electron competition and excessive iron sludge generation limit efficiency. This study reveals the dual roles of NO3−-N in the mZVI/O2 process: Inhibiting the oxidative removal of organic contaminants through electron competition and simultaneously enhancing iron dissolution with TFe increased by 17.5% to 65.7% compared to the system without NO3−-N. Nitrogen conversion analysis indicates that NO3−-N is mainly converted to NH4+-N via a direct 8-electron reduction pathway. To increase the utilization efficiency of iron electrons and enhance organic contaminant removal, a two-stage gradient oxidation process (mZVI/O2-Fenton) is designed: 1st stage utilizes NO3−-N to enhance Fe0 corrosion for NO3−-N reduction and Fe(II) release, while 2nd stage achieves efficient organic contaminants degradation via Fenton reaction with addition of H2O2. Actual wastewater validation confirms synergistic high organic contaminants removal (COD removal > 79.5%) and targeted nitrogen conversion (> 66.4% NO3−-N to NH4+-N). The study overcomes electron competition limitations in the mZVI/O2 process and provides a synergistic pollution control-resource recovery strategy for NO3−-N-contained refractory organic wastewaters.
The treatment of nitrogen-contained refractory organic wastewater faces challenges due to complex composition and high toxicity. While microscale zero-valent iron (mZVI) based processes enable simultaneous removal of organic contaminants and nitrate (NO3−-N), electron competition and excessive iron sludge generation limit efficiency. This study reveals the dual roles of NO3−-N in the mZVI/O2 process: Inhibiting the oxidative removal of organic contaminants through electron competition and simultaneously enhancing iron dissolution with TFe increased by 17.5% to 65.7% compared to the system without NO3−-N. Nitrogen conversion analysis indicates that NO3−-N is mainly converted to NH4+-N via a direct 8-electron reduction pathway. To increase the utilization efficiency of iron electrons and enhance organic contaminant removal, a two-stage gradient oxidation process (mZVI/O2-Fenton) is designed: 1st stage utilizes NO3−-N to enhance Fe0 corrosion for NO3−-N reduction and Fe(II) release, while 2nd stage achieves efficient organic contaminants degradation via Fenton reaction with addition of H2O2. Actual wastewater validation confirms synergistic high organic contaminants removal (COD removal > 79.5%) and targeted nitrogen conversion (> 66.4% NO3−-N to NH4+-N). The study overcomes electron competition limitations in the mZVI/O2 process and provides a synergistic pollution control-resource recovery strategy for NO3−-N-contained refractory organic wastewaters.
2026, 37(7): 112210
doi: 10.1016/j.cclet.2025.112210
Abstract:
In situ chemical oxidation (ISCO) technology using peroxymonosulfate (PMS) and natural iron-bearing minerals for groundwater remediation has received increasing interest. The interaction between PMS and active Fe sites in minerals significantly influences the effectiveness of groundwater remediation. Nevertheless, there has been limited research investigating the relationship between the minerals active Fe sites and PMS activation. Herein, we distinguished and quantified the active Fe sites of common natural iron-bearing minerals in groundwater aquifers. Lewis acid sites (Fe-OH) were confirmed as the reaction sites in iron oxide/hydroxide/bearing clay minerals. The activation performance of minerals is positively correlated with their Lewis acid content. In iron sulfide minerals, Fe-S sites act as electron transfer mediators, facilitating PMS adsorption and activation. The activation of PMS by Lewis acid and Fe-S sites free radical both led to the generation of free radicals (SO4·- and ·OH) for CPs removal. Moreover, typical ferrihydrite/PMS and pyrite/PMS systems exhibited resistance to environmental interference and broad pH adaptability. A one-dimensional sand column experiment further proved their feasibility and long-term applicability in saturated porous media. These findings highlight the critical influence of active Fe sites of natural iron-bearing minerals and provide technical support for the application of PMS-ISCO strategies for groundwater remediation.
In situ chemical oxidation (ISCO) technology using peroxymonosulfate (PMS) and natural iron-bearing minerals for groundwater remediation has received increasing interest. The interaction between PMS and active Fe sites in minerals significantly influences the effectiveness of groundwater remediation. Nevertheless, there has been limited research investigating the relationship between the minerals active Fe sites and PMS activation. Herein, we distinguished and quantified the active Fe sites of common natural iron-bearing minerals in groundwater aquifers. Lewis acid sites (Fe-OH) were confirmed as the reaction sites in iron oxide/hydroxide/bearing clay minerals. The activation performance of minerals is positively correlated with their Lewis acid content. In iron sulfide minerals, Fe-S sites act as electron transfer mediators, facilitating PMS adsorption and activation. The activation of PMS by Lewis acid and Fe-S sites free radical both led to the generation of free radicals (SO4·- and ·OH) for CPs removal. Moreover, typical ferrihydrite/PMS and pyrite/PMS systems exhibited resistance to environmental interference and broad pH adaptability. A one-dimensional sand column experiment further proved their feasibility and long-term applicability in saturated porous media. These findings highlight the critical influence of active Fe sites of natural iron-bearing minerals and provide technical support for the application of PMS-ISCO strategies for groundwater remediation.
2026, 37(7): 112228
doi: 10.1016/j.cclet.2025.112228
Abstract:
This study presents a OH− concentration-regulated one-step hydrothermal synthesis of a novel SrBi4Ti4O15/BiOCl heterojunction for efficient antibiotic degradation. Precise control of alkaline conditions enabled the in-situ generation of Ti–Cl bonds at the heterointerface, with their presence and nature further corroborated by Raman and XPS analyses. The SBTO/BOC heterojunction demonstrated significantly enhanced charge separation, achieving a 91.5% tetracycline degradation rate under illumination, outperforming pure BiOCl (71.9%) and SBTO (54.8%). Radical trapping and EPR studies identified •O2− and •OH as the primary reactive species. The catalyst exhibited robust stability, broad pH tolerance, and resistance to ionic interference. Tetracycline degradation efficiency further improves under combined light and ultrasonic irradiation, leveraging piezoelectric polarization to boost charge separation. LC-MS analysis revealed reduced toxicity of degradation intermediates. This work highlights the strategic role of OH−-mediated interface engineering in designing efficient ferroelectric heterojunctions for wastewater remediation.
This study presents a OH− concentration-regulated one-step hydrothermal synthesis of a novel SrBi4Ti4O15/BiOCl heterojunction for efficient antibiotic degradation. Precise control of alkaline conditions enabled the in-situ generation of Ti–Cl bonds at the heterointerface, with their presence and nature further corroborated by Raman and XPS analyses. The SBTO/BOC heterojunction demonstrated significantly enhanced charge separation, achieving a 91.5% tetracycline degradation rate under illumination, outperforming pure BiOCl (71.9%) and SBTO (54.8%). Radical trapping and EPR studies identified •O2− and •OH as the primary reactive species. The catalyst exhibited robust stability, broad pH tolerance, and resistance to ionic interference. Tetracycline degradation efficiency further improves under combined light and ultrasonic irradiation, leveraging piezoelectric polarization to boost charge separation. LC-MS analysis revealed reduced toxicity of degradation intermediates. This work highlights the strategic role of OH−-mediated interface engineering in designing efficient ferroelectric heterojunctions for wastewater remediation.
2026, 37(7): 112230
doi: 10.1016/j.cclet.2025.112230
Abstract:
Iron oxide based magnetic catalytic colorimetric (MCC) nanomaterials have attracted extensive attention as signal labels in lateral flow immunoassays (LFIA). However, the main challenge in this field is its weak catalytic activity leading to relatively low color intensity. Herein, a new strategy of using the metal-organic framework (MOF) as mediate interfacing layer for loading Pt nanoparticles (Pt NPs) on the magnetic nanoparticles (MNPs) was proposed to obtain MCC nanomaterials with high catalytic activity. First, Cu-Co MOF was grown in situ with MNPs as the core, and then the MOF interfacing layer facilitates the uniform growth of Pt NPs on it. The obtained MNPs@MOF@Pt nanocomposite exhibited enhanced color signal intensity, excellent peroxidase-like activity and strong magnetic separation ability. After integration with a dual-antibody sandwich LFIA platform, the highly sensitive detection of interleukin-6 was achieved with a detection limit of 8.3 and 2.8 pg/mL for the pre-catalytic and post-catalytic tests respectively, which were 58-fold and 171-fold higher than that of the LFIA based on gold nanoparticles. Moreover, it exhibited good specificity and high accuracy for detection of clinical serum samples. Therefore, the magnetic nanozyme material proposed in this study demonstrated great potential for application in point-of-care diseases diagnosis.
Iron oxide based magnetic catalytic colorimetric (MCC) nanomaterials have attracted extensive attention as signal labels in lateral flow immunoassays (LFIA). However, the main challenge in this field is its weak catalytic activity leading to relatively low color intensity. Herein, a new strategy of using the metal-organic framework (MOF) as mediate interfacing layer for loading Pt nanoparticles (Pt NPs) on the magnetic nanoparticles (MNPs) was proposed to obtain MCC nanomaterials with high catalytic activity. First, Cu-Co MOF was grown in situ with MNPs as the core, and then the MOF interfacing layer facilitates the uniform growth of Pt NPs on it. The obtained MNPs@MOF@Pt nanocomposite exhibited enhanced color signal intensity, excellent peroxidase-like activity and strong magnetic separation ability. After integration with a dual-antibody sandwich LFIA platform, the highly sensitive detection of interleukin-6 was achieved with a detection limit of 8.3 and 2.8 pg/mL for the pre-catalytic and post-catalytic tests respectively, which were 58-fold and 171-fold higher than that of the LFIA based on gold nanoparticles. Moreover, it exhibited good specificity and high accuracy for detection of clinical serum samples. Therefore, the magnetic nanozyme material proposed in this study demonstrated great potential for application in point-of-care diseases diagnosis.
