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2026 Volume 37 Issue 9
2026, 37(9): 111331
doi: 10.1016/j.cclet.2025.111331
Abstract:
This work investigates the impact of vertex modification on the host-guest chemistry of a hexahedral Zn(Ⅱ)-based metal-organic cage (MOC) 1 containing fluorinated components. Structural characterization via single-crystal X-ray diffraction (SCXRD), 1H NMR, and electrospray ionization time-of-flight mass spectra (ESI-TOF MS) confirmed the low-symmetry hexahedral architectures of 1·NTf2 and 1·OTf, with fluorine atoms positioned at cage windows. 1H/19F NMR spectra of 1·NTf2 and 1·OTf showed slow-exchange binding behavior with external anions. 1·NTf2 had a single set of peaks in the imine signal area, while 1·OTf had two distinct groups of signals. Combined with competitive anion titration results, it can be inferred that NTf2- has a stronger binding affinity with the cage structure. Host-guest studies with pyrene (Py) and its hydrogenated analogs revealed complete displacement of OTf- but not NTf2-, highlighting the superior binding strength of NTf2-. Comparative isothermal titration calorimetry (ITC) data showed reduced association constants for 1·OTf with pyrene (Py) and its analogs 4,5,9,10-tetrahydropyrene (4H-Py) and hexadecahydropyrene (16H-Py) compared to 2·OTf, attributed to electron-withdrawing fluorine substituents altering charge distribution, which was confirmed by the electrostatic potential analysis of the cage skeleton. These findings underscore how vertex functionalization modulates anion selectivity and guest-binding thermodynamics in MOCs, offering insights for designing tailored supramolecular hosts.
This work investigates the impact of vertex modification on the host-guest chemistry of a hexahedral Zn(Ⅱ)-based metal-organic cage (MOC) 1 containing fluorinated components. Structural characterization via single-crystal X-ray diffraction (SCXRD), 1H NMR, and electrospray ionization time-of-flight mass spectra (ESI-TOF MS) confirmed the low-symmetry hexahedral architectures of 1·NTf2 and 1·OTf, with fluorine atoms positioned at cage windows. 1H/19F NMR spectra of 1·NTf2 and 1·OTf showed slow-exchange binding behavior with external anions. 1·NTf2 had a single set of peaks in the imine signal area, while 1·OTf had two distinct groups of signals. Combined with competitive anion titration results, it can be inferred that NTf2- has a stronger binding affinity with the cage structure. Host-guest studies with pyrene (Py) and its hydrogenated analogs revealed complete displacement of OTf- but not NTf2-, highlighting the superior binding strength of NTf2-. Comparative isothermal titration calorimetry (ITC) data showed reduced association constants for 1·OTf with pyrene (Py) and its analogs 4,5,9,10-tetrahydropyrene (4H-Py) and hexadecahydropyrene (16H-Py) compared to 2·OTf, attributed to electron-withdrawing fluorine substituents altering charge distribution, which was confirmed by the electrostatic potential analysis of the cage skeleton. These findings underscore how vertex functionalization modulates anion selectivity and guest-binding thermodynamics in MOCs, offering insights for designing tailored supramolecular hosts.
2026, 37(9): 111344
doi: 10.1016/j.cclet.2025.111344
Abstract:
Poly(ethylene oxide) (PEO) electrolytes present a promising option for next-generation solid-state high-energy-density batteries. However, the poor ionic conductivity and inefficiency transference number pose significant barriers to its broader application. Herein, an in-built synthesis of poly(ethylene oxide) with zwitterionic poly(ionic liquid) composite electrolyte (PEO/Zwit PIL) is employed by a thio-lene click reaction. The introduction of Zwit PIL can help the composite electrolyte fully dissociation lithium salts and optimize the solvation structure. Molecular dynamics simulations elucidate fast Li+ transport through a structural diffusion mechanism upon the addition of Zwit PIL to the composite electrolyte, simultaneously facilitating a high ionic conductivity and transference number. The composite electrolyte also demonstrates a high self-adhesive to construct a robust and tough electrode-electrolyte interface. The assembled full cell (LiFePO4PEO-Zwit PILLi) exhibits a discharge capacity of 153 mAh/g at 60 ℃ and highly stable cyclic performance up to 200 cycles at 0.2 C. The employment of Zwit PIL within PEO for novel solid-state electrolytes furnishes an alternative approach to the design of high-performance, next-generation, sustainable batteries.
Poly(ethylene oxide) (PEO) electrolytes present a promising option for next-generation solid-state high-energy-density batteries. However, the poor ionic conductivity and inefficiency transference number pose significant barriers to its broader application. Herein, an in-built synthesis of poly(ethylene oxide) with zwitterionic poly(ionic liquid) composite electrolyte (PEO/Zwit PIL) is employed by a thio-lene click reaction. The introduction of Zwit PIL can help the composite electrolyte fully dissociation lithium salts and optimize the solvation structure. Molecular dynamics simulations elucidate fast Li+ transport through a structural diffusion mechanism upon the addition of Zwit PIL to the composite electrolyte, simultaneously facilitating a high ionic conductivity and transference number. The composite electrolyte also demonstrates a high self-adhesive to construct a robust and tough electrode-electrolyte interface. The assembled full cell (LiFePO4PEO-Zwit PILLi) exhibits a discharge capacity of 153 mAh/g at 60 ℃ and highly stable cyclic performance up to 200 cycles at 0.2 C. The employment of Zwit PIL within PEO for novel solid-state electrolytes furnishes an alternative approach to the design of high-performance, next-generation, sustainable batteries.
Ru-decorated defective tantalum oxide via laser synthesis for efficient photothermal CO2 methanation
2026, 37(9): 111345
doi: 10.1016/j.cclet.2025.111345
Abstract:
The conversion of carbon dioxide (CO2) into valuable fuels or chemicals through photothermal catalysis is an efficient way to alleviate the global energy crisis and climate change. Regulating active sites and modifying photothermal conversion characteristics are conducive to photothermal catalytic reactions. In this study, the defect-rich tantalum oxide on tantalum foil decorated with Ru nanoparticles (Ru/Ta2O5-x/Ta) was synthesized using pulsed laser under thermal ablation effects. The presence of oxygen defects enhanced the photothermal conversion efficiency. Meanwhile, the interface between Ru and Ta2O5-x facilitated the adsorption of CO2, and Ru nanoparticles served as efficient active sites for the hydrogenation of CO2 to methane (CH4). The Ru/Ta2O5-x/Ta catalyst exhibited excellent photothermal conversion efficiency (reaching 343.4 ℃ at 1.76 W/cm2) and excellent catalytic activity with a CH4 yield of 50.6 mol g(Ru)-1 h-1 (CH4 selectivity of 98%). The experimental and theoretical results demonstrated that the catalytic sites of Ru/Ta2O5-x/Ta in combination with light irradiation promoted CO2 activation, intermediate formation and CO* transformation, thereby accelerating the production of CH4. Moreover, the application of the pulsed laser was extended to construct the photothermal catalyst with high photothermal temperature and efficient catalytic sites.
The conversion of carbon dioxide (CO2) into valuable fuels or chemicals through photothermal catalysis is an efficient way to alleviate the global energy crisis and climate change. Regulating active sites and modifying photothermal conversion characteristics are conducive to photothermal catalytic reactions. In this study, the defect-rich tantalum oxide on tantalum foil decorated with Ru nanoparticles (Ru/Ta2O5-x/Ta) was synthesized using pulsed laser under thermal ablation effects. The presence of oxygen defects enhanced the photothermal conversion efficiency. Meanwhile, the interface between Ru and Ta2O5-x facilitated the adsorption of CO2, and Ru nanoparticles served as efficient active sites for the hydrogenation of CO2 to methane (CH4). The Ru/Ta2O5-x/Ta catalyst exhibited excellent photothermal conversion efficiency (reaching 343.4 ℃ at 1.76 W/cm2) and excellent catalytic activity with a CH4 yield of 50.6 mol g(Ru)-1 h-1 (CH4 selectivity of 98%). The experimental and theoretical results demonstrated that the catalytic sites of Ru/Ta2O5-x/Ta in combination with light irradiation promoted CO2 activation, intermediate formation and CO* transformation, thereby accelerating the production of CH4. Moreover, the application of the pulsed laser was extended to construct the photothermal catalyst with high photothermal temperature and efficient catalytic sites.
2026, 37(9): 111346
doi: 10.1016/j.cclet.2025.111346
Abstract:
In this work, the aggregation-enhanced antenna effect of chiral mononuclear Eu(Ⅲ) complexes containing dynamic modules in aqueous solution was used for the first time to significantly improve the optical imaging performance of various types of cells and zebrafish. Specifically, the chiral mononuclear Eu(Ⅲ) complexes (R/S-1 and R/S-2) containing molecular rotors or vibration unit modules have almost negligible emission in the molecule state, but after aggregation in aqueous solution, they form nanoparticles with a sharp increase in emission peaks. It is worth noting that the above photophysical properties lead to R/S-1 and R/S-2 having high-resolution cell imaging effects on various cells, and localizing in lysosomal organelles. In addition, R/S-1 and R/S-2 also show high-resolution optical imaging effects on zebrafish. This work not only opens a door to expand the bioimaging performance of lanthanide complex emitters but also opens a new perspective for the construction of new dynamic lanthanide complexes with bright emissions.
In this work, the aggregation-enhanced antenna effect of chiral mononuclear Eu(Ⅲ) complexes containing dynamic modules in aqueous solution was used for the first time to significantly improve the optical imaging performance of various types of cells and zebrafish. Specifically, the chiral mononuclear Eu(Ⅲ) complexes (R/S-1 and R/S-2) containing molecular rotors or vibration unit modules have almost negligible emission in the molecule state, but after aggregation in aqueous solution, they form nanoparticles with a sharp increase in emission peaks. It is worth noting that the above photophysical properties lead to R/S-1 and R/S-2 having high-resolution cell imaging effects on various cells, and localizing in lysosomal organelles. In addition, R/S-1 and R/S-2 also show high-resolution optical imaging effects on zebrafish. This work not only opens a door to expand the bioimaging performance of lanthanide complex emitters but also opens a new perspective for the construction of new dynamic lanthanide complexes with bright emissions.
2026, 37(9): 111348
doi: 10.1016/j.cclet.2025.111348
Abstract:
Aqueous zinc-ion batteries are promising candidates for large-scale energy storage, but their practical application is hindered by the issues of Zn dendrite growth and side reactions. To address these challenges, a mesoporous carbon anchored with zincophilic nitrogen and oxygen sites (NOPC) is prepared by pyrolyzing NH4Cl-incorporated ZIF-8 and constructed as a protective layer on Zn anode. In the NOPC layer, the zincophilic nitrogen and oxygen sites facilitate uniform Zn2+ nucleation, while the abundant mesopores homogenize Zn2+ flux, effectively enabling dendrite-free deposition. Moreover, the NOPC layer suppresses interfacial side reactions by isolating the Zn surface from active H2O. Remarkably, the Zn anode protected by the NOPC layer achieves an ultralong cycle life exceeding 6000 h at 1 mA/cm2 and 1 mAh/cm2, and maintains a high Coulombic efficiency of 99.8% for 4600 cycles, indicating superior stability and reversibility. When paired with NaV3O8·1·5H2O cathode, the full cell displays a capacity retention of 85.1% after 3000 cycles at 5 A/g. This study demonstrates that the engineering of zincophilic sites and meso-porosity in carbon-based protective layers represents an effective strategy for enhancing the performance of aqueous zinc-ion batteries.
Aqueous zinc-ion batteries are promising candidates for large-scale energy storage, but their practical application is hindered by the issues of Zn dendrite growth and side reactions. To address these challenges, a mesoporous carbon anchored with zincophilic nitrogen and oxygen sites (NOPC) is prepared by pyrolyzing NH4Cl-incorporated ZIF-8 and constructed as a protective layer on Zn anode. In the NOPC layer, the zincophilic nitrogen and oxygen sites facilitate uniform Zn2+ nucleation, while the abundant mesopores homogenize Zn2+ flux, effectively enabling dendrite-free deposition. Moreover, the NOPC layer suppresses interfacial side reactions by isolating the Zn surface from active H2O. Remarkably, the Zn anode protected by the NOPC layer achieves an ultralong cycle life exceeding 6000 h at 1 mA/cm2 and 1 mAh/cm2, and maintains a high Coulombic efficiency of 99.8% for 4600 cycles, indicating superior stability and reversibility. When paired with NaV3O8·1·5H2O cathode, the full cell displays a capacity retention of 85.1% after 3000 cycles at 5 A/g. This study demonstrates that the engineering of zincophilic sites and meso-porosity in carbon-based protective layers represents an effective strategy for enhancing the performance of aqueous zinc-ion batteries.
2026, 37(9): 111384
doi: 10.1016/j.cclet.2025.111384
Abstract:
Tin-oxo clusters (TOCs) have attracted considerable attention owing to their various structures and wide potential applications. However, there is still a lack of effective methods to assemble high-nuclearity TOCs. Moreover, the periphery of reported TOCs is rarely N-rich ligands, limiting the comprehensive investigation of the structure-property relationship. In this work, we used the strategy of pyrazole-thermal-assisted organotin aggregation to construct a series of the largest N-rich Sn18 clusters with S4 axial symmetry. These Sn18 clusters have inorganic electron-withdrawing halogen atoms and organic electron-rich pyrazole derivatives, differing from the reported high-nuclearity TOCs only with carboxylate ligands. Owing to the high symmetry and multiple electron-withdrawing/-donating ligands, the Sn18 clusters served as the platform to investigate the relationship between structure and third-order nonlinear optical (NLO) property by Z-scan measurement. Different from the single organic ligand in the previous study, the multiple kinds of ligands in the Sn18 clusters have an important effect on the NLO property. Enhancing the push-pull electronic effect and introducing C–Cl···π interactions between different ligands can promote the NLO properties. Thus, CTGU-SnC-16 exhibits the best broadband NLO properties at 532 and 1064 nm, differing from the reported metal-oxo clusters only at 532 nm. This work not only affords an effective synthetic strategy for constructing high-nuclearity TOCs but also deepens the understanding of the structure-property relationship of clusters.