2026, 37(7): 112231
doi: 10.1016/j.cclet.2025.112231
Abstract:
Current environmental and ecological risks associated with plastics are escalating. Cutting-edge research has focused on recycling waste plastics into monomers or energy resources. Fenton-like catalysis exhibits potential for technological development in this field. This study evaluates global warming potential (GWP), non-renewable energy use (NREU), and minimum selling price (MSP) during fuel recovery from waste plastics using Fenton-like processes. Adjusting operational strategies could enhance environmental sustainability and economic viability. Process parameters were optimized through controlled manipulation of catalyst pyrolysis temperature, catalyst concentration, hydrothermal temperature, and peroxymonosulfate (PMS) dosage. The optimization balanced environmental impact and economic returns in plastic recycling. Catalyst expenditure and PMS consumption emerged as primary barriers to sustainable and cost-efficient operations in homogeneous catalysis systems. When the superior-performance heterogeneous catalyst was used, Fenton-like process achieved 78% reduction in GWP, 99% decrease in NREU, and 63% MSP reduction for polypropylene (PP) recycling compared to homogeneous systems. With heterogeneous catalysis, polylactic acid (PLA) conversion demonstrates 29 times greater in terms of energy recovery efficiency for compared to PP processing. Sensitivity analysis revealed a variability of 8%-20% in outcomes due to oxidant loss. And the cost advantage for European operations compared to China was identified. The results underscored the importance of regional energy structures and process control for large-scale application. The system assessment framework has established quantifiable technical operation standards with the goal of environmental-economic benefits for implementing Fenton-like systems in plastic waste management. The results contribute directly to advancing circular economy principles and carbon reduction technologies.
Current environmental and ecological risks associated with plastics are escalating. Cutting-edge research has focused on recycling waste plastics into monomers or energy resources. Fenton-like catalysis exhibits potential for technological development in this field. This study evaluates global warming potential (GWP), non-renewable energy use (NREU), and minimum selling price (MSP) during fuel recovery from waste plastics using Fenton-like processes. Adjusting operational strategies could enhance environmental sustainability and economic viability. Process parameters were optimized through controlled manipulation of catalyst pyrolysis temperature, catalyst concentration, hydrothermal temperature, and peroxymonosulfate (PMS) dosage. The optimization balanced environmental impact and economic returns in plastic recycling. Catalyst expenditure and PMS consumption emerged as primary barriers to sustainable and cost-efficient operations in homogeneous catalysis systems. When the superior-performance heterogeneous catalyst was used, Fenton-like process achieved 78% reduction in GWP, 99% decrease in NREU, and 63% MSP reduction for polypropylene (PP) recycling compared to homogeneous systems. With heterogeneous catalysis, polylactic acid (PLA) conversion demonstrates 29 times greater in terms of energy recovery efficiency for compared to PP processing. Sensitivity analysis revealed a variability of 8%-20% in outcomes due to oxidant loss. And the cost advantage for European operations compared to China was identified. The results underscored the importance of regional energy structures and process control for large-scale application. The system assessment framework has established quantifiable technical operation standards with the goal of environmental-economic benefits for implementing Fenton-like systems in plastic waste management. The results contribute directly to advancing circular economy principles and carbon reduction technologies.
2026, 37(7): 112273
doi: 10.1016/j.cclet.2025.112273
Abstract:
The degradation of perfluorocarboxylic acids (PFCAs), persistent organic pollutants, remains a significant environmental challenge. Photolysis represents a key pathway for their degradation, yet the molecular mechanisms driving defluorination and decarboxylation remain unclear. This study investigates the first step of direct PFCA photolysis by analyzing excitation properties using density functional theory (DFT), aiming to elucidate the relationship between electronic structure changes and degradation pathways. To better demonstrate and analyze the impact of internal factors on the first step of PFCAs photolysis, quantum chemical calculations were conducted to quantify and compare the molecule’s properties in the ground state and the excited state, aiming to explore the changes in the molecule’s behavior. Key parameters, including α C–F bond elongation (0.31%–1.62%), α C–C bond contraction (−6.23% to −9.10%), and excitation energy reduction (5.76–5.47 eV), revealed chain-length-dependent trends. The lower bond dissociation energy of α C–C (90–93 kcal/mol) compared to α C–F (116–124 kcal/mol) rationalized the dominance of decarboxylation over defluorination. Charge transfer spectroscopy further indicated localized n → π* excitation at carboxyl groups, promoting decarboxylation. A quantitative structure-activity relationship (QSAR) model linking hole-electron indices to degradation rates (R2 = 0.91) was developed and validated via leave-one-out cross-validation (RMSE = 0.338). These findings not only advance the mechanistic understanding of PFCA photolysis but also provide a predictive tool for optimizing UV-based water treatment systems targeting persistent fluorinated pollutants.
The degradation of perfluorocarboxylic acids (PFCAs), persistent organic pollutants, remains a significant environmental challenge. Photolysis represents a key pathway for their degradation, yet the molecular mechanisms driving defluorination and decarboxylation remain unclear. This study investigates the first step of direct PFCA photolysis by analyzing excitation properties using density functional theory (DFT), aiming to elucidate the relationship between electronic structure changes and degradation pathways. To better demonstrate and analyze the impact of internal factors on the first step of PFCAs photolysis, quantum chemical calculations were conducted to quantify and compare the molecule’s properties in the ground state and the excited state, aiming to explore the changes in the molecule’s behavior. Key parameters, including α C–F bond elongation (0.31%–1.62%), α C–C bond contraction (−6.23% to −9.10%), and excitation energy reduction (5.76–5.47 eV), revealed chain-length-dependent trends. The lower bond dissociation energy of α C–C (90–93 kcal/mol) compared to α C–F (116–124 kcal/mol) rationalized the dominance of decarboxylation over defluorination. Charge transfer spectroscopy further indicated localized n → π* excitation at carboxyl groups, promoting decarboxylation. A quantitative structure-activity relationship (QSAR) model linking hole-electron indices to degradation rates (R2 = 0.91) was developed and validated via leave-one-out cross-validation (RMSE = 0.338). These findings not only advance the mechanistic understanding of PFCA photolysis but also provide a predictive tool for optimizing UV-based water treatment systems targeting persistent fluorinated pollutants.
2026, 37(7): 112275
doi: 10.1016/j.cclet.2025.112275
Abstract:
Photocatalytic water oxidation is considered as the bottleneck step for overall artificial photosynthesis, due to the slow photocarrier transfer kinetics and climbing thermodynamics. Developing the electronic structure of catalytic with more dynamic-thermodynamic advantages is crucial to deal with the above dilemma and realize the photocatalytic water oxidation. This work successfully explores an S-induced modification strategy to induce electronic delocalization and non-equilibrium states for unique Bi active sites. The introduction of V4+ species leads to asymmetric coordination of Bi atoms in the S-Bi-V4+ structure to provide more nonlocalized electrons, which initiates a concerted electron transfer in the system. The fine regulation on the local electron density and energy level structure of the Bi active site optimizes the reaction energy barriers to construct thermodynamically more favourable active centers for water oxidation. The optimized 2% S-BVO catalyst achieves outstanding water oxidation rate of 70.25 μmol/h (40 mg catalyst) triggering up to 11.06% apparent quantum efficiency at 420 nm. This work elucidates the influence of synergistic electron interaction of asymmetric coordination structure on both photocarrier transfer kinetics and reaction thermodynamic.
Photocatalytic water oxidation is considered as the bottleneck step for overall artificial photosynthesis, due to the slow photocarrier transfer kinetics and climbing thermodynamics. Developing the electronic structure of catalytic with more dynamic-thermodynamic advantages is crucial to deal with the above dilemma and realize the photocatalytic water oxidation. This work successfully explores an S-induced modification strategy to induce electronic delocalization and non-equilibrium states for unique Bi active sites. The introduction of V4+ species leads to asymmetric coordination of Bi atoms in the S-Bi-V4+ structure to provide more nonlocalized electrons, which initiates a concerted electron transfer in the system. The fine regulation on the local electron density and energy level structure of the Bi active site optimizes the reaction energy barriers to construct thermodynamically more favourable active centers for water oxidation. The optimized 2% S-BVO catalyst achieves outstanding water oxidation rate of 70.25 μmol/h (40 mg catalyst) triggering up to 11.06% apparent quantum efficiency at 420 nm. This work elucidates the influence of synergistic electron interaction of asymmetric coordination structure on both photocarrier transfer kinetics and reaction thermodynamic.
2026, 37(7): 112297
doi: 10.1016/j.cclet.2025.112297
Abstract:
Adsorption is the most effective technique for perfluoroalkyl substances removal, owing to its simplicity and cost-effectiveness. However, conventional adsorbents suffer from low capacity, slow kinetics, poor selectivity, and reusability challenge. This study introduced a novel amine and imine functionalized covalent organic frameworks (PDA@COFs) adsorbent. Benefiting from its functional groups and unobstructed channels, PDA@COFs exhibited an ultra-high maximum adsorption capacity (3200 mg/g) and excellent selectivity for perfluorooctanoic (PFOA), which is far more than most adsorbents. Theoretical calculations revealed that electrostatic attraction is the dominant mechanism driving the selective adsorption of PFOA by PDA@COFs. The five-stages analysis of adsorption isotherms revealed that PDA@COFs adsorbed PFOA monomers via electrostatic adsorption at low concentrations and adsorbed PFOA aggregates by electrostatic and hydrophobic synergistic adsorption at high concentrations, which significantly enhanced the adsorption capacity for PFOA. To explore the practical application potential of PDA@COFs, it was evaluated as a promising anode in capacitive deionization (CDI). The recovery of PFOA was as high as 98.2%, highlighting its potential for practical application. This study is the first to demonstrate that PDA@COFs has an ultra-high adsorption capacity toward PFOA and new insights into the PFOA adsorption mechanism with five stages, and explores its practical application potential through CDI.