Tin-oxo clusters (TOCs) have attracted considerable attention owing to their various structures and wide potential applications. However, there is still a lack of effective methods to assemble high-nuclearity TOCs. Moreover, the periphery of reported TOCs is rarely N-rich ligands, limiting the comprehensive investigation of the structure-property relationship. In this work, we used the strategy of pyrazole-thermal-assisted organotin aggregation to construct a series of the largest N-rich Sn18 clusters with S4 axial symmetry. These Sn18 clusters have inorganic electron-withdrawing halogen atoms and organic electron-rich pyrazole derivatives, differing from the reported high-nuclearity TOCs only with carboxylate ligands. Owing to the high symmetry and multiple electron-withdrawing/-donating ligands, the Sn18 clusters served as the platform to investigate the relationship between structure and third-order nonlinear optical (NLO) property by Z-scan measurement. Different from the single organic ligand in the previous study, the multiple kinds of ligands in the Sn18 clusters have an important effect on the NLO property. Enhancing the push-pull electronic effect and introducing C–Cl···π interactions between different ligands can promote the NLO properties. Thus, CTGU-SnC-16 exhibits the best broadband NLO properties at 532 and 1064 nm, differing from the reported metal-oxo clusters only at 532 nm. This work not only affords an effective synthetic strategy for constructing high-nuclearity TOCs but also deepens the understanding of the structure-property relationship of clusters.
2026, 37(9): 111388
doi: 10.1016/j.cclet.2025.111388
Abstract:
The instability of the Zn metal anode in aqueous zinc-ion batteries is the main culprit limiting promotion and practicability. Solid-liquid hybrid electrolytes, as an emerging system containing electrochemically inert fillers, have been proposed and shown significant progress in recent years. The electrolyte regulation for suppressing side reactions mainly depends on the state of bound water molecules, so exploring the influence of intrinsic properties of fillers on electrolyte structure is of great significance. This work compared the effects of kaolin and its derived mullite on the state of bound water molecules and electrochemical behaviors in hybrid electrolytes. Relying solely on the high specific surface area of mullite is not sufficient to provide enough ion diffusion paths and limit water molecule activity, resulting in severe polarization and side reactions. The layered structure of kaolin can accommodate a large number of water molecules, which constructs hydrogen bonding networks for H+ transport as the charge carrier with lower energy barrier. Hence, the kaolin-based electrolytes can inherit both low polarization of conventional liquid electrolytes and the durability to side reactions of hybrid electrolytes simultaneously. As a result, the aqueous Zn-MnO2 battery with kaolin-based electrolyte can provide high specific capacity of ~300 mAh/g at 100 mA/g, and maintain at least 164 and 85.2 mAh/g at 300 and 500 mA/g for > 500 cycles.
The instability of the Zn metal anode in aqueous zinc-ion batteries is the main culprit limiting promotion and practicability. Solid-liquid hybrid electrolytes, as an emerging system containing electrochemically inert fillers, have been proposed and shown significant progress in recent years. The electrolyte regulation for suppressing side reactions mainly depends on the state of bound water molecules, so exploring the influence of intrinsic properties of fillers on electrolyte structure is of great significance. This work compared the effects of kaolin and its derived mullite on the state of bound water molecules and electrochemical behaviors in hybrid electrolytes. Relying solely on the high specific surface area of mullite is not sufficient to provide enough ion diffusion paths and limit water molecule activity, resulting in severe polarization and side reactions. The layered structure of kaolin can accommodate a large number of water molecules, which constructs hydrogen bonding networks for H+ transport as the charge carrier with lower energy barrier. Hence, the kaolin-based electrolytes can inherit both low polarization of conventional liquid electrolytes and the durability to side reactions of hybrid electrolytes simultaneously. As a result, the aqueous Zn-MnO2 battery with kaolin-based electrolyte can provide high specific capacity of ~300 mAh/g at 100 mA/g, and maintain at least 164 and 85.2 mAh/g at 300 and 500 mA/g for > 500 cycles.
2026, 37(9): 111412
doi: 10.1016/j.cclet.2025.111412
Abstract:
Guest molecule intercalation is an effective strategy for engineering electron structures and enhancing photocatalytic CO2 reduction. Our designed charge-transfer system incorporates 28 nuclear H2O molecules as electron mediators within the POM-based photocatalyst, enabling efficient electron transport pathways. Comparative analysis of synthesized isostructural catalysts shows water-intercalated Na7[Co2(H2O)8(H11CoP8Mo12O62)]·44H2O (abbr. compound 1) achieves exceptional CO2 reduction activity (21,347.4 µmol g-1 h-1), outperforming anhydrous (C4H14N2)4[Co2(H10CoP8Mo12O62)]·4H2O (abbr. compound 2) by 68%. This work demonstrates that water intercalation simultaneously optimizes band structure and improves material stability, providing a novel paradigm for advanced photocatalytic system design.
Guest molecule intercalation is an effective strategy for engineering electron structures and enhancing photocatalytic CO2 reduction. Our designed charge-transfer system incorporates 28 nuclear H2O molecules as electron mediators within the POM-based photocatalyst, enabling efficient electron transport pathways. Comparative analysis of synthesized isostructural catalysts shows water-intercalated Na7[Co2(H2O)8(H11CoP8Mo12O62)]·44H2O (abbr. compound 1) achieves exceptional CO2 reduction activity (21,347.4 µmol g-1 h-1), outperforming anhydrous (C4H14N2)4[Co2(H10CoP8Mo12O62)]·4H2O (abbr. compound 2) by 68%. This work demonstrates that water intercalation simultaneously optimizes band structure and improves material stability, providing a novel paradigm for advanced photocatalytic system design.
2026, 37(9): 111413
doi: 10.1016/j.cclet.2025.111413
Abstract:
Achieving higher proton conductivity of proton-conducting materials in solid-state is one of the utmost challenges in materials science. Due to their oxygen-rich structure and negative surface charge, polyoxometalates (POMs) anions have high requirements for proton carrier density and proton mobility, and thus have great potential as proton conducting materials. Furthermore, the versatility in modifying the ligand environment or incorporating acidic functional groups in POMs allows for precise tuning of their proton conductivity and stability under operational conditions. Therefore, it is an effective strategy to select a suitable organic ligand to stabilize the [TeMo6O21]2- anion assembled in-situ by covalent modification. In this paper, three [TeMo6O21]2- anionic clusters have been designed and synthesized by using polydentate phosphonate ligands and guided by transition metals, H26[Co6{N(CH2PO3)2(CH2COO)}6(TeMo6O21)4(H2O)8]·64H2O (complex 1), H26[Cu6{N(CH2PO3)2(CH2COO)}6(TeMo6O21)4(H2O)6]·78H2O (complex 2) and H34Na2[Co8{N2(CH2)2(CH2PO3)3(CH2PO3H2)}4(TeMo6O21)6(PO3)4(H2O)16]·84H2O (complex 3). Among them, complexes 1 and 2 are isomorphic, and complexes 1–3 have good proton conduction properties, resulting in values of 1.3 × 10−2, 1.22 × 10−2, and 1.11 × 10−2 S/cm, respectively (75% relative humidity, 80 ℃). This work offers a promising strategy for the development and design of novel telluromolybdate clusters suitable for proton conductive materials.
Achieving higher proton conductivity of proton-conducting materials in solid-state is one of the utmost challenges in materials science. Due to their oxygen-rich structure and negative surface charge, polyoxometalates (POMs) anions have high requirements for proton carrier density and proton mobility, and thus have great potential as proton conducting materials. Furthermore, the versatility in modifying the ligand environment or incorporating acidic functional groups in POMs allows for precise tuning of their proton conductivity and stability under operational conditions. Therefore, it is an effective strategy to select a suitable organic ligand to stabilize the [TeMo6O21]2- anion assembled in-situ by covalent modification. In this paper, three [TeMo6O21]2- anionic clusters have been designed and synthesized by using polydentate phosphonate ligands and guided by transition metals, H26[Co6{N(CH2PO3)2(CH2COO)}6(TeMo6O21)4(H2O)8]·64H2O (complex 1), H26[Cu6{N(CH2PO3)2(CH2COO)}6(TeMo6O21)4(H2O)6]·78H2O (complex 2) and H34Na2[Co8{N2(CH2)2(CH2PO3)3(CH2PO3H2)}4(TeMo6O21)6(PO3)4(H2O)16]·84H2O (complex 3). Among them, complexes 1 and 2 are isomorphic, and complexes 1–3 have good proton conduction properties, resulting in values of 1.3 × 10−2, 1.22 × 10−2, and 1.11 × 10−2 S/cm, respectively (75% relative humidity, 80 ℃). This work offers a promising strategy for the development and design of novel telluromolybdate clusters suitable for proton conductive materials.
2026, 37(9): 111414
doi: 10.1016/j.cclet.2025.111414
Abstract:
Integration of redox ability and conductivity in binder is highly desirable to maximize their functions for high-performance battery requirements. Here, a novel redox covalent organic polymer binder (TTF-COP) has been developed by in-situ polymerizing redox/conductive tetrathiafulvalene unit and adhesive thiourea unit. TTF-COP can achieve one-pot cathode fabrication and simultaneously provide strong interactions with cathodic materials, showing significantly enhanced mechanical strength of the electrode, accelerated capture/conversion of lithium polysulfides (LiPSs), about 10,000 times higher viscosity (at shear rates of 0.1–1 s-1), and about 200 times enhanced electrical conductivity than that of PVDF. TTF-COP based cells exhibit high initial capacity (1126 mAh/g at 0.5 C, 928 mAh/g at 1 C, 611 mAh/g at 5 C, respectively) and excellent cycling stability over 800 cycles at 5 C (0.089% decay per cycle). Moreover, the cell shows an excellent specific capacity of 5.1 mAh/cm2 under a high sulfur loading of 7.1 mg/cm2 and low E/S ratio of 10.7 µL/mg. This work provides a new reference for designing multifunctional binders, hoping to enrich the binding chemistry for sustainable battery targets.
Integration of redox ability and conductivity in binder is highly desirable to maximize their functions for high-performance battery requirements. Here, a novel redox covalent organic polymer binder (TTF-COP) has been developed by in-situ polymerizing redox/conductive tetrathiafulvalene unit and adhesive thiourea unit. TTF-COP can achieve one-pot cathode fabrication and simultaneously provide strong interactions with cathodic materials, showing significantly enhanced mechanical strength of the electrode, accelerated capture/conversion of lithium polysulfides (LiPSs), about 10,000 times higher viscosity (at shear rates of 0.1–1 s-1), and about 200 times enhanced electrical conductivity than that of PVDF. TTF-COP based cells exhibit high initial capacity (1126 mAh/g at 0.5 C, 928 mAh/g at 1 C, 611 mAh/g at 5 C, respectively) and excellent cycling stability over 800 cycles at 5 C (0.089% decay per cycle). Moreover, the cell shows an excellent specific capacity of 5.1 mAh/cm2 under a high sulfur loading of 7.1 mg/cm2 and low E/S ratio of 10.7 µL/mg. This work provides a new reference for designing multifunctional binders, hoping to enrich the binding chemistry for sustainable battery targets.
2026, 37(9): 111416
doi: 10.1016/j.cclet.2025.111416
Abstract:
In this work, we report the controllable synthesis and characterization of four atomically precise silver clusters, Ag18(SbW9O33)2(DPPP)8 (1, DPPP = 1,3-bis(diphenyphosphino)propane), Ag18(SbW9O33)2(DPPB)8 (2, DPPB = 1,4-bis(diphenylphosphino)butane), Ag18(SbW9O33)2(DPPPe)8 (3, DPPPe = 1,5-bis(diphenylphosphino)pentane), and Ag18(SbW9O33)2(TPP)14 (4, TPP = triphenylphosphine) by using a facile one-pot solvothermal approach. The resulting four Ag clusters exhibit similar lacunary [SbW9O33]9‒ ({SbW9O33})-sandwiched structures, which can be adjusted by the external different phosphine ligands. In addition, all four clusters display variable physicochemical and catalytic performance, correlating well to their distinct molecular structures.
In this work, we report the controllable synthesis and characterization of four atomically precise silver clusters, Ag18(SbW9O33)2(DPPP)8 (1, DPPP = 1,3-bis(diphenyphosphino)propane), Ag18(SbW9O33)2(DPPB)8 (2, DPPB = 1,4-bis(diphenylphosphino)butane), Ag18(SbW9O33)2(DPPPe)8 (3, DPPPe = 1,5-bis(diphenylphosphino)pentane), and Ag18(SbW9O33)2(TPP)14 (4, TPP = triphenylphosphine) by using a facile one-pot solvothermal approach. The resulting four Ag clusters exhibit similar lacunary [SbW9O33]9‒ ({SbW9O33})-sandwiched structures, which can be adjusted by the external different phosphine ligands. In addition, all four clusters display variable physicochemical and catalytic performance, correlating well to their distinct molecular structures.
2026, 37(9): 111435
doi: 10.1016/j.cclet.2025.111435
Abstract:
Lithium-metal batteries (LMBs) are promising next-generation high-energy-density systems due to lithium's high theoretical capacity. However, while ester-based electrolytes support high-voltage cathodes, their poor compatibility with lithium metal hinders progress. In this study, a porous material with sub-nanochannels was constructed on lithium metal, inducing a pre-desolvation process that promotes a highly aggregative nano-confined electrolyte. This design mitigates solvent-lithium reactivity, enabling dendrite-free deposition and a stable LiF-rich solid electrolyte interphase (SEI). As a result, NCM-811//Li (LiNi0.8Co0.1Mn0.1O2//Li) cell achieved exceptional cycling stability (89.2% capacity retention after > 400 cycles). This strategy provides a viable pathway for advanced high-energy-density batteries.
Lithium-metal batteries (LMBs) are promising next-generation high-energy-density systems due to lithium's high theoretical capacity. However, while ester-based electrolytes support high-voltage cathodes, their poor compatibility with lithium metal hinders progress. In this study, a porous material with sub-nanochannels was constructed on lithium metal, inducing a pre-desolvation process that promotes a highly aggregative nano-confined electrolyte. This design mitigates solvent-lithium reactivity, enabling dendrite-free deposition and a stable LiF-rich solid electrolyte interphase (SEI). As a result, NCM-811//Li (LiNi0.8Co0.1Mn0.1O2//Li) cell achieved exceptional cycling stability (89.2% capacity retention after > 400 cycles). This strategy provides a viable pathway for advanced high-energy-density batteries.
2026, 37(9): 111436
doi: 10.1016/j.cclet.2025.111436
Abstract:
Although the incorporation of fillers has improved the high temperature (150–200 ℃) capacitance of polymer composite dielectrics, effective strategies for designing filler-matrix interface structures remains a formidable challenge. Herein, defect-rich nanosheets (Ca2Nb2.75Ti0.25O10, CT) were coated with a zeolite imidazolate frameworks-8 (ZIF-8, Zn(C4H5N2)2) layer (mCT). The mCT was integrated into polyetherimide (PEI) to create the polymer-based dielectrics. The defects on the surface of the negative CT nanosheets exhibited strong anchoring effects on the Zn2+ in ZIF-8, enhancing the filler-coating layer interface. Additionally, X-ray absorption fine structure analysis and density functional theory confirmed that the porous ZIF-8 coating layer forms strong coordination bonds with the PEI molecular chains, thereby an increased band gap (3.3 eV) of PEI/mCT compared to PEI (3.0 eV). It demonstrated exceptional performance at high temperatures, achieving ultra-high energy storage densities of 5.25 and 4.47 J/cm3 with efficiency > 90% at 150 and 200 ℃, which are higher than PEI (0.4 and 0.4 J/cm3). This work offers a new approach and reference for designing high-temperature polymer composite dielectrics for energy storage applications.
Although the incorporation of fillers has improved the high temperature (150–200 ℃) capacitance of polymer composite dielectrics, effective strategies for designing filler-matrix interface structures remains a formidable challenge. Herein, defect-rich nanosheets (Ca2Nb2.75Ti0.25O10, CT) were coated with a zeolite imidazolate frameworks-8 (ZIF-8, Zn(C4H5N2)2) layer (mCT). The mCT was integrated into polyetherimide (PEI) to create the polymer-based dielectrics. The defects on the surface of the negative CT nanosheets exhibited strong anchoring effects on the Zn2+ in ZIF-8, enhancing the filler-coating layer interface. Additionally, X-ray absorption fine structure analysis and density functional theory confirmed that the porous ZIF-8 coating layer forms strong coordination bonds with the PEI molecular chains, thereby an increased band gap (3.3 eV) of PEI/mCT compared to PEI (3.0 eV). It demonstrated exceptional performance at high temperatures, achieving ultra-high energy storage densities of 5.25 and 4.47 J/cm3 with efficiency > 90% at 150 and 200 ℃, which are higher than PEI (0.4 and 0.4 J/cm3). This work offers a new approach and reference for designing high-temperature polymer composite dielectrics for energy storage applications.
2026, 37(9): 111438
doi: 10.1016/j.cclet.2025.111438
Abstract:
Li-S batteries (LSBs) offer significant promise for next-generation energy storage systems on account of their high energy density and the high capacity of sulfur. Nevertheless, the severe shuttle effect of lithium polysulfide (LiPSs) and the sluggish reaction kinetics greatly hinder the further application of LSBs. In this manuscript, Hollow CeOx/CoS core-shell hybrid were designed and synthesized using ZIF-67 as the self-template to prepare hollow CoS dodecahedral nanoboxs and the subsequent generation of CeOx nanodots. When used as the polyolefin separator modifier, the unique dodecahedral structure of hollow CoS/CeOx presents large specific surface area, abundant porous structure and enough active sites, which not only ensures the fast transport of electrolyte/ions and offers numerous active catalytic sites to accelerate the reaction kinetics of LiPSs. In addition, the catalytic activity of the CeOx/CoS hybrid greatly enhance the uniform ion diffusion and stable growth of lithium nucleation on the lithium metal anode side. The cell with CeOx/CoS modified separator presented excellent long cycle stability and satisfactory rate performance. The battery can maintain the capacity of 502.2 mAh/g after 900 cycles at the current density of 1 C, accompanying by a minimal 2 decay rate of 0.057%. Even at a current density of 3 C, a high specific capacity of 735.58 mAh/g can still obtained. Besides, when the sulfur loading increase into 4.480 mg/cm2, the battery still can maintain excellent cycling stability with the capacity retention ratio of 94.5% after 100 cycles. This study will provide new strategy for the design and preparation of heterostructure with outstanding catalytic performance for LSBs.
Li-S batteries (LSBs) offer significant promise for next-generation energy storage systems on account of their high energy density and the high capacity of sulfur. Nevertheless, the severe shuttle effect of lithium polysulfide (LiPSs) and the sluggish reaction kinetics greatly hinder the further application of LSBs. In this manuscript, Hollow CeOx/CoS core-shell hybrid were designed and synthesized using ZIF-67 as the self-template to prepare hollow CoS dodecahedral nanoboxs and the subsequent generation of CeOx nanodots. When used as the polyolefin separator modifier, the unique dodecahedral structure of hollow CoS/CeOx presents large specific surface area, abundant porous structure and enough active sites, which not only ensures the fast transport of electrolyte/ions and offers numerous active catalytic sites to accelerate the reaction kinetics of LiPSs. In addition, the catalytic activity of the CeOx/CoS hybrid greatly enhance the uniform ion diffusion and stable growth of lithium nucleation on the lithium metal anode side. The cell with CeOx/CoS modified separator presented excellent long cycle stability and satisfactory rate performance. The battery can maintain the capacity of 502.2 mAh/g after 900 cycles at the current density of 1 C, accompanying by a minimal 2 decay rate of 0.057%. Even at a current density of 3 C, a high specific capacity of 735.58 mAh/g can still obtained. Besides, when the sulfur loading increase into 4.480 mg/cm2, the battery still can maintain excellent cycling stability with the capacity retention ratio of 94.5% after 100 cycles. This study will provide new strategy for the design and preparation of heterostructure with outstanding catalytic performance for LSBs.
2026, 37(9): 111439
doi: 10.1016/j.cclet.2025.111439
Abstract:
Bromine, a vital industrial chemical raw material with extensive applications, faces extraction challenges from diluted underground brine due to high energy consumption and low efficiency in conventional methods. In this study, we introduce a CO2 activation of acid-thermal treated graphite felt (AHGF-Y) as a highly effective negative electrode for bromine extraction, achieving remarkable efficiency exceeding 90%. With enriched oxygen-containing functional groups introduced by CO2 activation serving as active sites, the engineered bromine extraction electrodes demonstrates superior bromine oxidation reaction (BrOR) under high Cl/Br ratio conditions. Coupled with hydrogen production, in electrolyte with a Cl/Br ratio of 38, AHGF-Y operated at a low overpotential and achieved remarkable bromine extraction efficiency (94%), with minimal energy consumption (1.61 kJ/g). Notably, when applied to underground brine with high Cl/Br ratio of 255 and multiple interfering ions, AHGF-Y maintained extraction efficiency of 95.5%, significantly outperforming other reported works. Furthermore, AHGF-Y achieved an near-unity Faradaic efficiency (F.E.) of up to 99.7% in a scale-up hydrogen-bromine flow cell (HBFC), enabling simultaneous bromine extraction and hydrogen production. These results highlighted the potential of AHGF-Y as a sustainable and efficient material for large-scale bromine extraction from underground brine.
Bromine, a vital industrial chemical raw material with extensive applications, faces extraction challenges from diluted underground brine due to high energy consumption and low efficiency in conventional methods. In this study, we introduce a CO2 activation of acid-thermal treated graphite felt (AHGF-Y) as a highly effective negative electrode for bromine extraction, achieving remarkable efficiency exceeding 90%. With enriched oxygen-containing functional groups introduced by CO2 activation serving as active sites, the engineered bromine extraction electrodes demonstrates superior bromine oxidation reaction (BrOR) under high Cl/Br ratio conditions. Coupled with hydrogen production, in electrolyte with a Cl/Br ratio of 38, AHGF-Y operated at a low overpotential and achieved remarkable bromine extraction efficiency (94%), with minimal energy consumption (1.61 kJ/g). Notably, when applied to underground brine with high Cl/Br ratio of 255 and multiple interfering ions, AHGF-Y maintained extraction efficiency of 95.5%, significantly outperforming other reported works. Furthermore, AHGF-Y achieved an near-unity Faradaic efficiency (F.E.) of up to 99.7% in a scale-up hydrogen-bromine flow cell (HBFC), enabling simultaneous bromine extraction and hydrogen production. These results highlighted the potential of AHGF-Y as a sustainable and efficient material for large-scale bromine extraction from underground brine.
2026, 37(9): 111456
doi: 10.1016/j.cclet.2025.111456
Abstract:
Layered V5O12·6H2O is a cathode material with great development potential for aqueous zinc-ion batteries due to its large interlayer spacing (~1.18 nm), high proportion of V4+, and abundant interlayer H2O. However, its low electronic conductivity and poor lattice stability lead to significant capacity degradation. In this regard, we develop a synergistic pre-intercalation & coating engineering, where Ni2+, Mn2+, or Zn2+ cations are pre-intercalated by one-step hydrothermal approach, and graphite oxides (GO) are coated by an electrostatic self-assembly strategy. It is found that Zn2+ pre-intercalation shows a better enhancement effect on the Zn2+/H+ storage reversibility and stability, and the charge and mass transfer kinetics. Meanwhile, the synergistic effect of Zn2+ pre-intercalation and GO coating achieves the enhancement of the cycling performance and rate capacity with the minimal loss of initial capacities, where the discharge capacity of 288.3 and 183.3 mAh/g with the retention of 85.0% and 61.6% are achieved at 1 and 3 A/g after 150 and 600 cycles, respectively. The excellent electrochemical performance is attributed to the biggest downward shift of the p-band center of oxygen, the moderate radius of Zn2+, and the coating of ultrathin GO with high electrical conductivity.
Layered V5O12·6H2O is a cathode material with great development potential for aqueous zinc-ion batteries due to its large interlayer spacing (~1.18 nm), high proportion of V4+, and abundant interlayer H2O. However, its low electronic conductivity and poor lattice stability lead to significant capacity degradation. In this regard, we develop a synergistic pre-intercalation & coating engineering, where Ni2+, Mn2+, or Zn2+ cations are pre-intercalated by one-step hydrothermal approach, and graphite oxides (GO) are coated by an electrostatic self-assembly strategy. It is found that Zn2+ pre-intercalation shows a better enhancement effect on the Zn2+/H+ storage reversibility and stability, and the charge and mass transfer kinetics. Meanwhile, the synergistic effect of Zn2+ pre-intercalation and GO coating achieves the enhancement of the cycling performance and rate capacity with the minimal loss of initial capacities, where the discharge capacity of 288.3 and 183.3 mAh/g with the retention of 85.0% and 61.6% are achieved at 1 and 3 A/g after 150 and 600 cycles, respectively. The excellent electrochemical performance is attributed to the biggest downward shift of the p-band center of oxygen, the moderate radius of Zn2+, and the coating of ultrathin GO with high electrical conductivity.
2026, 37(9): 111457
doi: 10.1016/j.cclet.2025.111457
Abstract:
The sluggish dynamics of photogenerated carriers and low sunlight absorption rate severely impede the performance of ZnIn2S4-based photocatalysts. To enhance their photoactivity, Sv-ZnIn2S4@AgBiS2 (Sv-ZIS@ABS) heterostructure composites with sulfur-rich vacancies were synthesized by growing ZnIn2S4 nanosheets on the surface of AgBiS2 through a one-step solvothermal method. The results demonstrate that the Sv-ZIS@ABS composites possess a substantially larger specific surface area and remarkable photocatalytic performance, achieving a hydrogen evolution rate of 4560.2 µmol h-1 g-1, approximately 14.27 times higher than that of pristine ZIS. The electron transfer kinetics in the ZIS@ABS heterojunction were thoroughly investigated using photoluminescence (PL), charge differential density, kelvin probe force microscope (KPFM), and in situ XPS, etc. Based on photocatalytic H2 evolution experiments and density functional theory (DFT) calculations, a plausible photocatalytic mechanism for the Sv-ZIS@ABS composites was proposed. This study provides valuable insights into the design of highly efficient transition metal sulfide-based heterojunction photocatalysts, with a focus on optimizing electron transfer kinetics in these semiconductor materials.