Adsorption is the most effective technique for perfluoroalkyl substances removal, owing to its simplicity and cost-effectiveness. However, conventional adsorbents suffer from low capacity, slow kinetics, poor selectivity, and reusability challenge. This study introduced a novel amine and imine functionalized covalent organic frameworks (PDA@COFs) adsorbent. Benefiting from its functional groups and unobstructed channels, PDA@COFs exhibited an ultra-high maximum adsorption capacity (3200 mg/g) and excellent selectivity for perfluorooctanoic (PFOA), which is far more than most adsorbents. Theoretical calculations revealed that electrostatic attraction is the dominant mechanism driving the selective adsorption of PFOA by PDA@COFs. The five-stages analysis of adsorption isotherms revealed that PDA@COFs adsorbed PFOA monomers via electrostatic adsorption at low concentrations and adsorbed PFOA aggregates by electrostatic and hydrophobic synergistic adsorption at high concentrations, which significantly enhanced the adsorption capacity for PFOA. To explore the practical application potential of PDA@COFs, it was evaluated as a promising anode in capacitive deionization (CDI). The recovery of PFOA was as high as 98.2%, highlighting its potential for practical application. This study is the first to demonstrate that PDA@COFs has an ultra-high adsorption capacity toward PFOA and new insights into the PFOA adsorption mechanism with five stages, and explores its practical application potential through CDI.
2026, 37(7): 112375
doi: 10.1016/j.cclet.2026.112375
Abstract:
Supported catalysts are an effective approach in proton exchange membrane water electrolysis (PEMWE) owing to their enhanced metal-support interfacial interaction. We propose a novel high-temperature shock (HTS) technique by Joule-heating to construct an electronic coupling interface between IrO2 nanoclusters catalysts and TiO2 support (IrO2/TiO2-HTS). The HTS strategy features an ultrafast heating rate and compresses the synthesis time from hours to seconds (2 h to 60 s). The as-prepared catalyst features uniformly embedding the ultrafine IrO2 nanoclusters enrich oxygen vacancies within the redox-active metal oxide matrix, yielding exceptional mass activity and ultrastable performance. The mass activity of the catalyst is 1081 A/gIr at 1.6 V vs. RHE, 13 times higher than of commercial IrO2, and it demonstrates operation time for over 1100 h at 10 mA/cm2 with a voltage decay rate of only 40 μV/h. This HTS strategy offers a scalable route to accelerate vacancy engineering and strong metal oxide-support interaction (SMOSI) formation, enabling high activity at reduced Ir loading and long-term stability under acidic conditions. The approach is general and can be extended to other supported binary oxides, opening opportunities for the development of additional high–performance OER catalysts and PEM–relevant electrolysis systems.
Supported catalysts are an effective approach in proton exchange membrane water electrolysis (PEMWE) owing to their enhanced metal-support interfacial interaction. We propose a novel high-temperature shock (HTS) technique by Joule-heating to construct an electronic coupling interface between IrO2 nanoclusters catalysts and TiO2 support (IrO2/TiO2-HTS). The HTS strategy features an ultrafast heating rate and compresses the synthesis time from hours to seconds (2 h to 60 s). The as-prepared catalyst features uniformly embedding the ultrafine IrO2 nanoclusters enrich oxygen vacancies within the redox-active metal oxide matrix, yielding exceptional mass activity and ultrastable performance. The mass activity of the catalyst is 1081 A/gIr at 1.6 V vs. RHE, 13 times higher than of commercial IrO2, and it demonstrates operation time for over 1100 h at 10 mA/cm2 with a voltage decay rate of only 40 μV/h. This HTS strategy offers a scalable route to accelerate vacancy engineering and strong metal oxide-support interaction (SMOSI) formation, enabling high activity at reduced Ir loading and long-term stability under acidic conditions. The approach is general and can be extended to other supported binary oxides, opening opportunities for the development of additional high–performance OER catalysts and PEM–relevant electrolysis systems.
2026, 37(7): 112611
doi: 10.1016/j.cclet.2026.112611
Abstract:
The outer membrane (OM) of Gram-negative bacteria, with its unique and complex structure, serves as a critical structural foundation for their heightened pathogenicity and drug resistance. However, with a thickness of only 7–9 nm, the OM is highly fragile and undergoes continuous remodeling, making it difficult to elucidate its structural dynamics and functional mechanisms during bacterial growth, division, and host invasion. Here, we developed Rho-PMXB as an OM-specific fluorescent probe that incorporates a polymyxin-derived moiety for highly specific recognition of OM lipopolysaccharides (LPS) and a rhodamine fluorophore that confers excellent photostability and high fluorescence brightness. Rho-PMXB enables selective labeling of the OMs of various Gram-negative bacteria and supports super-resolution imaging, allowing real-time visualization of OM dynamics during bacterial growth, division, and antibiotic treatment, thereby providing insight into antimicrobial mechanisms. Furthermore, Rho-PMXB enables dynamic super-resolution imaging of pathogen-host cell interactions, visualizing OM behavior during Porphyromonas gingivalis invasion of human gingival epithelial (HGE) cells and revealing its interplay with the host plasma membrane and actin cytoskeleton.
The outer membrane (OM) of Gram-negative bacteria, with its unique and complex structure, serves as a critical structural foundation for their heightened pathogenicity and drug resistance. However, with a thickness of only 7–9 nm, the OM is highly fragile and undergoes continuous remodeling, making it difficult to elucidate its structural dynamics and functional mechanisms during bacterial growth, division, and host invasion. Here, we developed Rho-PMXB as an OM-specific fluorescent probe that incorporates a polymyxin-derived moiety for highly specific recognition of OM lipopolysaccharides (LPS) and a rhodamine fluorophore that confers excellent photostability and high fluorescence brightness. Rho-PMXB enables selective labeling of the OMs of various Gram-negative bacteria and supports super-resolution imaging, allowing real-time visualization of OM dynamics during bacterial growth, division, and antibiotic treatment, thereby providing insight into antimicrobial mechanisms. Furthermore, Rho-PMXB enables dynamic super-resolution imaging of pathogen-host cell interactions, visualizing OM behavior during Porphyromonas gingivalis invasion of human gingival epithelial (HGE) cells and revealing its interplay with the host plasma membrane and actin cytoskeleton.
In situ real-time imaging of photothermal-induced rupture of self-assembled naphthalimide nanofibers
2026, 37(7): 112627
doi: 10.1016/j.cclet.2026.112627
Abstract:
Photoresponsive supramolecular polymers hold great promise for applications in sensing, actuation, and biomedicine. However, the role of photothermal effects in regulating supramolecular assemblies and their dynamic structural evolution at the microscopic level remains poorly understood, as most studies have primarily focused on molecular photochemical mechanisms. Herein, we report a photothermal-responsive supramolecular system based on 1,8-naphthalimide building blocks. By reducing hydrogen-bonding sites through modification of the amide N-substituent of BAze from 4-(hydroxymethyl)benzyl to benzyl, an OH-free derivative, PhAze, was obtained. This subtle structural change endows PhAze assemblies with photoresponsive behavior that markedly differs from that of BAze assemblies. Upon 488 nm laser irradiation, PhAze assemblies undergo nanofiber rupture accompanied by ~40% fluorescence enhancement, whereas BAze assemblies show only a slight fluorescence decrease without morphological change. Real-time in situ observation based on confocal laser scanning microscopy (CLSM) reveals the dynamic photoresponse of PhAze nanofibers. Localized fluorescence enhancement first appears along the fibers, followed by the formation of molten-like microspheres that ultimately lead to fiber rupture. Two distinct modes of microsphere formation, synchronous and asynchronous, are identified during this process. Moreover, thermal imaging further confirms that the response originates from a photothermal effect, where localized temperature rise weakens noncovalent interactions and induces partial melting of the supramolecular fibers. This study provides direct in situ insights into photothermal-driven structural evolution in supramolecular assemblies and offers a new strategy for designing photothermal-responsive supramolecular materials.
Photoresponsive supramolecular polymers hold great promise for applications in sensing, actuation, and biomedicine. However, the role of photothermal effects in regulating supramolecular assemblies and their dynamic structural evolution at the microscopic level remains poorly understood, as most studies have primarily focused on molecular photochemical mechanisms. Herein, we report a photothermal-responsive supramolecular system based on 1,8-naphthalimide building blocks. By reducing hydrogen-bonding sites through modification of the amide N-substituent of BAze from 4-(hydroxymethyl)benzyl to benzyl, an OH-free derivative, PhAze, was obtained. This subtle structural change endows PhAze assemblies with photoresponsive behavior that markedly differs from that of BAze assemblies. Upon 488 nm laser irradiation, PhAze assemblies undergo nanofiber rupture accompanied by ~40% fluorescence enhancement, whereas BAze assemblies show only a slight fluorescence decrease without morphological change. Real-time in situ observation based on confocal laser scanning microscopy (CLSM) reveals the dynamic photoresponse of PhAze nanofibers. Localized fluorescence enhancement first appears along the fibers, followed by the formation of molten-like microspheres that ultimately lead to fiber rupture. Two distinct modes of microsphere formation, synchronous and asynchronous, are identified during this process. Moreover, thermal imaging further confirms that the response originates from a photothermal effect, where localized temperature rise weakens noncovalent interactions and induces partial melting of the supramolecular fibers. This study provides direct in situ insights into photothermal-driven structural evolution in supramolecular assemblies and offers a new strategy for designing photothermal-responsive supramolecular materials.