The sluggish dynamics of photogenerated carriers and low sunlight absorption rate severely impede the performance of ZnIn2S4-based photocatalysts. To enhance their photoactivity, Sv-ZnIn2S4@AgBiS2 (Sv-ZIS@ABS) heterostructure composites with sulfur-rich vacancies were synthesized by growing ZnIn2S4 nanosheets on the surface of AgBiS2 through a one-step solvothermal method. The results demonstrate that the Sv-ZIS@ABS composites possess a substantially larger specific surface area and remarkable photocatalytic performance, achieving a hydrogen evolution rate of 4560.2 µmol h-1 g-1, approximately 14.27 times higher than that of pristine ZIS. The electron transfer kinetics in the ZIS@ABS heterojunction were thoroughly investigated using photoluminescence (PL), charge differential density, kelvin probe force microscope (KPFM), and in situ XPS, etc. Based on photocatalytic H2 evolution experiments and density functional theory (DFT) calculations, a plausible photocatalytic mechanism for the Sv-ZIS@ABS composites was proposed. This study provides valuable insights into the design of highly efficient transition metal sulfide-based heterojunction photocatalysts, with a focus on optimizing electron transfer kinetics in these semiconductor materials.
2026, 37(9): 111478
doi: 10.1016/j.cclet.2025.111478
Abstract:
The efficient removal of CF3CH2F and CF3CHF2 to obtain high-purity C2F6 is of critical importance for electronics industry but remains a big challenge. Currently, few adsorbents have been developed for one-step purification of C2F6 from multicomponent perfluorocarbons and hydrofluorocarbons mixtures. Herein, we report a metal-organic framework (FJI-W20) with multiple immobilized hydrogen-bond acceptors including F, O, N atoms which can form hydrogen bonds interactions with the H atoms of CF3CH2F and CF3CHF2, prompting it high selectivities for CF3CH2F/C2F6 and CF3CHF2/C2F6. More importantly, the special cage-like structure in turn ensures the high adsorption capacities of CF3CH2F and CF3CHF2. Adsorption experiments show that FJI-W20 can absorb 132.9 cm3/g of CF3CH2F and 110.1 cm3/g of CF3CHF2 but only adsorb 57.9 cm3/g of C2F6 at 298 K and 1 bar, delivering the selectivities as high as 17.6 and 12.3 for CF3CH2F/C2F6 (5/95, v/v) and CF3CHF2/C2F6 (5/95, v/v). Practical breakthrough experiments indicate that FJI-W20 can purify C2F6 from CF3CH2F/CF3CHF2/C2F6 (5/5/90, v/v/v) in one step at different gas flow rates as well as various temperatures and 20.6 mol/kg of high-purity (≥99.99%) C2F6 can be directly obtained under ambient conditions.
The efficient removal of CF3CH2F and CF3CHF2 to obtain high-purity C2F6 is of critical importance for electronics industry but remains a big challenge. Currently, few adsorbents have been developed for one-step purification of C2F6 from multicomponent perfluorocarbons and hydrofluorocarbons mixtures. Herein, we report a metal-organic framework (FJI-W20) with multiple immobilized hydrogen-bond acceptors including F, O, N atoms which can form hydrogen bonds interactions with the H atoms of CF3CH2F and CF3CHF2, prompting it high selectivities for CF3CH2F/C2F6 and CF3CHF2/C2F6. More importantly, the special cage-like structure in turn ensures the high adsorption capacities of CF3CH2F and CF3CHF2. Adsorption experiments show that FJI-W20 can absorb 132.9 cm3/g of CF3CH2F and 110.1 cm3/g of CF3CHF2 but only adsorb 57.9 cm3/g of C2F6 at 298 K and 1 bar, delivering the selectivities as high as 17.6 and 12.3 for CF3CH2F/C2F6 (5/95, v/v) and CF3CHF2/C2F6 (5/95, v/v). Practical breakthrough experiments indicate that FJI-W20 can purify C2F6 from CF3CH2F/CF3CHF2/C2F6 (5/5/90, v/v/v) in one step at different gas flow rates as well as various temperatures and 20.6 mol/kg of high-purity (≥99.99%) C2F6 can be directly obtained under ambient conditions.
2026, 37(9): 111480
doi: 10.1016/j.cclet.2025.111480
Abstract:
Composite bipolar plates (CBPs) composed of resin and conductive fillers have the potential to combine excellent conductivity with superior mechanical properties, as key components in proton exchange membrane fuel cells (PEMFCs). However, the industrial scalability is hindered by slow curing kinetics and trade-offs between conductivity and mechanical integrity. In this work, we propose a rapid compression molding strategy catalyzed by 2-methylimidazole (2MI), which utilizes the synergistic effect of tertiary amine catalysis and nucleophilic enhancement to reduce the energy barrier of epoxy ring opening, enabling the resin to achieve ultrafast curing. And with temperature and pressure regulation, CBPs achieve good contact between graphite particles and a dense structure, resulting in outstanding in-plane conductivity of 190 S/cm, flexural strength of 85 MPa, and hydrogen permeability below 1.5 × 10–10 cm3/(cm2 s). The work provides a paradigm for resin-curing synergy, bridging rapid processing with multifunctional performance, and advancing scalable PEMFC component manufacturing.
Composite bipolar plates (CBPs) composed of resin and conductive fillers have the potential to combine excellent conductivity with superior mechanical properties, as key components in proton exchange membrane fuel cells (PEMFCs). However, the industrial scalability is hindered by slow curing kinetics and trade-offs between conductivity and mechanical integrity. In this work, we propose a rapid compression molding strategy catalyzed by 2-methylimidazole (2MI), which utilizes the synergistic effect of tertiary amine catalysis and nucleophilic enhancement to reduce the energy barrier of epoxy ring opening, enabling the resin to achieve ultrafast curing. And with temperature and pressure regulation, CBPs achieve good contact between graphite particles and a dense structure, resulting in outstanding in-plane conductivity of 190 S/cm, flexural strength of 85 MPa, and hydrogen permeability below 1.5 × 10–10 cm3/(cm2 s). The work provides a paradigm for resin-curing synergy, bridging rapid processing with multifunctional performance, and advancing scalable PEMFC component manufacturing.
2026, 37(9): 111481
doi: 10.1016/j.cclet.2025.111481
Abstract:
Diabetic wound healing is hindered by multidrug-resistant bacteria, hyperglycemia, and oxidative stress, making bacterial control and microenvironment modulation crucial. However, an all-in-one strategy is still under development. We report a cascade catalytic hydrogel by incorporating quantum-sized Au−Cu bimetallic nanoclusters with dual enzyme-mimetic activities and glucose oxidase into a cross-linked matrix of oxidized chondroitin sulfate and carboxymethyl chitosan. Three objectives are achieved in this system: (1) Utilizing glucose oxidase to decrease blood glucose levels while generating H2O2. (2) Producing hydroxyl radicals via peroxidase-like activity of Au−Cu nanoclusters, while simultaneously functioning as a glutathione peroxidase-like to deplete GSH levels, thereby achieving effective antibacterial effect. (3) The Schiff base bonds (-CH=N-) within the hydrogel will responsively cleavage under slightly acidic environment of wound to release the oxidized chondroitin sulfate, which is benefit for down-regulating the levels of inflammatory factors (TNF-α and IL-6), ultimately achieving an anti-inflammatory effect. Comprehensive in vitro and in vivo evaluations, including antibacterial testing, biocompatibility, rapid hemostasis (within 7 min), and 16S rRNA gene sequencing, revealed that the hydrogel effectively restored microbial diversity and rectified the disrupted wound microenvironment. This work established the Au−Cu/GOx-integrated hydrogel as a promising therapeutic platform for treating infected diabetic wounds and highlights the potential of Au–Cu nanoclusters in clinical application.
Diabetic wound healing is hindered by multidrug-resistant bacteria, hyperglycemia, and oxidative stress, making bacterial control and microenvironment modulation crucial. However, an all-in-one strategy is still under development. We report a cascade catalytic hydrogel by incorporating quantum-sized Au−Cu bimetallic nanoclusters with dual enzyme-mimetic activities and glucose oxidase into a cross-linked matrix of oxidized chondroitin sulfate and carboxymethyl chitosan. Three objectives are achieved in this system: (1) Utilizing glucose oxidase to decrease blood glucose levels while generating H2O2. (2) Producing hydroxyl radicals via peroxidase-like activity of Au−Cu nanoclusters, while simultaneously functioning as a glutathione peroxidase-like to deplete GSH levels, thereby achieving effective antibacterial effect. (3) The Schiff base bonds (-CH=N-) within the hydrogel will responsively cleavage under slightly acidic environment of wound to release the oxidized chondroitin sulfate, which is benefit for down-regulating the levels of inflammatory factors (TNF-α and IL-6), ultimately achieving an anti-inflammatory effect. Comprehensive in vitro and in vivo evaluations, including antibacterial testing, biocompatibility, rapid hemostasis (within 7 min), and 16S rRNA gene sequencing, revealed that the hydrogel effectively restored microbial diversity and rectified the disrupted wound microenvironment. This work established the Au−Cu/GOx-integrated hydrogel as a promising therapeutic platform for treating infected diabetic wounds and highlights the potential of Au–Cu nanoclusters in clinical application.
2026, 37(9): 111490
doi: 10.1016/j.cclet.2025.111490
Abstract:
With the rapid advancement of solar cell and radiation detector technology, understanding and controlling intrinsic defects in semiconductor materials is crucial for improving photovoltaic device performance. This study employs density functional theory (DFT) and non-adiabatic molecular dynamics (NAMD) methods to investigate the ground-state properties of intrinsic defects in CdTeSe (CTS) material and their impact on carrier dynamics. The results demonstrate that defect formation is strongly influenced by the chemical environment: acceptor defects are favored in Te-rich conditions, donor defects are promoted in Cd-rich conditions, while Se substitution at the Te site (SeTe) and Te substitution at the Se site (TeSe) defects are readily formed under various conditions due to their low formation energies. Carrier lifetime is significantly affected by various defects, as shown by their modulation of electron-phonon coupling interactions in electron-hole recombination dynamics. SeCd and TeCd defects are characterized by strong coupling between local vibrational modes and band-edge states, which enhances non-adiabatic coupling (NAC) strength and reduces recombination times to 9.44 ns and 30.95 ns, respectively. In contrast, SeTe and TeSe defects suppress the NAC by markedly reducing coupling, thereby extending the recombination times to 198.04 ns and 239.5 ns. Fourier transform analysis further indicates that the low-frequency phonon modes associated with SeTe and TeSe defects enhance carrier dynamics by optimizing phonon-assisted processes. Finally, it is found that variations in carrier concentration have a significant impact on carrier recombination, especially at high non-equilibrium carrier concentrations, which notably shorten the carrier lifetime. This study offers a theoretical framework for the performance optimization and defect engineering of CTS material in high-efficiency solar cell applications.
With the rapid advancement of solar cell and radiation detector technology, understanding and controlling intrinsic defects in semiconductor materials is crucial for improving photovoltaic device performance. This study employs density functional theory (DFT) and non-adiabatic molecular dynamics (NAMD) methods to investigate the ground-state properties of intrinsic defects in CdTeSe (CTS) material and their impact on carrier dynamics. The results demonstrate that defect formation is strongly influenced by the chemical environment: acceptor defects are favored in Te-rich conditions, donor defects are promoted in Cd-rich conditions, while Se substitution at the Te site (SeTe) and Te substitution at the Se site (TeSe) defects are readily formed under various conditions due to their low formation energies. Carrier lifetime is significantly affected by various defects, as shown by their modulation of electron-phonon coupling interactions in electron-hole recombination dynamics. SeCd and TeCd defects are characterized by strong coupling between local vibrational modes and band-edge states, which enhances non-adiabatic coupling (NAC) strength and reduces recombination times to 9.44 ns and 30.95 ns, respectively. In contrast, SeTe and TeSe defects suppress the NAC by markedly reducing coupling, thereby extending the recombination times to 198.04 ns and 239.5 ns. Fourier transform analysis further indicates that the low-frequency phonon modes associated with SeTe and TeSe defects enhance carrier dynamics by optimizing phonon-assisted processes. Finally, it is found that variations in carrier concentration have a significant impact on carrier recombination, especially at high non-equilibrium carrier concentrations, which notably shorten the carrier lifetime. This study offers a theoretical framework for the performance optimization and defect engineering of CTS material in high-efficiency solar cell applications.
Anchoring Co nanoparticles in P, I-doped carbon skeleton for highly efficient potassium metal anodes
2026, 37(9): 111508
doi: 10.1016/j.cclet.2025.111508
Abstract:
Owing to the low redox potential and high theoretical specific capacity, potassium metal batteries (PMBs) have become one of the suitable candidates for high specific energy batteries. However, challenges including uncontrolled dendrite growth and interfacial instability severely hinder their practical applications. Herein, we develop a cobalt-anchored, phosphorus-iodine co-doped 3D carbon skeleton (PI-Co/GCNT) that synergistically integrates heteroatom co-doping effects and structural engineering to address these limitations. Experiments reveal that the doping of P and I induces charge redistribution on the Co/GCNT, which collectively enhances the K+ adsorption energy compared to Co/GCNT and GCNT. This strategy creates abundant potassiophilic sites that reduce nucleation overpotential (14 mV) and inhibit dendrite growth. The 3D porous architecture not only accommodates volume fluctuations but also ensures rapid ion transport through low-tortuosity channels. The assembled K-PI-Co/GCNT symmetrical cells keep cycling over 1000 h at 1 mA/cm2 with a low polarization of 40 mV. Paired with organic cathodes (PTCDA), the K-PI-Co/GCNT anode delivers superior cycle and rate performance compared to the bare K in full cells. This work elucidates the critical role of heteroatom co-doping for dendrite-free anodes, providing a universal design paradigm for alkali metal batteries.
Owing to the low redox potential and high theoretical specific capacity, potassium metal batteries (PMBs) have become one of the suitable candidates for high specific energy batteries. However, challenges including uncontrolled dendrite growth and interfacial instability severely hinder their practical applications. Herein, we develop a cobalt-anchored, phosphorus-iodine co-doped 3D carbon skeleton (PI-Co/GCNT) that synergistically integrates heteroatom co-doping effects and structural engineering to address these limitations. Experiments reveal that the doping of P and I induces charge redistribution on the Co/GCNT, which collectively enhances the K+ adsorption energy compared to Co/GCNT and GCNT. This strategy creates abundant potassiophilic sites that reduce nucleation overpotential (14 mV) and inhibit dendrite growth. The 3D porous architecture not only accommodates volume fluctuations but also ensures rapid ion transport through low-tortuosity channels. The assembled K-PI-Co/GCNT symmetrical cells keep cycling over 1000 h at 1 mA/cm2 with a low polarization of 40 mV. Paired with organic cathodes (PTCDA), the K-PI-Co/GCNT anode delivers superior cycle and rate performance compared to the bare K in full cells. This work elucidates the critical role of heteroatom co-doping for dendrite-free anodes, providing a universal design paradigm for alkali metal batteries.
2026, 37(9): 111515
doi: 10.1016/j.cclet.2025.111515
Abstract:
Mn-based organic-inorganic hybrid metal halides have attracted extensive attention due to their excellent luminescence properties, easy processing, low cost, and non-toxicity. Herein, we effectively improved the luminescence properties and stability of the [C6H14N]2MnBr4 adopting the chlorination effect. Specifically, through the introduction of chlorine atom on the cations, the Mn-Mn distance in [C6H13NCl]2MnBr4 increases from 8.061 Å to 8.668 Å, thereby suppressing excitation energy transfer between adjacent Mn2+ centers and enhancing the overall luminescent efficiency from 38.8% to 74.5%. Further experimental and theoretical analyses reveal that such chlorination effect increased the H···Cl interactions, significantly improving the environmental stability of Mn-based metal halides. Moreover, compare to [C6H14N]2MnBr4, the CIE chromaticity coordinates of [C6H13NCl]2MnBr4 are much closer to the NTSC green standard (0.23, 0.69). Our work provides new insights into the relationship between the cation structure and optical properties in Mn-based metal halides and sheds light on the design of stable metal halide materials.
Mn-based organic-inorganic hybrid metal halides have attracted extensive attention due to their excellent luminescence properties, easy processing, low cost, and non-toxicity. Herein, we effectively improved the luminescence properties and stability of the [C6H14N]2MnBr4 adopting the chlorination effect. Specifically, through the introduction of chlorine atom on the cations, the Mn-Mn distance in [C6H13NCl]2MnBr4 increases from 8.061 Å to 8.668 Å, thereby suppressing excitation energy transfer between adjacent Mn2+ centers and enhancing the overall luminescent efficiency from 38.8% to 74.5%. Further experimental and theoretical analyses reveal that such chlorination effect increased the H···Cl interactions, significantly improving the environmental stability of Mn-based metal halides. Moreover, compare to [C6H14N]2MnBr4, the CIE chromaticity coordinates of [C6H13NCl]2MnBr4 are much closer to the NTSC green standard (0.23, 0.69). Our work provides new insights into the relationship between the cation structure and optical properties in Mn-based metal halides and sheds light on the design of stable metal halide materials.
2026, 37(9): 111528
doi: 10.1016/j.cclet.2025.111528
Abstract:
Solid polymer electrolyte (SPEs) modified by inorganic fillers has become a simple and effective strategy to improve ionic conductivity and mechanical strength. However, the uneven charge distribution at the interface of polymer electrolyte/electrode results in unstable interfaces and poor cycle performances. Herein, ferromagnetic (La0.60Sr0.40)0.95Co0.20Fe0.80O3-δ (LSCF) has been firstly proposed as filler for PVDF-based electrolyte (PLSCF) to address these critical challenges in solid-state Li metal battery. It has been demonstrated that LSCF filler cannot only increase the ratio of amorphous phase in the polymer, but also induce the rearrangement of PVDF molecular chains under an applied external magnetic field during the preparation process, which can facilitate the generation of the β-phase and promote the dissociation of Li+. The synthesized PLSCF electrolyte exhibits appealing physicochemical properties, including enhanced ionic conductivity (2.09×10−4 S/cm), reduced activation energy (0.142 eV), and improved mechanical robustness (1.286 MPa), which can contribute to a homogeneous lithium deposition on Li metal anode. Furthermore, LSCF can establish an even electric field at the PLSCF/cathode interface, which helps to weaken the space charging layer and construct a robust cathode/electrolyte interface (CEI). As a result, both solid-state Li/Li symmetric cells and LiNi0.6Co0.2Mn0.2O2/Li full cells incorporating the PLSCF electrolyte exhibit significantly improved cycling stability and rate capability. This work enriches inorganic fillers to stabilize electrode/electrolyte interface for high-performance solid-state Li metal batteries.
Solid polymer electrolyte (SPEs) modified by inorganic fillers has become a simple and effective strategy to improve ionic conductivity and mechanical strength. However, the uneven charge distribution at the interface of polymer electrolyte/electrode results in unstable interfaces and poor cycle performances. Herein, ferromagnetic (La0.60Sr0.40)0.95Co0.20Fe0.80O3-δ (LSCF) has been firstly proposed as filler for PVDF-based electrolyte (PLSCF) to address these critical challenges in solid-state Li metal battery. It has been demonstrated that LSCF filler cannot only increase the ratio of amorphous phase in the polymer, but also induce the rearrangement of PVDF molecular chains under an applied external magnetic field during the preparation process, which can facilitate the generation of the β-phase and promote the dissociation of Li+. The synthesized PLSCF electrolyte exhibits appealing physicochemical properties, including enhanced ionic conductivity (2.09×10−4 S/cm), reduced activation energy (0.142 eV), and improved mechanical robustness (1.286 MPa), which can contribute to a homogeneous lithium deposition on Li metal anode. Furthermore, LSCF can establish an even electric field at the PLSCF/cathode interface, which helps to weaken the space charging layer and construct a robust cathode/electrolyte interface (CEI). As a result, both solid-state Li/Li symmetric cells and LiNi0.6Co0.2Mn0.2O2/Li full cells incorporating the PLSCF electrolyte exhibit significantly improved cycling stability and rate capability. This work enriches inorganic fillers to stabilize electrode/electrolyte interface for high-performance solid-state Li metal batteries.
2026, 37(9): 111529
doi: 10.1016/j.cclet.2025.111529
Abstract:
Zero-dimensional (0D) scintillation materials have demonstrated great potential in X-ray detection and imaging due to their advantages in fabricating flexible screens. Compared with the current lead-halide perovskite-based nanocrystals and quantum dots, copper iodide clusters have gradually attracted attention due to their better air stability, eco-friendliness, and processability performance. Here, we demonstrate large-scale synthesis of an eco-friendly 0D microcrystalline Cu4I6(DABCO–CH3)2 (Cu4I6, DABCO–CH3 = 1-methyl-4-aza-1-azoniabicyclo[2.2.2]octane) scintillator exhibiting crystallization-induced emission enhancement (CIEE). High X-ray absorption efficiency and excellent optical properties endow Cu4I6 microcrystals with high-quality scintillation performance, which displays an ultralow X-ray detection limit of 38.4 nGy/s and a light yield of ~21,700 photons/MeV. Specifically, a microcrystal-based flexible scintillation screen was fabricated for high-resolution static and dynamic X-ray imaging applications, achieving a spatial resolution of 12.3 LP/mm. This study introduces a practical design concept for CIEE-based scintillators and seeks to further investigate their potential applications in X-ray imaging.
Zero-dimensional (0D) scintillation materials have demonstrated great potential in X-ray detection and imaging due to their advantages in fabricating flexible screens. Compared with the current lead-halide perovskite-based nanocrystals and quantum dots, copper iodide clusters have gradually attracted attention due to their better air stability, eco-friendliness, and processability performance. Here, we demonstrate large-scale synthesis of an eco-friendly 0D microcrystalline Cu4I6(DABCO–CH3)2 (Cu4I6, DABCO–CH3 = 1-methyl-4-aza-1-azoniabicyclo[2.2.2]octane) scintillator exhibiting crystallization-induced emission enhancement (CIEE). High X-ray absorption efficiency and excellent optical properties endow Cu4I6 microcrystals with high-quality scintillation performance, which displays an ultralow X-ray detection limit of 38.4 nGy/s and a light yield of ~21,700 photons/MeV. Specifically, a microcrystal-based flexible scintillation screen was fabricated for high-resolution static and dynamic X-ray imaging applications, achieving a spatial resolution of 12.3 LP/mm. This study introduces a practical design concept for CIEE-based scintillators and seeks to further investigate their potential applications in X-ray imaging.
2026, 37(9): 111568
doi: 10.1016/j.cclet.2025.111568
Abstract:
Electron beam (EB) irradiation has gained significant attention in industrial wastewater due to its high efficiency and absence of chemical additives or secondary waste. However, its application remains constrained by relatively high operational costs. To address this limitation, we develop a sustainable advanced oxidation platform by synergistically integrating EB irradiation with a bimetallic catalyst (Cu0.97Co0.03/AC) for enhanced phenol (Ph) degradation. The Cu-Co bimetallic catalyst activated a dual reaction network encompassing both radical (•OH, •O2-) and non-radical (1O2, h+, e-) pathways, enabling effective Ph degradation. Compared to EB irradiation alone, this integrated system achieved 6.92-fold and 41.43-fold enhancements in Ph degradation and total organic carbon (TOC) removal, respectively. Quenching and trapping experiments confirmed 1O2 and •OH as the dominant reactive species. The system demonstrated broad pH adaptability while avoiding sulfate byproduct formation typically associated with 1O2-based processes. Toxicity assessment confirmed substantial reduction in intermediate toxicity. Meanwhile, the catalyst maintained excellent cycling stability under prolonged irradiation. This work presents a novel approach for efficient degradation and mineralization of highly toxic organic pollutants through radical/non-radical pathway coupling enabled by EB-bimetallic synergy.
Electron beam (EB) irradiation has gained significant attention in industrial wastewater due to its high efficiency and absence of chemical additives or secondary waste. However, its application remains constrained by relatively high operational costs. To address this limitation, we develop a sustainable advanced oxidation platform by synergistically integrating EB irradiation with a bimetallic catalyst (Cu0.97Co0.03/AC) for enhanced phenol (Ph) degradation. The Cu-Co bimetallic catalyst activated a dual reaction network encompassing both radical (•OH, •O2-) and non-radical (1O2, h+, e-) pathways, enabling effective Ph degradation. Compared to EB irradiation alone, this integrated system achieved 6.92-fold and 41.43-fold enhancements in Ph degradation and total organic carbon (TOC) removal, respectively. Quenching and trapping experiments confirmed 1O2 and •OH as the dominant reactive species. The system demonstrated broad pH adaptability while avoiding sulfate byproduct formation typically associated with 1O2-based processes. Toxicity assessment confirmed substantial reduction in intermediate toxicity. Meanwhile, the catalyst maintained excellent cycling stability under prolonged irradiation. This work presents a novel approach for efficient degradation and mineralization of highly toxic organic pollutants through radical/non-radical pathway coupling enabled by EB-bimetallic synergy.
2026, 37(9): 111595
doi: 10.1016/j.cclet.2025.111595
Abstract:
The utilization of piezo-photocatalytic technology to achieve the efficient decomposition of antibiotics and stable CO2 reduction (dual-functional catalytic system) represents a cutting-edge approach for concurrently mitigating environmental pollution and the energy crisis. In this work, Ti3C2 MXene quantum dots with high electrical conductivity were uniformly modified on the surface of three-dimensional flower-like MoS2, aiming to realize the piezo-photocatalytic degradation of tetracycline hydrochloride (TC-HCl) coupled with the reduction of CO2 to CO. Remarkably, the degradation rate constant of the optimal Ti3C2 MXene quantum dots/MoS2 sample reached 0.178 min-1, which was 7.7 times higher than that of pure MoS2 under single photocatalysis and 7.1 times higher than that under single piezocatalysis. Meanwhile, the CO yield rates reached 28 µmol g-1 h-1, which was 4.6 times and 6.5 times higher than that of the single catalytic systems based on MoS2, respectively. The introduction of Ti3C2 MXene quantum dots significantly enhanced the current density, charge transfer efficiency, and light absorption capacity, and also effectively suppressed the recombination of electron-hole pairs. This work provides a novel strategy for MoS2-based composites to construct a dual-functional catalytic system via piezo-photocatalytic technology, offering a potential solution to address the concurrent challenges of environmental pollution and the energy crisis.