2026, 37(7): 112645
doi: 10.1016/j.cclet.2026.112645
Abstract:
Photocatalytic conversion of polylactic acid (PLA) into high-value-added pyruvic acid (PA) presents a promising strategy for carbon-efficient resource cycling. However, successive dehydrogenation at the α-C of lactic acid (the monomer of PLA) remains a critical challenge. In this study, we fabricated an Au-modified CdS nanosphere photocatalyst (Au-CdS), where the introduction of Au facilitates the activation of the Cα-H bond in lactic acid (LA). Through combined theoretical calculations and in-situ EPR analysis, Au-CdS reduces the Cα-H bond cleavage energy barrier from 1.02 eV to 0.49 eV, substantially elevating the generation of carbon-centered radical intermediates. In addition, Au-CdS demonstrates enhanced separation efficiency of photogenerated electron-hole pairs relative to pristine CdS, thus efficiently activating O2 to generate O2•− radicals and further driving the conversion of O2•− to •OH radicals. The produced •OH radicals facilitate the successive dehydrogenation reactions via interacting with the Cα-H and α-OH bonds on the α-C of LA, thereby promoting the selective conversion of LA to PA. As a result, the Au-CdS catalyst achieves a PA production rate of 1340 ± 25 μmol g-1 h-1, surpassing that of pristine CdS by 8.9-fold. This work presents a novel strategy for the value-added upcycling of plastic waste.
Photocatalytic conversion of polylactic acid (PLA) into high-value-added pyruvic acid (PA) presents a promising strategy for carbon-efficient resource cycling. However, successive dehydrogenation at the α-C of lactic acid (the monomer of PLA) remains a critical challenge. In this study, we fabricated an Au-modified CdS nanosphere photocatalyst (Au-CdS), where the introduction of Au facilitates the activation of the Cα-H bond in lactic acid (LA). Through combined theoretical calculations and in-situ EPR analysis, Au-CdS reduces the Cα-H bond cleavage energy barrier from 1.02 eV to 0.49 eV, substantially elevating the generation of carbon-centered radical intermediates. In addition, Au-CdS demonstrates enhanced separation efficiency of photogenerated electron-hole pairs relative to pristine CdS, thus efficiently activating O2 to generate O2•− radicals and further driving the conversion of O2•− to •OH radicals. The produced •OH radicals facilitate the successive dehydrogenation reactions via interacting with the Cα-H and α-OH bonds on the α-C of LA, thereby promoting the selective conversion of LA to PA. As a result, the Au-CdS catalyst achieves a PA production rate of 1340 ± 25 μmol g-1 h-1, surpassing that of pristine CdS by 8.9-fold. This work presents a novel strategy for the value-added upcycling of plastic waste.
2026, 37(7): 112676
doi: 10.1016/j.cclet.2026.112676
Abstract:
To address the challenges of active metal leaching and sluggish redox cycling in heterogeneous metal-catalyzed peroxymonosulfate (PMS) activation, this study proposes a double heteroatom co-anchoring and regulation strategy to design a sulfur-nitrogen co-doped carbon-supported cobalt nanoparticle catalyst (Co-S-CN). This strategy successfully constructs a “S2--Co0” dual micro-reduction environment, significantly accelerating the Co3+/Co2+ redox cycle. Experimental results demonstrate that the Co-S-CN+PMS system achieves 100% phenol degradation within 5 min while exhibiting exceptional resistance to anion interference (SO42−, Cl−, HCO3−, H2PO4−). Low cobalt leaching rate (<1%) across various pH conditions confirms strong metal anchoring via S-N synergy. Structural characterizations verify the existence of S2- and Co0, and co-optimizing cobalt valence cycling. Electron paramagnetic resonance (EPR) and quenching experiments indicate the reaction proceeds primarily via a nonradical pathway, with singlet oxygen (1O2) as the key reactive species. Density functional theory (DFT) calculations reveal that S-N synergy enhances PMS adsorption strength (adsorption energy optimized from −3.51 eV to −3.77 eV), increases charge density (Bader charge increased from 0.75 e to 0.80 e), and optimizes the electronic structure of Co 3d orbitals (d-band center upshifted from −1.341 eV to −1.330 eV). This work provides a strategy for rational design of highly active and stable catalysts.
To address the challenges of active metal leaching and sluggish redox cycling in heterogeneous metal-catalyzed peroxymonosulfate (PMS) activation, this study proposes a double heteroatom co-anchoring and regulation strategy to design a sulfur-nitrogen co-doped carbon-supported cobalt nanoparticle catalyst (Co-S-CN). This strategy successfully constructs a “S2--Co0” dual micro-reduction environment, significantly accelerating the Co3+/Co2+ redox cycle. Experimental results demonstrate that the Co-S-CN+PMS system achieves 100% phenol degradation within 5 min while exhibiting exceptional resistance to anion interference (SO42−, Cl−, HCO3−, H2PO4−). Low cobalt leaching rate (<1%) across various pH conditions confirms strong metal anchoring via S-N synergy. Structural characterizations verify the existence of S2- and Co0, and co-optimizing cobalt valence cycling. Electron paramagnetic resonance (EPR) and quenching experiments indicate the reaction proceeds primarily via a nonradical pathway, with singlet oxygen (1O2) as the key reactive species. Density functional theory (DFT) calculations reveal that S-N synergy enhances PMS adsorption strength (adsorption energy optimized from −3.51 eV to −3.77 eV), increases charge density (Bader charge increased from 0.75 e to 0.80 e), and optimizes the electronic structure of Co 3d orbitals (d-band center upshifted from −1.341 eV to −1.330 eV). This work provides a strategy for rational design of highly active and stable catalysts.
2026, 37(7): 111564
doi: 10.1016/j.cclet.2025.111564
Abstract:
The severe threat of heavy metal pollution to ecological sustainability and human health has made the urgent development of efficient and environmentally friendly remediation technologies a necessity. Polyoxometalates (POMs), a class of unique metal-oxygen clusters with regulable structures and excellent properties, have emerged as promising candidates for removal of heavy metal ions. This review summarized the recent advances in POM-based functional materials (e.g., host-guest, heterojunction, and POM-based metal-organic frameworks) for heavy metal ion remediation (such as U(VI), Pb(II), and Cr(VI)). The removal mechanisms, including adsorption, chemical reduction, photocatalytic reduction, adsorption-photocatalysis synergy, as well as the chemical sensor or probe for heavy metal detection, have been highlighted. Additionally, the challenges in improving material recyclability, scaling up synthesis, and understanding the long-term environmental impact of POMs are identified, while future research directions toward sustainable, cost-effective, and multifunctional POM-based systems are proposed. This review provides a comprehensive overview of POM-based functional materials potential in addressing heavy metal pollution, offering insights for designing next-generation environmental remediation materials.
The severe threat of heavy metal pollution to ecological sustainability and human health has made the urgent development of efficient and environmentally friendly remediation technologies a necessity. Polyoxometalates (POMs), a class of unique metal-oxygen clusters with regulable structures and excellent properties, have emerged as promising candidates for removal of heavy metal ions. This review summarized the recent advances in POM-based functional materials (e.g., host-guest, heterojunction, and POM-based metal-organic frameworks) for heavy metal ion remediation (such as U(VI), Pb(II), and Cr(VI)). The removal mechanisms, including adsorption, chemical reduction, photocatalytic reduction, adsorption-photocatalysis synergy, as well as the chemical sensor or probe for heavy metal detection, have been highlighted. Additionally, the challenges in improving material recyclability, scaling up synthesis, and understanding the long-term environmental impact of POMs are identified, while future research directions toward sustainable, cost-effective, and multifunctional POM-based systems are proposed. This review provides a comprehensive overview of POM-based functional materials potential in addressing heavy metal pollution, offering insights for designing next-generation environmental remediation materials.
2026, 37(7): 111597
doi: 10.1016/j.cclet.2025.111597
Abstract:
Compared to synthetic chemical compounds, plant extracts derived from natural sources have emerged as the "new favorites" in the treatment and care of skin diseases due to their distinct advantages, including being environmentally friendly, sustainable, and safe. However, challenges such as poor solubility, limited permeability, and the barrier function of the stratum corneum significantly restrict the application of natural products in dermal drug delivery. Fortunately, advancements in nanotechnology offer promising solutions to overcome these challenges. Different skin diseases and treatments require the precise delivery of natural active ingredients to specific skin layers, and the unique structure of nanocarriers enables targeted delivery to achieve desired therapeutic outcomes. This paper begins by exploring the pathogenesis and therapeutic targets of common skin conditions, including atopic dermatitis (AD), psoriasis, decubitus ulcers, diabetic foot ulcers (DFUs), as well as applications in antioxidant therapies and anti-aging strategies. Furthermore, it provides a detailed overview of the depths and locations within the skin where active compounds must be delivered to exert their effects effectively. Subsequently, this review categorizes and examines natural products based on their therapeutic effects on various skin diseases. It then highlights the skin depths and specific sites that can be targeted by different delivery systems designed to enhance skin permeability, tailored to meet the needs of skin disease treatment or care. By addressing these aspects, this review aims to provide a valuable reference for advancing research on nano-delivery systems in the field of topical skin drug delivery for the treatment and management of skin diseases.
Compared to synthetic chemical compounds, plant extracts derived from natural sources have emerged as the "new favorites" in the treatment and care of skin diseases due to their distinct advantages, including being environmentally friendly, sustainable, and safe. However, challenges such as poor solubility, limited permeability, and the barrier function of the stratum corneum significantly restrict the application of natural products in dermal drug delivery. Fortunately, advancements in nanotechnology offer promising solutions to overcome these challenges. Different skin diseases and treatments require the precise delivery of natural active ingredients to specific skin layers, and the unique structure of nanocarriers enables targeted delivery to achieve desired therapeutic outcomes. This paper begins by exploring the pathogenesis and therapeutic targets of common skin conditions, including atopic dermatitis (AD), psoriasis, decubitus ulcers, diabetic foot ulcers (DFUs), as well as applications in antioxidant therapies and anti-aging strategies. Furthermore, it provides a detailed overview of the depths and locations within the skin where active compounds must be delivered to exert their effects effectively. Subsequently, this review categorizes and examines natural products based on their therapeutic effects on various skin diseases. It then highlights the skin depths and specific sites that can be targeted by different delivery systems designed to enhance skin permeability, tailored to meet the needs of skin disease treatment or care. By addressing these aspects, this review aims to provide a valuable reference for advancing research on nano-delivery systems in the field of topical skin drug delivery for the treatment and management of skin diseases.
2026, 37(7): 111610
doi: 10.1016/j.cclet.2025.111610
Abstract:
Macrophage membrane-camouflaged nanoparticles (MmNPs) are emerging as efficient nanoplatforms for targeted delivery to inflammatory sites, tumors, and infected tissues due to the innate characteristics of macrophages. This biomimetic strategy effectively addresses several limitations of traditional targeted drug delivery systems, offering improved biocompatibility, extended blood circulation, immune evasion, and site-specific homing. Compared to conventional functionalization methods, MmNPs provide a simplified method for creating multifunctional nanoparticles. In this review, we explore the origins and functions of macrophages, highlighting how MmNP platforms are leveraged for precise drug delivery. The latest applications of MmNPs in targeted delivery are summarized, focusing on their intrinsic targeting properties, membrane surface modifications and designs for environmental stimulus response. Finally, we discuss the prospects and challenges in translating MmNP technology from experimental settings to clinical applications, aiming to inspire continued innovation in the design of MmNP for precise and effective drug delivery strategies against complex diseases.
Macrophage membrane-camouflaged nanoparticles (MmNPs) are emerging as efficient nanoplatforms for targeted delivery to inflammatory sites, tumors, and infected tissues due to the innate characteristics of macrophages. This biomimetic strategy effectively addresses several limitations of traditional targeted drug delivery systems, offering improved biocompatibility, extended blood circulation, immune evasion, and site-specific homing. Compared to conventional functionalization methods, MmNPs provide a simplified method for creating multifunctional nanoparticles. In this review, we explore the origins and functions of macrophages, highlighting how MmNP platforms are leveraged for precise drug delivery. The latest applications of MmNPs in targeted delivery are summarized, focusing on their intrinsic targeting properties, membrane surface modifications and designs for environmental stimulus response. Finally, we discuss the prospects and challenges in translating MmNP technology from experimental settings to clinical applications, aiming to inspire continued innovation in the design of MmNP for precise and effective drug delivery strategies against complex diseases.
2026, 37(7): 111671
doi: 10.1016/j.cclet.2025.111671
Abstract:
Cerium oxide nanozymes (CeO2 NZs) exhibit enzyme mimetic activities and great promise for biomedical applications by mediating the dynamic cycling between Ce3+ and Ce4+. However, traditional preparation methods are often expensive and detrimental to the environment. Meanwhile, the problems of easy agglomeration, poor targeting and weak biocompatibility need to be solved. The available literatures have mainly reviewed CeO2 NZs in terms of its material properties, mechanisms and potential clinical applications. The literatures on the limitations of CeO2 NZs and the corresponding improvement methods are fragmented. Consequently, the limitations of CeO2 NZs and the strategies involving green preparation technology and modification mainly summarized, while the biosafety of the modification strategies are compared. Meanwhile, representative studies of potential clinical applications of CeO2 NZs over the past three years are outlined, along with a summary of their clinical translational prospects and challenges. Finally, the challenges of CeO2 NZs promotion technology are discussed.
Cerium oxide nanozymes (CeO2 NZs) exhibit enzyme mimetic activities and great promise for biomedical applications by mediating the dynamic cycling between Ce3+ and Ce4+. However, traditional preparation methods are often expensive and detrimental to the environment. Meanwhile, the problems of easy agglomeration, poor targeting and weak biocompatibility need to be solved. The available literatures have mainly reviewed CeO2 NZs in terms of its material properties, mechanisms and potential clinical applications. The literatures on the limitations of CeO2 NZs and the corresponding improvement methods are fragmented. Consequently, the limitations of CeO2 NZs and the strategies involving green preparation technology and modification mainly summarized, while the biosafety of the modification strategies are compared. Meanwhile, representative studies of potential clinical applications of CeO2 NZs over the past three years are outlined, along with a summary of their clinical translational prospects and challenges. Finally, the challenges of CeO2 NZs promotion technology are discussed.
2026, 37(7): 111695
doi: 10.1016/j.cclet.2025.111695
Abstract:
With growing emphasis on drug efficacy, safety, and adverse reactions, many traditional Chinese medicines and their active ingredients, as well as compounds such as antibiotics, immunosuppressants, and hormones often face limited efficacy or give rise to adverse effects during application. To improve therapeutic outcomes and reduce systemic side effects, oral targeted drug delivery systems have become an important research direction. Hydrogels have shown great potential in the field of oral delivery to treat many diseases due to their superior drug protection ability and excellent biocompatibility. This review explores the physiological characteristics of the gastrointestinal tract and the significant advantages of oral hydrogels in drug delivery, and systematically introduces hydrogel carrier design strategies through physical crosslinking, chemical crosslinking, small molecule self-assembly, and metal ion coordination. Furthermore, it emphasizes recent advances in intelligent oral hydrogels and drug loading strategy. Lastly, the review summarizes the innovative applications of oral hydrogels in the treatment of diseases such as esophagitis, GI disorders, metabolic and endocrine diseases, osteoporosis, detoxification, and cardiovascular diseases, offering valuable insights and guidance for optimizing and advancing hydrogel-based drug delivery systems.
With growing emphasis on drug efficacy, safety, and adverse reactions, many traditional Chinese medicines and their active ingredients, as well as compounds such as antibiotics, immunosuppressants, and hormones often face limited efficacy or give rise to adverse effects during application. To improve therapeutic outcomes and reduce systemic side effects, oral targeted drug delivery systems have become an important research direction. Hydrogels have shown great potential in the field of oral delivery to treat many diseases due to their superior drug protection ability and excellent biocompatibility. This review explores the physiological characteristics of the gastrointestinal tract and the significant advantages of oral hydrogels in drug delivery, and systematically introduces hydrogel carrier design strategies through physical crosslinking, chemical crosslinking, small molecule self-assembly, and metal ion coordination. Furthermore, it emphasizes recent advances in intelligent oral hydrogels and drug loading strategy. Lastly, the review summarizes the innovative applications of oral hydrogels in the treatment of diseases such as esophagitis, GI disorders, metabolic and endocrine diseases, osteoporosis, detoxification, and cardiovascular diseases, offering valuable insights and guidance for optimizing and advancing hydrogel-based drug delivery systems.
2026, 37(7): 111831
doi: 10.1016/j.cclet.2025.111831
Abstract:
Aqueous zinc-ion batteries (ZIBs) have gained tremendous interests by virtue of their intrinsic safety, low cost and favorable theoretical capacities. As the promising candidates of cathode materials of ZIBs, ammonium vanadates (NVO) have captured widespread attentions owing to their tunable chemical properties and enhanced structural stabilities owing to the existence of NH4+ in the [VO]n layers. However, the pristine NVO fails to meet the expectations due to the strong interlayer electrostatic repulsion and comparatively sluggish transfer kinetics, which necessitates the exploration of appropriate modification strategies to fully dig its potential. Herein, this review systematically summarizes five core molecular engineering strategies, intercalation, defect, interfacial, doping, and structural engineering strategies, and their significances in modulating structural and electrochemical properties of NVO are elaborately discussed. Moreover, the perspectives on the future developments and potential energy-related applications of NVO are presented. This review is anticipated to deepen the researchers' understandings of the potentials of molecular engineering strategies on improving zinc-ion storage capabilities of cathode materials, and further promote the practicality of NVO in ZIBs.
Aqueous zinc-ion batteries (ZIBs) have gained tremendous interests by virtue of their intrinsic safety, low cost and favorable theoretical capacities. As the promising candidates of cathode materials of ZIBs, ammonium vanadates (NVO) have captured widespread attentions owing to their tunable chemical properties and enhanced structural stabilities owing to the existence of NH4+ in the [VO]n layers. However, the pristine NVO fails to meet the expectations due to the strong interlayer electrostatic repulsion and comparatively sluggish transfer kinetics, which necessitates the exploration of appropriate modification strategies to fully dig its potential. Herein, this review systematically summarizes five core molecular engineering strategies, intercalation, defect, interfacial, doping, and structural engineering strategies, and their significances in modulating structural and electrochemical properties of NVO are elaborately discussed. Moreover, the perspectives on the future developments and potential energy-related applications of NVO are presented. This review is anticipated to deepen the researchers' understandings of the potentials of molecular engineering strategies on improving zinc-ion storage capabilities of cathode materials, and further promote the practicality of NVO in ZIBs.