The utilization of piezo-photocatalytic technology to achieve the efficient decomposition of antibiotics and stable CO2 reduction (dual-functional catalytic system) represents a cutting-edge approach for concurrently mitigating environmental pollution and the energy crisis. In this work, Ti3C2 MXene quantum dots with high electrical conductivity were uniformly modified on the surface of three-dimensional flower-like MoS2, aiming to realize the piezo-photocatalytic degradation of tetracycline hydrochloride (TC-HCl) coupled with the reduction of CO2 to CO. Remarkably, the degradation rate constant of the optimal Ti3C2 MXene quantum dots/MoS2 sample reached 0.178 min-1, which was 7.7 times higher than that of pure MoS2 under single photocatalysis and 7.1 times higher than that under single piezocatalysis. Meanwhile, the CO yield rates reached 28 µmol g-1 h-1, which was 4.6 times and 6.5 times higher than that of the single catalytic systems based on MoS2, respectively. The introduction of Ti3C2 MXene quantum dots significantly enhanced the current density, charge transfer efficiency, and light absorption capacity, and also effectively suppressed the recombination of electron-hole pairs. This work provides a novel strategy for MoS2-based composites to construct a dual-functional catalytic system via piezo-photocatalytic technology, offering a potential solution to address the concurrent challenges of environmental pollution and the energy crisis.
2026, 37(9): 111664
doi: 10.1016/j.cclet.2025.111664
Abstract:
With high fuel flexibility, high energy efficiency, and low carbon emissions, protonic ceramic fuel cells (PCFCs) have been recognized as a promising energy conversion device. However, the sluggish oxygen reduction reaction (ORR) kinetics occurring at the cathodes significantly hinder the further development of PCFCs. Herein, a Yb-doped cathode material based on PrBaCo2O5+δ (PBC) perovskite with a nominal composition of PrBaCo1.95Yb0.05O5+δ (PBCYb0.05) is reported. The PBCYb0.05 is made up of two phases, which are deficient-PrBa1-xCo1.95–0.99xYb0.05–0.1xO5+δ (D-PBCYb0.05) major phase and BaCo0.99Yb0.01O3-δ (BCYO) secondary phase, demonstrating a low area-specific resistance of 0.249 Ω cm2 and commendable electrocatalytic stability at 600 ℃. In comparison to PBC, the PBCYb0.05 exhibits accelerated oxygen transport kinetics and higher oxygen vacancy concentration, confirmed by the analyses of electrical conductivity relaxation and X-ray photoelectron spectroscopy. When implemented as the air electrode in PCFCs, PBCYb0.05 delivers an outstanding peak power density (PPD) of 2.25 W/cm2 at 700 ℃, representing a high enhancement over undoped PBC cells.
With high fuel flexibility, high energy efficiency, and low carbon emissions, protonic ceramic fuel cells (PCFCs) have been recognized as a promising energy conversion device. However, the sluggish oxygen reduction reaction (ORR) kinetics occurring at the cathodes significantly hinder the further development of PCFCs. Herein, a Yb-doped cathode material based on PrBaCo2O5+δ (PBC) perovskite with a nominal composition of PrBaCo1.95Yb0.05O5+δ (PBCYb0.05) is reported. The PBCYb0.05 is made up of two phases, which are deficient-PrBa1-xCo1.95–0.99xYb0.05–0.1xO5+δ (D-PBCYb0.05) major phase and BaCo0.99Yb0.01O3-δ (BCYO) secondary phase, demonstrating a low area-specific resistance of 0.249 Ω cm2 and commendable electrocatalytic stability at 600 ℃. In comparison to PBC, the PBCYb0.05 exhibits accelerated oxygen transport kinetics and higher oxygen vacancy concentration, confirmed by the analyses of electrical conductivity relaxation and X-ray photoelectron spectroscopy. When implemented as the air electrode in PCFCs, PBCYb0.05 delivers an outstanding peak power density (PPD) of 2.25 W/cm2 at 700 ℃, representing a high enhancement over undoped PBC cells.
2026, 37(9): 111866
doi: 10.1016/j.cclet.2025.111866
Abstract:
Considering the urgency of endocrine disrupting chemicals (EDCs) management, a novel 2D MXene/1D Bi5O7I Schottky junction photocatalyst was constructed for the degradation of bisphenol AF (BPAF) by peroxymonosulfate (PMS)-assisted photocatalytic system. Under visible light, the 8-MXene/Bi5O7I/PMS system could degrade 93.4% (0.02984 min-1) of BPAF at 90 min, which was 5.04 and 3.35 times that of Bi5O7I and MXene/Bi5O7I, respectively. This demonstrated the synergistic interaction between photocatalysis and PMS activation, and the ability of MXene to promote the reaction. Density functional theory (DFT) calculations combined with experiments revealed the catalytic reaction mechanism of the system. Additionally, based on Gaussian calculations, the key intermediates of the degradation process were proposed. This study provides a new insight into PMS-assisted photocatalytic systems for effective degradation of organic pollutants.
Considering the urgency of endocrine disrupting chemicals (EDCs) management, a novel 2D MXene/1D Bi5O7I Schottky junction photocatalyst was constructed for the degradation of bisphenol AF (BPAF) by peroxymonosulfate (PMS)-assisted photocatalytic system. Under visible light, the 8-MXene/Bi5O7I/PMS system could degrade 93.4% (0.02984 min-1) of BPAF at 90 min, which was 5.04 and 3.35 times that of Bi5O7I and MXene/Bi5O7I, respectively. This demonstrated the synergistic interaction between photocatalysis and PMS activation, and the ability of MXene to promote the reaction. Density functional theory (DFT) calculations combined with experiments revealed the catalytic reaction mechanism of the system. Additionally, based on Gaussian calculations, the key intermediates of the degradation process were proposed. This study provides a new insight into PMS-assisted photocatalytic systems for effective degradation of organic pollutants.
2026, 37(9): 111889
doi: 10.1016/j.cclet.2025.111889
Abstract:
Latent fingerprints (LFPs) serve as indispensable forensic evidence, yet achieving visualization to Level 3 detail, crucial for conclusive identification, remains highly challenging due to poor contrast, substrate limitations, operational toxicity, and aggregation-caused quenching of classic methods. Here, we present a water-soluble thiazolo[5,4-d]thiazole (TzTz)-based aggregation-induced emission (AIE) luminogen, TPA-TzTz-OH, rationally designed to address these issues. This probe, integrating triphenylamine electron donors, a TzTz π-bridge, and a pyridinium acceptor, enables a distinctive fluorescence "off−on" switch upon visible light (425 nm) excitation, visualizing LFPs within 40 s, completely avoiding organic solvents or post-processing. TPA-TzTz-OH offers broad substrate compatibility, producing high-contrast, high-fidelity fingerprint images on metals, glass, plastics, ceramics, and wood, consistently resolving sweat pores and ridge microstructures (Level 3 features) essential for individualization. Mechanistic studies indicate that restricted intramolecular motion upon specific binding to fingerprint lipids (oleic acid and cholesterol) triggers pronounced AIE enhancement, with electrostatic and hydrogen-bonding interactions enabling specificity. The probe exhibits excellent biocompatibility (>85% cell viability at working concentration), retains efficacy for aged fingerprints (≥10 days), and can be used via immersion or spraying. Comparison with control derivatives confirms the synergistic importance of both the pyridinium charge and hydroxyl group in realizing these unique advantages. This work establishes TPA-TzTz-OH as a promising, sustainable solution for high-resolution forensic visualization, bridging fundamental AIE photophysics and real-world criminalistics while providing a greener and safer technique over conventional methods.
Latent fingerprints (LFPs) serve as indispensable forensic evidence, yet achieving visualization to Level 3 detail, crucial for conclusive identification, remains highly challenging due to poor contrast, substrate limitations, operational toxicity, and aggregation-caused quenching of classic methods. Here, we present a water-soluble thiazolo[5,4-d]thiazole (TzTz)-based aggregation-induced emission (AIE) luminogen, TPA-TzTz-OH, rationally designed to address these issues. This probe, integrating triphenylamine electron donors, a TzTz π-bridge, and a pyridinium acceptor, enables a distinctive fluorescence "off−on" switch upon visible light (425 nm) excitation, visualizing LFPs within 40 s, completely avoiding organic solvents or post-processing. TPA-TzTz-OH offers broad substrate compatibility, producing high-contrast, high-fidelity fingerprint images on metals, glass, plastics, ceramics, and wood, consistently resolving sweat pores and ridge microstructures (Level 3 features) essential for individualization. Mechanistic studies indicate that restricted intramolecular motion upon specific binding to fingerprint lipids (oleic acid and cholesterol) triggers pronounced AIE enhancement, with electrostatic and hydrogen-bonding interactions enabling specificity. The probe exhibits excellent biocompatibility (>85% cell viability at working concentration), retains efficacy for aged fingerprints (≥10 days), and can be used via immersion or spraying. Comparison with control derivatives confirms the synergistic importance of both the pyridinium charge and hydroxyl group in realizing these unique advantages. This work establishes TPA-TzTz-OH as a promising, sustainable solution for high-resolution forensic visualization, bridging fundamental AIE photophysics and real-world criminalistics while providing a greener and safer technique over conventional methods.
2026, 37(9): 111924
doi: 10.1016/j.cclet.2025.111924
Abstract:
Copper (Cu) is essential for life, with its redox cycling (Cu+/Cu2+) underpinning key biological processes. Although significant progress has been made in developing fluorescent probes for Cu+, reliable tools for detecting intracellular Cu2+ remain limited, leaving a critical gap in the bioinorganic chemistry toolkit. To address this need, we developed an activity-based sensing (ABS) strategy for live-cell Cu2+ detection that leverages Cu2+-dependent bioorthogonal conjugation. Specifically, we engineered thiophosphoryl pyridinol/pyrimidinol dyes that undergo Cu2+-mediated activation, enabling covalent labeling of proximal proteins within intracellular Cu2+-enriched microdomains and concomitant turn-on fluorescence. This work not only offers a powerful tool for detecting intracellular Cu2+ fluctuations under exogenous stimuli but also proposes thiophosphorylated pyridinol/pyrimidinol scaffolds as a versatile platform for future intracellular Cu2+ sensing applications.
Copper (Cu) is essential for life, with its redox cycling (Cu+/Cu2+) underpinning key biological processes. Although significant progress has been made in developing fluorescent probes for Cu+, reliable tools for detecting intracellular Cu2+ remain limited, leaving a critical gap in the bioinorganic chemistry toolkit. To address this need, we developed an activity-based sensing (ABS) strategy for live-cell Cu2+ detection that leverages Cu2+-dependent bioorthogonal conjugation. Specifically, we engineered thiophosphoryl pyridinol/pyrimidinol dyes that undergo Cu2+-mediated activation, enabling covalent labeling of proximal proteins within intracellular Cu2+-enriched microdomains and concomitant turn-on fluorescence. This work not only offers a powerful tool for detecting intracellular Cu2+ fluctuations under exogenous stimuli but also proposes thiophosphorylated pyridinol/pyrimidinol scaffolds as a versatile platform for future intracellular Cu2+ sensing applications.
2026, 37(9): 111936
doi: 10.1016/j.cclet.2025.111936
Abstract:
The escalating incidence of breast cancer threatens to women's health, underscoring the urgent need for the development of new therapies with reduced toxicity and increased efficacy. Combination therapy strategy holds promising potential to improve therapeutic outcomes, however, most chemotherapeutic drugs agents are hindered by poor water solubility and non-specific toxicity. The combination of chemotherapy drugs with targeted therapies represents a reliable approach. In this study, we designed a combination regimen utilizing the chemotherapeutic agent doxorubicin (Dox) alongside the anti-angiogenic drug apatinib (AP) for breast cancer treatment. Methoxy poly(ethylene glycol)-disulfide-poly(lactic acid) (PEG-SS-PLA) and cyclo(Arg-Gly-Asp-D-Tyr-Cys) conjugated PEG-PLA (cRGD-PEG-PLA) were prepared to achieve both reductive response and active targeting for co-delivery of drugs. The self-assembled drug-loaded micelles exhibited an average particle size of 61.50 nm. Our findings indicate that AP significantly enhances Dox uptake in breast cancer cells. Cellular and animal experimental results consistently demonstrated that the AP+Dox/cRGD-m effectively promotes apoptosis of breast cancer cells, while markedly inhibiting tumor growth and pulmonary metastasis. Additionally, AP+Dox/cRGD-m is biodegradable and sustainable, exhibiting a favorable safety profile in vivo. This study suggests that AP+Dox/cRGD-m may have potential clinical application in the treatment of breast cancer.
The escalating incidence of breast cancer threatens to women's health, underscoring the urgent need for the development of new therapies with reduced toxicity and increased efficacy. Combination therapy strategy holds promising potential to improve therapeutic outcomes, however, most chemotherapeutic drugs agents are hindered by poor water solubility and non-specific toxicity. The combination of chemotherapy drugs with targeted therapies represents a reliable approach. In this study, we designed a combination regimen utilizing the chemotherapeutic agent doxorubicin (Dox) alongside the anti-angiogenic drug apatinib (AP) for breast cancer treatment. Methoxy poly(ethylene glycol)-disulfide-poly(lactic acid) (PEG-SS-PLA) and cyclo(Arg-Gly-Asp-D-Tyr-Cys) conjugated PEG-PLA (cRGD-PEG-PLA) were prepared to achieve both reductive response and active targeting for co-delivery of drugs. The self-assembled drug-loaded micelles exhibited an average particle size of 61.50 nm. Our findings indicate that AP significantly enhances Dox uptake in breast cancer cells. Cellular and animal experimental results consistently demonstrated that the AP+Dox/cRGD-m effectively promotes apoptosis of breast cancer cells, while markedly inhibiting tumor growth and pulmonary metastasis. Additionally, AP+Dox/cRGD-m is biodegradable and sustainable, exhibiting a favorable safety profile in vivo. This study suggests that AP+Dox/cRGD-m may have potential clinical application in the treatment of breast cancer.