2026, 37(7): 112141
doi: 10.1016/j.cclet.2025.112141
Abstract:
Nitrate contamination has prompted global concern due to its far-reaching effects on human health and the ecosystem. As an emerging technology, electrochemical nitrate reduction reaction (eNO3RR) provides a promising approach for converting nitrate to valuable ammonia (NH3) or harmless nitrogen gas (N2). However, the conversion efficiency of eNO3RR is still constrained by the mismatch between catalysts and the reaction microenvironment at lower nitrate concentrations (< 0.1 mol/L). In this review, we have systematically discussed the feasibility of electrochemical methods in treating low-concentration nitrate by summarizing recent advances and their reaction mechanisms. Meanwhile, the selection between NH3 and N2 pathways was evaluated based on the nitrate concentration range and safety considerations associated with each scenario. Finally, the dominant factors for applying eNO3RR to real-world scenarios were also thoroughly discussed. We hope this review can provide comprehensive insights into the design of optimal catalysts and systems for treating low-concentration nitrates in practical scenarios, thereby promoting the environmental sustainability of electrocatalytic technologies.
Nitrate contamination has prompted global concern due to its far-reaching effects on human health and the ecosystem. As an emerging technology, electrochemical nitrate reduction reaction (eNO3RR) provides a promising approach for converting nitrate to valuable ammonia (NH3) or harmless nitrogen gas (N2). However, the conversion efficiency of eNO3RR is still constrained by the mismatch between catalysts and the reaction microenvironment at lower nitrate concentrations (< 0.1 mol/L). In this review, we have systematically discussed the feasibility of electrochemical methods in treating low-concentration nitrate by summarizing recent advances and their reaction mechanisms. Meanwhile, the selection between NH3 and N2 pathways was evaluated based on the nitrate concentration range and safety considerations associated with each scenario. Finally, the dominant factors for applying eNO3RR to real-world scenarios were also thoroughly discussed. We hope this review can provide comprehensive insights into the design of optimal catalysts and systems for treating low-concentration nitrates in practical scenarios, thereby promoting the environmental sustainability of electrocatalytic technologies.
2026, 37(7): 112160
doi: 10.1016/j.cclet.2025.112160
Abstract:
The wastewater produced in the antibiotic manufacturing process is a significant source of antibiotic pollution in the aquatic environment, posing a severe threat to ecological health and human well-being. Researchers have explored various methods, including source reduction technologies such as enzymatic engineering and green process control, to enhance antibiotic extraction efficiency. In addition, high-efficiency end-of-line processing technology has also been widely developed. This review first provides a detailed introduction to the characteristics of various antibiotics and their distribution levels in the environment. Then we systematically summarize and analyze the full-chain antibiotic end-of-pipe treatment processes, including conventional treatment processes and typical advanced treatment processes. Especially compares and analyzes the removal efficiency and carbon emissions of different conventional treatment processes, aiming to select efficient and low-carbon treatment processes. We intend to provide effective solutions to tackle the issue of antibiotic pollution while ensuring public health and ecological security.
The wastewater produced in the antibiotic manufacturing process is a significant source of antibiotic pollution in the aquatic environment, posing a severe threat to ecological health and human well-being. Researchers have explored various methods, including source reduction technologies such as enzymatic engineering and green process control, to enhance antibiotic extraction efficiency. In addition, high-efficiency end-of-line processing technology has also been widely developed. This review first provides a detailed introduction to the characteristics of various antibiotics and their distribution levels in the environment. Then we systematically summarize and analyze the full-chain antibiotic end-of-pipe treatment processes, including conventional treatment processes and typical advanced treatment processes. Especially compares and analyzes the removal efficiency and carbon emissions of different conventional treatment processes, aiming to select efficient and low-carbon treatment processes. We intend to provide effective solutions to tackle the issue of antibiotic pollution while ensuring public health and ecological security.
2026, 37(7): 112174
doi: 10.1016/j.cclet.2025.112174
Abstract:
As a new wastewater treatment technology, the microalgae-fungi consortia system (MFCS) has attracted much attention because of its high efficiency, environmental protection and energy saving features. Extracellular polymeric substances (EPS) play a key role in MFCS treatment of wastewater and microalgae harvesting. In this review, the definition and formation process of MFCS, thoroughly examines the composition, properties, and influencing factors of EPS, as well as systematically explains the mechanism of action of EPS in wastewater treatment and microalgae harvesting. EPS surface functional groups have negative charge, adsorption, flocculation, and hydrophilicity/hydrophobicity properties. Microalgae and fungi form MFCS through EPS electrostatic attraction and protein bridging. EPS achieves adsorption, aggregation, and degradation of pollutants through targeted binding, chelation, coordination mechanisms, hydrophobic interactions, and complexation degradation mechanisms via functional groups. EPS achieves microalgae harvesting through electrostatic neutralization, surface protein interaction, and polysaccharide adhesion. However, current research still faces the following challenges, the selection of algal strains in the formation process of MFCS is still unclear. The mechanism of EPS removal of new pollutants and internal signaling pathways are still unclear. FSH takes too long, while FPH requires higher costs during harvesting. In the future, MFCS should be explored in combination with actual engineering applications, and different combinations of algae species and strains should be explored. Using genetic engineering to explore the synergistic mechanism of microalgae and fungi EPS in pollutant treatment. Improve the process conditions for harvesting microalgae using fungi, optimizing the two methods of microalgae harvesting, and conduct experiments on the efficient harvesting of microalgae. This review systematically explored the mechanism of action of EPS in MFCS, which is important for wastewater treatment and microalgal biomass harvesting.
As a new wastewater treatment technology, the microalgae-fungi consortia system (MFCS) has attracted much attention because of its high efficiency, environmental protection and energy saving features. Extracellular polymeric substances (EPS) play a key role in MFCS treatment of wastewater and microalgae harvesting. In this review, the definition and formation process of MFCS, thoroughly examines the composition, properties, and influencing factors of EPS, as well as systematically explains the mechanism of action of EPS in wastewater treatment and microalgae harvesting. EPS surface functional groups have negative charge, adsorption, flocculation, and hydrophilicity/hydrophobicity properties. Microalgae and fungi form MFCS through EPS electrostatic attraction and protein bridging. EPS achieves adsorption, aggregation, and degradation of pollutants through targeted binding, chelation, coordination mechanisms, hydrophobic interactions, and complexation degradation mechanisms via functional groups. EPS achieves microalgae harvesting through electrostatic neutralization, surface protein interaction, and polysaccharide adhesion. However, current research still faces the following challenges, the selection of algal strains in the formation process of MFCS is still unclear. The mechanism of EPS removal of new pollutants and internal signaling pathways are still unclear. FSH takes too long, while FPH requires higher costs during harvesting. In the future, MFCS should be explored in combination with actual engineering applications, and different combinations of algae species and strains should be explored. Using genetic engineering to explore the synergistic mechanism of microalgae and fungi EPS in pollutant treatment. Improve the process conditions for harvesting microalgae using fungi, optimizing the two methods of microalgae harvesting, and conduct experiments on the efficient harvesting of microalgae. This review systematically explored the mechanism of action of EPS in MFCS, which is important for wastewater treatment and microalgal biomass harvesting.
2026, 37(7): 112191
doi: 10.1016/j.cclet.2025.112191
Abstract:
In heterogeneous Fenton-like systems, the oxidative polymerization pathway is of great significance in the field of sustainable water treatment. Unlike the traditional mineralization pathway, it can convert organic pollutants into polymers, thereby achieving the recovery of carbon resources. This paper focuses on the core content related to this pathway, expounding that the mechanism of oxidative polymerization is influenced by multiple factors (catalysts, oxidants, organic matters). Meanwhile, various methods exist for identifying the polymerization pathway, such as electrochemical experiments, Raman spectroscopy analysis, and mass spectrometry technology, which can infer the reaction process and product structure. Additionally, this paper reveals two pathways for pollutant removal through oxidative polymerization: The radical pathway and the non-radical pathway. In the future, advanced characterization techniques should be used to deeply explore the microscopic mechanism of oxidative polymerization, optimize catalyst design, expand practical application research, and explore comprehensive utilization pathways for its products, so as to promote the development of sustainable water treatment technologies.
In heterogeneous Fenton-like systems, the oxidative polymerization pathway is of great significance in the field of sustainable water treatment. Unlike the traditional mineralization pathway, it can convert organic pollutants into polymers, thereby achieving the recovery of carbon resources. This paper focuses on the core content related to this pathway, expounding that the mechanism of oxidative polymerization is influenced by multiple factors (catalysts, oxidants, organic matters). Meanwhile, various methods exist for identifying the polymerization pathway, such as electrochemical experiments, Raman spectroscopy analysis, and mass spectrometry technology, which can infer the reaction process and product structure. Additionally, this paper reveals two pathways for pollutant removal through oxidative polymerization: The radical pathway and the non-radical pathway. In the future, advanced characterization techniques should be used to deeply explore the microscopic mechanism of oxidative polymerization, optimize catalyst design, expand practical application research, and explore comprehensive utilization pathways for its products, so as to promote the development of sustainable water treatment technologies.
2026, 37(7): 112192
doi: 10.1016/j.cclet.2025.112192
Abstract:
Single-atom catalysts (SACs), especially defective-SACs, have been developed into low-cost, high-selectivity and high-performance advanced catalysts due to their unique synergistic effects, and have occupied a place in the energy and environmental fields. However, there is a lack of comprehensive and comprehensive summaries and discussions on the structure-property relationships. Therefore, an exhaustive review on the topic of the synergistic interaction of SACs with defective catalysts is imminent. Firstly, this review offers an overview of the most recent generation pathways of defective-SACs based on SACs and defect formation time differences, with a focus on the important influencing factors in the different synthesis processes. Immediately thereafter, the different roles of defects in the constructed defective-SACs are comprehensively analyzed to unravel the mystery of the high stability and performance of defective-SACs. Subsequently, this article systematically analyzes the synergistic interaction mechanism between defects and SACs from the perspective of reaction mechanisms and explains how this mechanism drives significant performance improvements in various catalytic reactions. The article concludes with limitations of current research and future directions to guide the design of more perfect catalysts for defective-SACs.
Single-atom catalysts (SACs), especially defective-SACs, have been developed into low-cost, high-selectivity and high-performance advanced catalysts due to their unique synergistic effects, and have occupied a place in the energy and environmental fields. However, there is a lack of comprehensive and comprehensive summaries and discussions on the structure-property relationships. Therefore, an exhaustive review on the topic of the synergistic interaction of SACs with defective catalysts is imminent. Firstly, this review offers an overview of the most recent generation pathways of defective-SACs based on SACs and defect formation time differences, with a focus on the important influencing factors in the different synthesis processes. Immediately thereafter, the different roles of defects in the constructed defective-SACs are comprehensively analyzed to unravel the mystery of the high stability and performance of defective-SACs. Subsequently, this article systematically analyzes the synergistic interaction mechanism between defects and SACs from the perspective of reaction mechanisms and explains how this mechanism drives significant performance improvements in various catalytic reactions. The article concludes with limitations of current research and future directions to guide the design of more perfect catalysts for defective-SACs.
2026, 37(7): 112194
doi: 10.1016/j.cclet.2025.112194
Abstract:
Micro/nanoplastics (MNPs) have emerged as a global environmental concern, which leads to an urgent need for sensitive and specific MNPs detection technologies. Fluorescence-based methods with high sensitivity and dynamic tracking capabilities have become a significant and promising tool in MNPs analysis. This review systematically summarizes recent developments in fluorescent probes including traditional organic dyes, nanomaterials, aggregation-induced emission (AIE) molecules, binding peptides, and aptamers, for MNPs detection. The fluorescence sensing technology coupled with micro-imaging developed for in situ detection and dynamic tracking is also discussed. The current challenges for MNPs detection including matrix interference and lack of quantification standards are discussed and perspectives including developing multifunctional probes and AI-assisted platforms are proposed. This review provides theoretical reference and innovative ideas for developing new fluorescence probes and methods for MNPs detection and monitoring.
Micro/nanoplastics (MNPs) have emerged as a global environmental concern, which leads to an urgent need for sensitive and specific MNPs detection technologies. Fluorescence-based methods with high sensitivity and dynamic tracking capabilities have become a significant and promising tool in MNPs analysis. This review systematically summarizes recent developments in fluorescent probes including traditional organic dyes, nanomaterials, aggregation-induced emission (AIE) molecules, binding peptides, and aptamers, for MNPs detection. The fluorescence sensing technology coupled with micro-imaging developed for in situ detection and dynamic tracking is also discussed. The current challenges for MNPs detection including matrix interference and lack of quantification standards are discussed and perspectives including developing multifunctional probes and AI-assisted platforms are proposed. This review provides theoretical reference and innovative ideas for developing new fluorescence probes and methods for MNPs detection and monitoring.
2026, 37(7): 112208
doi: 10.1016/j.cclet.2025.112208
Abstract:
Mass spectrometry is a highly sensitive and precise analytical technique widely utilized in biomedical research, drug development, and environmental monitoring. Nonetheless, before mass spectrometry analysis, complex matrix samples frequently harbor numerous salts, which may compromise the stability and accuracy of mass spectrometry signals. Hence, it is imperative to employ effective desalting techniques, which serve as critical pretreatment steps in sample preparation for mass spectrometry analysis. While numerous scholars have developed desalting techniques, a comprehensive overview of such techniques is lacking. This paper provides a summary of desalination methods for mass spectrometry analysis developed since the twenty-first century (including extraction techniques, chromatography, ion exchange, crystallography, ambient ionization mass spectrometry and desalting agents, etc.), along with their principles, advantages, and disadvantages. Furthermore, recent research advancements and technological enhancements are discussed to introduce novel ideas and methodologies for sample desalting as a pretreatment step before mass spectrometry analysis. Against the backdrop of the growing importance of precision medicine and environmental monitoring, the continuous improvement of desalination technology will promote its wide application in areas such as clinical diagnosis, food safety testing, and environmental pollution assessment.
Mass spectrometry is a highly sensitive and precise analytical technique widely utilized in biomedical research, drug development, and environmental monitoring. Nonetheless, before mass spectrometry analysis, complex matrix samples frequently harbor numerous salts, which may compromise the stability and accuracy of mass spectrometry signals. Hence, it is imperative to employ effective desalting techniques, which serve as critical pretreatment steps in sample preparation for mass spectrometry analysis. While numerous scholars have developed desalting techniques, a comprehensive overview of such techniques is lacking. This paper provides a summary of desalination methods for mass spectrometry analysis developed since the twenty-first century (including extraction techniques, chromatography, ion exchange, crystallography, ambient ionization mass spectrometry and desalting agents, etc.), along with their principles, advantages, and disadvantages. Furthermore, recent research advancements and technological enhancements are discussed to introduce novel ideas and methodologies for sample desalting as a pretreatment step before mass spectrometry analysis. Against the backdrop of the growing importance of precision medicine and environmental monitoring, the continuous improvement of desalination technology will promote its wide application in areas such as clinical diagnosis, food safety testing, and environmental pollution assessment.
2026, 37(7): 112237
doi: 10.1016/j.cclet.2025.112237
Abstract:
Macrocyclic compounds play a fundamental role in supramolecular chemistry, demonstrating significant prospect in functional materials owing to their precise cavities and tunable molecular recognition and assembly capabilities. However, the only cavity of the mono-macrocyclic hosts limited the development of traditional mono-macrocycle-based supramolecular materials in assembly dimensionality, recognition selectivity, and synergistic performance. Therefore, multi-macrocyclic hosts attracted increasing attention due to their unique advantages originated from multi-cavity cooperativity, which include more abundant guest suitability, multiple-dimension assembly, precise collaborative effect, and so on. Based on these merits, introducing multi-macrocyclic hosts into supramolecular materials can efficiently improve and enrich the properties of these kinds of materials. This review summarizes recent innovative design and constructing strategies for multi-macrocyclic hosts, including covalent chain bridged, covalent fused, coordinated, and mechanically interlocked pathway. And their applications in recognition, luminescence, catalysis, biomedical and chiral materials are highlighted, while the advantages of multi-macrocycles in enhancing binding affinity, selectivity, and stimulus-responsive behavior are elucidated. Furthermore, we discuss future directions, such as novel multifunctional hosts design, optimization of assembly strategies, and interdisciplinary applications, providing theoretical insights and practical guidance for the development of multi-macrocycles-based high performance supramolecular materials.
Macrocyclic compounds play a fundamental role in supramolecular chemistry, demonstrating significant prospect in functional materials owing to their precise cavities and tunable molecular recognition and assembly capabilities. However, the only cavity of the mono-macrocyclic hosts limited the development of traditional mono-macrocycle-based supramolecular materials in assembly dimensionality, recognition selectivity, and synergistic performance. Therefore, multi-macrocyclic hosts attracted increasing attention due to their unique advantages originated from multi-cavity cooperativity, which include more abundant guest suitability, multiple-dimension assembly, precise collaborative effect, and so on. Based on these merits, introducing multi-macrocyclic hosts into supramolecular materials can efficiently improve and enrich the properties of these kinds of materials. This review summarizes recent innovative design and constructing strategies for multi-macrocyclic hosts, including covalent chain bridged, covalent fused, coordinated, and mechanically interlocked pathway. And their applications in recognition, luminescence, catalysis, biomedical and chiral materials are highlighted, while the advantages of multi-macrocycles in enhancing binding affinity, selectivity, and stimulus-responsive behavior are elucidated. Furthermore, we discuss future directions, such as novel multifunctional hosts design, optimization of assembly strategies, and interdisciplinary applications, providing theoretical insights and practical guidance for the development of multi-macrocycles-based high performance supramolecular materials.
2026, 37(7): 112274
doi: 10.1016/j.cclet.2025.112274
Abstract:
Fe-bearing clay minerals have garnered significant attention in environmental catalysis due to their unique Fe(Ⅱ)/Fe(Ⅲ) redox cycling and high surface area, which enable the effective activation of oxidants such as molecular oxygen (O2), peroxymonosulfate, and other species, and the subsequent generation of reactive oxygen species (ROS). This review offers a comprehensive overview of the structural characteristics and iron coordination environments within these minerals that govern electron transfer processes from Fe(Ⅱ) to oxidant species. It further explores the mechanistic pathways that lead to the formation of superoxide, hydroxyl radicals (•OH), and singlet oxygen, detailing the chemical reactions involved. Additionally, the influence of various co-substrates and chelating agents, such as humic acids and ethylenediaminetetraacetic acid (EDTA), on the enhancement of redox processes and ROS generation is discussed, focusing on their roles in modulating reaction kinetics and improving catalytic efficiency. Furthermore, the review highlights the recent advancements in applying Fe-bearing clay minerals for the degradation of persistent organic pollutants, including dyes, pharmaceuticals, and pesticides, in both aqueous and soil environments. The potential for optimizing these mineral-based catalytic systems by tailoring their composition or creating hybrid materials is also explored to develop more efficient and scalable solutions for environmental remediation. This review outlines future research directions, emphasizing the integration of fundamental mechanistic insights with practical applications for pollutant degradation.