2026, 37(9): 111937
doi: 10.1016/j.cclet.2025.111937
Abstract:
Liver cancer, particularly hepatocellular carcinoma (HCC), is a leading cause of cancer-related mortality worldwide. The therapeutic potential of norcantharidin (NCTD), a small-molecule chemotherapeutic agent, is often limited by its rapid systemic clearance and dose-dependent nephrotoxicity. Here, a novel folic acid (FA)-modified erythrocyte membrane (EM)-coated nanoplatform (FA/EM@PEI-NCTD) was developed to improve tumor targeting, prolong circulation, and mitigate renal toxicity. This nanoplatform preserves CD47 expression, transmitting “don't eat me” signal to evade macrophage uptake. In vitro, FA/EM@PEI-NCTD showed enhanced cytotoxicity against HCC cells and favorable drug release kinetics with low hemolytic activity. In vivo, the system demonstrated superior tumor targeting, growth inhibition, prolonged survival, and reduced nephrotoxicity. Mechanistically, the treatment promoted apoptosis in H22 cells by upregulating Bax and caspase-3 while downregulating Bcl-2. These results highlight FA/EM@PEI-NCTD as a promising strategy for safe and effective targeted HCC therapy.
Liver cancer, particularly hepatocellular carcinoma (HCC), is a leading cause of cancer-related mortality worldwide. The therapeutic potential of norcantharidin (NCTD), a small-molecule chemotherapeutic agent, is often limited by its rapid systemic clearance and dose-dependent nephrotoxicity. Here, a novel folic acid (FA)-modified erythrocyte membrane (EM)-coated nanoplatform (FA/EM@PEI-NCTD) was developed to improve tumor targeting, prolong circulation, and mitigate renal toxicity. This nanoplatform preserves CD47 expression, transmitting “don't eat me” signal to evade macrophage uptake. In vitro, FA/EM@PEI-NCTD showed enhanced cytotoxicity against HCC cells and favorable drug release kinetics with low hemolytic activity. In vivo, the system demonstrated superior tumor targeting, growth inhibition, prolonged survival, and reduced nephrotoxicity. Mechanistically, the treatment promoted apoptosis in H22 cells by upregulating Bax and caspase-3 while downregulating Bcl-2. These results highlight FA/EM@PEI-NCTD as a promising strategy for safe and effective targeted HCC therapy.
2026, 37(9): 111942
doi: 10.1016/j.cclet.2025.111942
Abstract:
Androgenetic alopecia (AGA) is the most common type of hair loss in clinical practice. Currently, the approved clinically used regimens for the treatment of alopecia include topical administration of minoxidil and oral finasteride. However, the two treatment approaches always demonstrate adverse effects and safety concerns. In the study, an aqueous transdermal delivery system (AqEDs) of Cacumen Platycladi essential oil (EO) was developed for the treatment of AGA, using deep eutectic solvent (DES) to solubilize the complex components of EOs. The AqEDs can stabilize EOs and allows transdermal delivery through lipid extraction with keratin conformational changes. AqEDs induced more significant hair regrowth effects in AGA model mice at a lower dosing frequency compared to minoxidil. This study potentially provides a safer and more effective strategy for the treatment of AGA.
Androgenetic alopecia (AGA) is the most common type of hair loss in clinical practice. Currently, the approved clinically used regimens for the treatment of alopecia include topical administration of minoxidil and oral finasteride. However, the two treatment approaches always demonstrate adverse effects and safety concerns. In the study, an aqueous transdermal delivery system (AqEDs) of Cacumen Platycladi essential oil (EO) was developed for the treatment of AGA, using deep eutectic solvent (DES) to solubilize the complex components of EOs. The AqEDs can stabilize EOs and allows transdermal delivery through lipid extraction with keratin conformational changes. AqEDs induced more significant hair regrowth effects in AGA model mice at a lower dosing frequency compared to minoxidil. This study potentially provides a safer and more effective strategy for the treatment of AGA.
2026, 37(9): 111970
doi: 10.1016/j.cclet.2025.111970
Abstract:
The multidrug resistance and robust biofilm-forming capacity of methicillin-resistant Staphylococcus aureus (MRSA) present significant challenges to clinical therapy, underscoring the urgent need for the effective antibacterial strategies. While synergistic approaches combining photodynamic therapy (PDT) and photothermal therapy (PTT) exhibit considerable promise, their efficacy is frequently constrained by limitations in targeted delivery to bacteria and biofilms. This study developed a multifunctional nanoparticle (BDPV) through the conjugation of vancomycin (VAN) with distearoylphosphatidylethanolamine-polyethylene glycol 2000 (DSPE-PEG2000) and the encapsulation of a 4,4-difluoro-4-bora-3a,4a-diaza-s-indacene derivative (BODIPY) possessing both photodynamic and photothermal properties. BDPV employs a dual-targeting mechanism: (1) VAN enables specific targeting of peptidoglycan in the bacterial cell wall; (2) under the conditions of infection microenvironments, BODIPY undergoes protonation, resulting in charge reversal from negative to positive, thereby enhancing electrostatic interaction to bacteria. Upon irradiation with the near-infrared (NIR) laser, BDPV synergistically generates potent photodynamic and photothermal antibacterial effects, which facilitates highly efficient targeting and effective eradication of drug-resistant bacterial infections. Furthermore, BDPV demonstrated remarkable therapeutic efficacy in both deep-tissue infection models (pneumonia) and superficial infection models (skin wounds). This strategy provides a promising new approach for overcoming drug-resistant bacterial infections and treating associated biofilm-related diseases.
The multidrug resistance and robust biofilm-forming capacity of methicillin-resistant Staphylococcus aureus (MRSA) present significant challenges to clinical therapy, underscoring the urgent need for the effective antibacterial strategies. While synergistic approaches combining photodynamic therapy (PDT) and photothermal therapy (PTT) exhibit considerable promise, their efficacy is frequently constrained by limitations in targeted delivery to bacteria and biofilms. This study developed a multifunctional nanoparticle (BDPV) through the conjugation of vancomycin (VAN) with distearoylphosphatidylethanolamine-polyethylene glycol 2000 (DSPE-PEG2000) and the encapsulation of a 4,4-difluoro-4-bora-3a,4a-diaza-s-indacene derivative (BODIPY) possessing both photodynamic and photothermal properties. BDPV employs a dual-targeting mechanism: (1) VAN enables specific targeting of peptidoglycan in the bacterial cell wall; (2) under the conditions of infection microenvironments, BODIPY undergoes protonation, resulting in charge reversal from negative to positive, thereby enhancing electrostatic interaction to bacteria. Upon irradiation with the near-infrared (NIR) laser, BDPV synergistically generates potent photodynamic and photothermal antibacterial effects, which facilitates highly efficient targeting and effective eradication of drug-resistant bacterial infections. Furthermore, BDPV demonstrated remarkable therapeutic efficacy in both deep-tissue infection models (pneumonia) and superficial infection models (skin wounds). This strategy provides a promising new approach for overcoming drug-resistant bacterial infections and treating associated biofilm-related diseases.
2026, 37(9): 111974
doi: 10.1016/j.cclet.2025.111974
Abstract:
Palladium (Pd)-based catalysts are commonly used for ethanol oxidation reaction (EOR) in direct ethanol fuel cells, but their performance is hindered by sluggish kinetics and CO poisoning. Engineering p-d orbital hybridization between p-block metals and Pd can optimize the electronic properties and thus boosting the electrocatalytic activities. Therefore, Pd8Sb3 intermetallic nanodisks (NDs) with an unconventional trigonal phase are synthesized through a simple hydrothermal method, promoting a strong p-d hybridization between Pd and Sb. These Pd8Sb3 NDs exhibit exceptional EOR performance with a mass activity of 4.6 A/mg, approximately six times as high as commercial Pd/C. Density functional theory (DFT) calculations confirm that p-d hybridization optimizes intermediates adsorption and reduces reaction energy barriers. This work provides an effective pathway to fabricate strong p-d orbital hybridization and enhance the catalytic performance of Pd-based catalysts for renewable energy applications.
Palladium (Pd)-based catalysts are commonly used for ethanol oxidation reaction (EOR) in direct ethanol fuel cells, but their performance is hindered by sluggish kinetics and CO poisoning. Engineering p-d orbital hybridization between p-block metals and Pd can optimize the electronic properties and thus boosting the electrocatalytic activities. Therefore, Pd8Sb3 intermetallic nanodisks (NDs) with an unconventional trigonal phase are synthesized through a simple hydrothermal method, promoting a strong p-d hybridization between Pd and Sb. These Pd8Sb3 NDs exhibit exceptional EOR performance with a mass activity of 4.6 A/mg, approximately six times as high as commercial Pd/C. Density functional theory (DFT) calculations confirm that p-d hybridization optimizes intermediates adsorption and reduces reaction energy barriers. This work provides an effective pathway to fabricate strong p-d orbital hybridization and enhance the catalytic performance of Pd-based catalysts for renewable energy applications.
2026, 37(9): 111981
doi: 10.1016/j.cclet.2025.111981
Abstract:
Diabetic wounds are characterized by local oxidative stress, bacterial infection, and persistent inflammation, all of which hinder effective clinical healing. To address these challenges, we developed a glucose/reactive oxygen species (ROS) dual-responsive hydrogel (hyaluronic acid-phenylboronic acid (HA-PBA)/polyvinyl alcohol (PVA)/mangiferin (MF), HPM) composed of HA-PBA and PVA. This hydrogel incorporates MF, a bioactive compound with multiple therapeutic properties, through dynamic boronate ester bonds, enabling stimulus-responsive drug release tailored to the diabetic wound microenvironment, thereby enhancing wound repair. Physicochemical analyses demonstrated that HPM exhibits a favorable porous structure, excellent swelling behavior, appropriate rheological characteristics, and self-healing capability. In vitro studies revealed that HPM effectively scavenges ROS, inhibits bacterial proliferation, attenuates inflammation, and promotes angiogenesis. In a diabetic rat model, HPM significantly accelerated wound closure, as indicated by enhanced epithelial regeneration, increased collagen deposition, improved neovascularization, and suppressed inflammatory. Moreover, biocompatibility evaluations confirmed the excellent biosafety of HPM both in vitro and in vivo. This multifunctional hydrogel dressing, combining glucose and ROS sensitivity with robust therapeutic efficacy and biocompatibility, offers a promising strategy for diabetic wound management.
Diabetic wounds are characterized by local oxidative stress, bacterial infection, and persistent inflammation, all of which hinder effective clinical healing. To address these challenges, we developed a glucose/reactive oxygen species (ROS) dual-responsive hydrogel (hyaluronic acid-phenylboronic acid (HA-PBA)/polyvinyl alcohol (PVA)/mangiferin (MF), HPM) composed of HA-PBA and PVA. This hydrogel incorporates MF, a bioactive compound with multiple therapeutic properties, through dynamic boronate ester bonds, enabling stimulus-responsive drug release tailored to the diabetic wound microenvironment, thereby enhancing wound repair. Physicochemical analyses demonstrated that HPM exhibits a favorable porous structure, excellent swelling behavior, appropriate rheological characteristics, and self-healing capability. In vitro studies revealed that HPM effectively scavenges ROS, inhibits bacterial proliferation, attenuates inflammation, and promotes angiogenesis. In a diabetic rat model, HPM significantly accelerated wound closure, as indicated by enhanced epithelial regeneration, increased collagen deposition, improved neovascularization, and suppressed inflammatory. Moreover, biocompatibility evaluations confirmed the excellent biosafety of HPM both in vitro and in vivo. This multifunctional hydrogel dressing, combining glucose and ROS sensitivity with robust therapeutic efficacy and biocompatibility, offers a promising strategy for diabetic wound management.
2026, 37(9): 111985
doi: 10.1016/j.cclet.2025.111985
Abstract:
Chronic skin wounds with persistent bacterial infections present a formidable clinical challenge, characterized by recurrent infections and delayed healing. These issues stem from incomplete bacterial eradication, a lack of sustained antibacterial ability, and slow tissue repair. We developed a dual-responsive nanocatalytic membrane to address these limitations for advanced infected chronic wound management. This platform integrates MXene/CuO2 bio-heterojunctions (MX/CO bio-HJs) with polydopamine (PDA) and electrospun polycaprolactone (PCL) scaffolds, creating a multifunctional system that synergistically enhances debridement and regeneration. Diverging from traditional dressings, this membrane leverages near-infrared (NIR) light to trigger robust antibacterial action through synergistic photodynamic (PDT) and photothermal (PTT) therapies, ensuring complete sterilization. In the absence of NIR, it autonomously responds to the infection microenvironments (IMEs) by initiating Fenton-like cascades via chemodynamic therapy (CDT) and metal-ion therapy (MIT), sustaining reactive oxygen species (ROS) production and Cu2+ ions release to prevent recurrent infections. Simultaneously, the released Cu2+ ions enhance vascular endothelial growth factor (VEGF) expression, fostering angiogenesis and hastening wound closure, thus reducing infection risks linked to prolonged exposure. In vivo studies demonstrate rapid bacterial elimination, significant remodeling of the wound milieu, and enhanced epithelialization, collagen deposition, and vascularization. This innovative design overcomes the deficiencies of existing modalities, offering a NIR/IMEs dual-responsive approach to managing chronic infected wounds with precision and efficacy.
Chronic skin wounds with persistent bacterial infections present a formidable clinical challenge, characterized by recurrent infections and delayed healing. These issues stem from incomplete bacterial eradication, a lack of sustained antibacterial ability, and slow tissue repair. We developed a dual-responsive nanocatalytic membrane to address these limitations for advanced infected chronic wound management. This platform integrates MXene/CuO2 bio-heterojunctions (MX/CO bio-HJs) with polydopamine (PDA) and electrospun polycaprolactone (PCL) scaffolds, creating a multifunctional system that synergistically enhances debridement and regeneration. Diverging from traditional dressings, this membrane leverages near-infrared (NIR) light to trigger robust antibacterial action through synergistic photodynamic (PDT) and photothermal (PTT) therapies, ensuring complete sterilization. In the absence of NIR, it autonomously responds to the infection microenvironments (IMEs) by initiating Fenton-like cascades via chemodynamic therapy (CDT) and metal-ion therapy (MIT), sustaining reactive oxygen species (ROS) production and Cu2+ ions release to prevent recurrent infections. Simultaneously, the released Cu2+ ions enhance vascular endothelial growth factor (VEGF) expression, fostering angiogenesis and hastening wound closure, thus reducing infection risks linked to prolonged exposure. In vivo studies demonstrate rapid bacterial elimination, significant remodeling of the wound milieu, and enhanced epithelialization, collagen deposition, and vascularization. This innovative design overcomes the deficiencies of existing modalities, offering a NIR/IMEs dual-responsive approach to managing chronic infected wounds with precision and efficacy.
2026, 37(9): 112015
doi: 10.1016/j.cclet.2025.112015
Abstract:
Hyperbranched polymers (HBPs) comprising polyether and polyacrylate segments are effective for enhancing the performance of polyether and polyacrylate blends. However, this approach is limited by difficulties associated with efficient synthetic strategies and structural modifications. Herein, we develop a strategy for synthesizing HBPs through the copolymerization of epoxides and acrylates, wherein glycidyl acrylate (GA), a bifunctional monomer comprising epoxy and acrylate groups, was added as the branching point. The dinuclear Cr-complex-catalyzed copolymerization of epoxides and acrylates occurred in a monomer reactivity-determined manner. By varying the feed ratio of GA, HBPs with various branching degrees were accessed, attaining HBPs with different molecular weights. Furthermore, the obtained HBPs are effective in promoting the mechanical performances of polyether and polyacrylate blends. Morphological characterization revealed that the incorporation of HBPs into blends improved the microphase fusion of immiscible domains within the blend, highlighting their excellent compatibilization performances.
Hyperbranched polymers (HBPs) comprising polyether and polyacrylate segments are effective for enhancing the performance of polyether and polyacrylate blends. However, this approach is limited by difficulties associated with efficient synthetic strategies and structural modifications. Herein, we develop a strategy for synthesizing HBPs through the copolymerization of epoxides and acrylates, wherein glycidyl acrylate (GA), a bifunctional monomer comprising epoxy and acrylate groups, was added as the branching point. The dinuclear Cr-complex-catalyzed copolymerization of epoxides and acrylates occurred in a monomer reactivity-determined manner. By varying the feed ratio of GA, HBPs with various branching degrees were accessed, attaining HBPs with different molecular weights. Furthermore, the obtained HBPs are effective in promoting the mechanical performances of polyether and polyacrylate blends. Morphological characterization revealed that the incorporation of HBPs into blends improved the microphase fusion of immiscible domains within the blend, highlighting their excellent compatibilization performances.
2026, 37(9): 112027
doi: 10.1016/j.cclet.2025.112027
Abstract:
Central nervous system diseases (CNSDs), such as Parkinson's disease (PD) and depression, have attracted considerable attention due to their high morbidity and mortality rates. Neuronal damage in CNSDs is primarily driven by inflammation and oxidative stress induced by activated astrocytes and microglia. Thus, new therapeutic strategies are urgently needed that not only enable effective drug delivery across the blood-brain barrier (BBB), but also specifically target lesions while exerting antioxidant and anti-inflammatory effects on glial cells. To address this challenge, we developed an exosome-liposome hybrid system targeting glial cells co-loaded with fisetin (FIS) and pioglitazone (PIO) (RMP7-EL-FIS-PIO). This hybrid system crosses the BBB through the B2 bradykinin receptor-mediated opening and takes advantage of the homing properties of exosomes to accumulate at the site of brain lesions in murine models of PD and of depression. Through receptor-ligand binding and phagocytosis, the hybrid system targets glial cells to deliver drugs that inhibit their activation, thus protecting neurons. Our study demonstrates the great potential of the developed exosome-liposome hybrid system for the targeted treatment of CNSDs.
Central nervous system diseases (CNSDs), such as Parkinson's disease (PD) and depression, have attracted considerable attention due to their high morbidity and mortality rates. Neuronal damage in CNSDs is primarily driven by inflammation and oxidative stress induced by activated astrocytes and microglia. Thus, new therapeutic strategies are urgently needed that not only enable effective drug delivery across the blood-brain barrier (BBB), but also specifically target lesions while exerting antioxidant and anti-inflammatory effects on glial cells. To address this challenge, we developed an exosome-liposome hybrid system targeting glial cells co-loaded with fisetin (FIS) and pioglitazone (PIO) (RMP7-EL-FIS-PIO). This hybrid system crosses the BBB through the B2 bradykinin receptor-mediated opening and takes advantage of the homing properties of exosomes to accumulate at the site of brain lesions in murine models of PD and of depression. Through receptor-ligand binding and phagocytosis, the hybrid system targets glial cells to deliver drugs that inhibit their activation, thus protecting neurons. Our study demonstrates the great potential of the developed exosome-liposome hybrid system for the targeted treatment of CNSDs.
2026, 37(9): 112028
doi: 10.1016/j.cclet.2025.112028
Abstract:
Given the widespread use of pyriproxyfen (PPF) in public health and agricultural pest management, accurate residue monitoring is critical to ensuring food safety, preserving ecological equilibrium, and protecting human health. While fluorescent sensing techniques represent promising paradigm for PPF detection, existing probes often lack rapid response and high specificity. To address this issue, we present the development of a novel FA1-targeting albumin-based supramolecular probe (DOCD@ALB) for the ratiometric detection of PPF. The strategy design minimizes competitive interference from DS1-binding compounds (e.g., epicatechin), thereby significantly improving its detection accuracy and specificity. When integrated with a smartphone-assisted portable sensing device, the DOCD@ALB system enables on-site PPF quantification in tea matrices, demonstrating its clear translational potential. These findings highlight the pivotal role of binding site selection in modulating the sensing performance of the supramolecular probe system, offering a robust analytical tool with implications for food safety surveillance and environmental protection.
Given the widespread use of pyriproxyfen (PPF) in public health and agricultural pest management, accurate residue monitoring is critical to ensuring food safety, preserving ecological equilibrium, and protecting human health. While fluorescent sensing techniques represent promising paradigm for PPF detection, existing probes often lack rapid response and high specificity. To address this issue, we present the development of a novel FA1-targeting albumin-based supramolecular probe (DOCD@ALB) for the ratiometric detection of PPF. The strategy design minimizes competitive interference from DS1-binding compounds (e.g., epicatechin), thereby significantly improving its detection accuracy and specificity. When integrated with a smartphone-assisted portable sensing device, the DOCD@ALB system enables on-site PPF quantification in tea matrices, demonstrating its clear translational potential. These findings highlight the pivotal role of binding site selection in modulating the sensing performance of the supramolecular probe system, offering a robust analytical tool with implications for food safety surveillance and environmental protection.
2026, 37(9): 112029
doi: 10.1016/j.cclet.2025.112029
Abstract:
Solid additives have emerged as effective tools for morphology regulation in organic photovoltaics (OPVs), yet simultaneous control over donor and acceptor domains remains challenging. Here, we report a dual-functional solid additive, NSA2, designed to optimize vertical phase distribution and suppress energy loss in PM6:Y6 systems. Compared to the control device with a power conversion efficiency (PCE) of 16.28%, NSA2-incorporated devices achieve a PCE of 18.51%, and up to 19.31% using a layer-by-layer structure with co-additive (DIB). Detailed characterization reveals improved π-π stacking, prolonged crystallization, reduced trap-assisted and bimolecular recombination, and enhanced charge transport. Notably, the non-radiative energy loss (ΔE3) is reduced from 0.214 eV to 0.204 eV, contributing to higher open-circuit voltage. The additive also improves device stability and shows broad compatibility, across other acceptor systems (BTP-eC9-based binary device), achieving PCE of 19.68%. This work demonstrates a general and scalable strategy for designing multifunctional solid additives to boost efficiency and stability in high-performance OPVs.
Solid additives have emerged as effective tools for morphology regulation in organic photovoltaics (OPVs), yet simultaneous control over donor and acceptor domains remains challenging. Here, we report a dual-functional solid additive, NSA2, designed to optimize vertical phase distribution and suppress energy loss in PM6:Y6 systems. Compared to the control device with a power conversion efficiency (PCE) of 16.28%, NSA2-incorporated devices achieve a PCE of 18.51%, and up to 19.31% using a layer-by-layer structure with co-additive (DIB). Detailed characterization reveals improved π-π stacking, prolonged crystallization, reduced trap-assisted and bimolecular recombination, and enhanced charge transport. Notably, the non-radiative energy loss (ΔE3) is reduced from 0.214 eV to 0.204 eV, contributing to higher open-circuit voltage. The additive also improves device stability and shows broad compatibility, across other acceptor systems (BTP-eC9-based binary device), achieving PCE of 19.68%. This work demonstrates a general and scalable strategy for designing multifunctional solid additives to boost efficiency and stability in high-performance OPVs.
2026, 37(9): 112031
doi: 10.1016/j.cclet.2025.112031
Abstract:
MicroRNA (miRNA)-based therapeutics hold great promise for the treatment of ocular fundus diseases. However, naked miRNAs exhibit poor stability in vivo, are readily degraded by nucleases in body fluids, and their negative charge hinders efficient uptake by target cells. Therefore, a safe and effective nucleic acid delivery system is essential. In this study, we developed an efficient and safe polycationic nucleic acid carrier by modifying polyethyleneimine (PEI) with p-toluenesulfonyl chloride (i.e., PEI-T3). The introduction of tosyl groups onto PEI enhanced the hydrophobic interactions between polymer and cell membrane, and contributed to the cellular uptake of miRNA. Intravitreal injection of PEI-T3/miRNA complexes caused negligible effects on retinal structure and function and did not induce neurotoxicity. Using microRNA-578 (miR-578) as the therapeutic gene, PEI-T3/miR-578 treatment effectively downregulated the levels of vascular endothelial growth factor A (VEGF-A) and vascular cell adhesion molecule 1 (VCAM-1), suppressed the proliferation, migration, and tube formation of vascular endothelial cells. In a choroidal neovascularization (CNV) model, a single dose of PEI-T3/miR-578 significantly relieved the disease progression and showed an excellent in vivo safety profile. This study provides a valuable reference for the in vivo delivery of miRNAs using polymeric carriers for the treatment of ocular fundus diseases.
MicroRNA (miRNA)-based therapeutics hold great promise for the treatment of ocular fundus diseases. However, naked miRNAs exhibit poor stability in vivo, are readily degraded by nucleases in body fluids, and their negative charge hinders efficient uptake by target cells. Therefore, a safe and effective nucleic acid delivery system is essential. In this study, we developed an efficient and safe polycationic nucleic acid carrier by modifying polyethyleneimine (PEI) with p-toluenesulfonyl chloride (i.e., PEI-T3). The introduction of tosyl groups onto PEI enhanced the hydrophobic interactions between polymer and cell membrane, and contributed to the cellular uptake of miRNA. Intravitreal injection of PEI-T3/miRNA complexes caused negligible effects on retinal structure and function and did not induce neurotoxicity. Using microRNA-578 (miR-578) as the therapeutic gene, PEI-T3/miR-578 treatment effectively downregulated the levels of vascular endothelial growth factor A (VEGF-A) and vascular cell adhesion molecule 1 (VCAM-1), suppressed the proliferation, migration, and tube formation of vascular endothelial cells. In a choroidal neovascularization (CNV) model, a single dose of PEI-T3/miR-578 significantly relieved the disease progression and showed an excellent in vivo safety profile. This study provides a valuable reference for the in vivo delivery of miRNAs using polymeric carriers for the treatment of ocular fundus diseases.
2026, 37(9): 112063
doi: 10.1016/j.cclet.2025.112063
Abstract:
Inducing ferroptosis is a promising strategy for oral cancer therapy, but existing inducers often lack selectivity and possess poor drug-like properties. Our preliminary work identified 26a as a potent ferroptosis inducer targeting glutathione peroxidase 4 (GPX4), yet its selectivity and safety needed improvement. In this study, we designed a series of hybrid molecules by integrating the privileged fragment of 26a with the known GPX4 inhibitor ML210. Subsequent structural modifications led to the discovery of XW19, a novel structural scaffold exhibiting GPX4 inhibitory activity. XW19 demonstrated enhanced ferroptosis-inducing potency and highly selectivity (selectivity index (SI) = 1200) as well as inhibitory effects against oral cancer (half maximal inhibitory concentration (IC50) values ranging from 0.71 µmol/L to 2.39 µmol/L). Cellular thermal shift assay (CETSA) confirmed the strong binding affinity of XW19 with GPX4. Notably, XW19 exhibited significant tumor suppression and an improved safety profile in a nude mouse model bearing Cal27 ectopic xenografts, positioning XW19 as a promising therapeutic candidate for oral cancer treatment.
Inducing ferroptosis is a promising strategy for oral cancer therapy, but existing inducers often lack selectivity and possess poor drug-like properties. Our preliminary