Fe-bearing clay minerals have garnered significant attention in environmental catalysis due to their unique Fe(Ⅱ)/Fe(Ⅲ) redox cycling and high surface area, which enable the effective activation of oxidants such as molecular oxygen (O2), peroxymonosulfate, and other species, and the subsequent generation of reactive oxygen species (ROS). This review offers a comprehensive overview of the structural characteristics and iron coordination environments within these minerals that govern electron transfer processes from Fe(Ⅱ) to oxidant species. It further explores the mechanistic pathways that lead to the formation of superoxide, hydroxyl radicals (•OH), and singlet oxygen, detailing the chemical reactions involved. Additionally, the influence of various co-substrates and chelating agents, such as humic acids and ethylenediaminetetraacetic acid (EDTA), on the enhancement of redox processes and ROS generation is discussed, focusing on their roles in modulating reaction kinetics and improving catalytic efficiency. Furthermore, the review highlights the recent advancements in applying Fe-bearing clay minerals for the degradation of persistent organic pollutants, including dyes, pharmaceuticals, and pesticides, in both aqueous and soil environments. The potential for optimizing these mineral-based catalytic systems by tailoring their composition or creating hybrid materials is also explored to develop more efficient and scalable solutions for environmental remediation. This review outlines future research directions, emphasizing the integration of fundamental mechanistic insights with practical applications for pollutant degradation.
2026, 37(7): 112279
doi: 10.1016/j.cclet.2025.112279
Abstract:
Chiral recognition is a central tenet of life sciences and biomolecular interactions. It is indispensable for the enantiomeric analysis of pharmaceuticals and agrochemicals, as well as for the development of chiral materials and devices, with significant implications for biomedical applications. Despite its importance, the creation of efficient and highly selective enantiomer recognition in synthetic systems presents a major challenge. Supramolecular macrocycles address this by providing well-defined cavities and synergistically positioned functional groups, which enhance chiral selectivity and sensitivity beyond the capabilities of traditional small molecules. While the design and synthesis of macrocyclic hosts have advanced considerably, their practical utility is often constrained by their recognition efficiency, binding affinity, and their ability to recognize a diverse range of analytes. This article reviews recent chemical strategies for enhancing chiral complexation and recognition, and discusses the future outlook and obstacles within this field.
Chiral recognition is a central tenet of life sciences and biomolecular interactions. It is indispensable for the enantiomeric analysis of pharmaceuticals and agrochemicals, as well as for the development of chiral materials and devices, with significant implications for biomedical applications. Despite its importance, the creation of efficient and highly selective enantiomer recognition in synthetic systems presents a major challenge. Supramolecular macrocycles address this by providing well-defined cavities and synergistically positioned functional groups, which enhance chiral selectivity and sensitivity beyond the capabilities of traditional small molecules. While the design and synthesis of macrocyclic hosts have advanced considerably, their practical utility is often constrained by their recognition efficiency, binding affinity, and their ability to recognize a diverse range of analytes. This article reviews recent chemical strategies for enhancing chiral complexation and recognition, and discusses the future outlook and obstacles within this field.
2026, 37(7): 112280
doi: 10.1016/j.cclet.2025.112280
Abstract:
Imidazole derivatives exhibit broad-spectrum agricultural biological activities and serve as important molecular scaffolds in the discovery of new pesticides, particularly novel herbicides and fungicides. In recent years, there have been rapid developments in the research of imidazole-derived agricultural chemicals, such as the discovery of imidazole herbicides and fungicides. Therefore, it is significant to provide a review and update on the latest advances in the discovery of imidazole derivatives for pesticide development. Based on this, we systematically reviewed the latest research progress of imidazole derivatives in pesticide discovery, summarized the antiviral, insecticidal, nematicidal, and antibacterial activities of imidazole compounds, analyzed the synthetic methods of representative imidazole compounds, and discussed the active moieties, pharmacophores, structure-activity relationships (SAR), and mechanisms of action. This review aims to provide novel insights and inspiration for the discovery of novel imidazole pesticides.
Imidazole derivatives exhibit broad-spectrum agricultural biological activities and serve as important molecular scaffolds in the discovery of new pesticides, particularly novel herbicides and fungicides. In recent years, there have been rapid developments in the research of imidazole-derived agricultural chemicals, such as the discovery of imidazole herbicides and fungicides. Therefore, it is significant to provide a review and update on the latest advances in the discovery of imidazole derivatives for pesticide development. Based on this, we systematically reviewed the latest research progress of imidazole derivatives in pesticide discovery, summarized the antiviral, insecticidal, nematicidal, and antibacterial activities of imidazole compounds, analyzed the synthetic methods of representative imidazole compounds, and discussed the active moieties, pharmacophores, structure-activity relationships (SAR), and mechanisms of action. This review aims to provide novel insights and inspiration for the discovery of novel imidazole pesticides.
2026, 37(7): 112308
doi: 10.1016/j.cclet.2025.112308
Abstract:
Broflanilide is the first listed meta-diamide insecticide, which has shown potential in the field of pesticide research and development due to its unique structure and mechanism of action. The key to the development of the meta-diamide insecticides is the derivatization of various sites in the meta-diamide compounds. It is of great research significance to develop highly effective, broad spectrum, safe, and environmentally compatible meta-diamide insecticide using Broflanilide as a lead compound to obtain structurally diverse meta-diamide compounds. An overview of meta-diamide derivatives from the perspectives of insecticidal activities and mechanism of action is offered. Their potentials as a dominant active structure for development of insecticides are also discussed.
Broflanilide is the first listed meta-diamide insecticide, which has shown potential in the field of pesticide research and development due to its unique structure and mechanism of action. The key to the development of the meta-diamide insecticides is the derivatization of various sites in the meta-diamide compounds. It is of great research significance to develop highly effective, broad spectrum, safe, and environmentally compatible meta-diamide insecticide using Broflanilide as a lead compound to obtain structurally diverse meta-diamide compounds. An overview of meta-diamide derivatives from the perspectives of insecticidal activities and mechanism of action is offered. Their potentials as a dominant active structure for development of insecticides are also discussed.
2026, 37(7): 112503
doi: 10.1016/j.cclet.2026.112503
Abstract:
Skin aging is a multifactorial biological process driven by oxidative stress (OS), chronic inflammation, cellular senescence, mitochondrial dysfunction, and non-enzymatic glycation (NEG), and is markedly accelerated by environmental stressors such as ultraviolet radiation (UVR) and air pollution. Natural bioactive compounds, including flavonoids, polyphenols, terpenoids, alkaloids, vitamins, polysaccharides, peptides, and indole derivatives, have demonstrated considerable potential in mitigating these processes through multi-target antioxidant, anti-inflammatory, anti-photoaging, and extracellular matrix (ECM)–protective mechanisms. However, their clinical and cosmetic translation is often limited by poor solubility, chemical instability, and insufficient skin penetration. Rather than providing a simple compilation of existing studies, this review offers a mechanism-oriented and delivery-driven synthesis of recent advances in natural anti-skin-aging research. We systematically integrate current knowledge on the molecular drivers of skin aging with a critical comparison of emerging transdermal and nanotechnology-based delivery systems, including lipid-based, polymer-based, inorganic/hybrid, and nucleic acid–assembled nanocarriers. Particular attention is given to how rational carrier design modulates stability, permeability, skin-layer targeting, and controlled release behavior. Furthermore, this review critically discusses current limitations, contradictory findings across studies, and key translational challenges, and identifies promising future research directions, such as stimuli-responsive systems, skin-layer-specific targeting, and mechanism-guided material selection. By bridging biological mechanisms with delivery material innovation, this work provides a forward-looking framework for the development of safer, more effective, and scientifically grounded anti-skin-aging therapeutics and cosmeceuticals.
Skin aging is a multifactorial biological process driven by oxidative stress (OS), chronic inflammation, cellular senescence, mitochondrial dysfunction, and non-enzymatic glycation (NEG), and is markedly accelerated by environmental stressors such as ultraviolet radiation (UVR) and air pollution. Natural bioactive compounds, including flavonoids, polyphenols, terpenoids, alkaloids, vitamins, polysaccharides, peptides, and indole derivatives, have demonstrated considerable potential in mitigating these processes through multi-target antioxidant, anti-inflammatory, anti-photoaging, and extracellular matrix (ECM)–protective mechanisms. However, their clinical and cosmetic translation is often limited by poor solubility, chemical instability, and insufficient skin penetration. Rather than providing a simple compilation of existing studies, this review offers a mechanism-oriented and delivery-driven synthesis of recent advances in natural anti-skin-aging research. We systematically integrate current knowledge on the molecular drivers of skin aging with a critical comparison of emerging transdermal and nanotechnology-based delivery systems, including lipid-based, polymer-based, inorganic/hybrid, and nucleic acid–assembled nanocarriers. Particular attention is given to how rational carrier design modulates stability, permeability, skin-layer targeting, and controlled release behavior. Furthermore, this review critically discusses current limitations, contradictory findings across studies, and key translational challenges, and identifies promising future research directions, such as stimuli-responsive systems, skin-layer-specific targeting, and mechanism-guided material selection. By bridging biological mechanisms with delivery material innovation, this work provides a forward-looking framework for the development of safer, more effective, and scientifically grounded anti-skin-aging therapeutics and cosmeceuticals.
2026, 37(7): 112238
doi: 10.1016/j.cclet.2025.112238
Abstract:
2026, 37(7): 112552
doi: 10.1016/j.cclet.2026.112552
Abstract:
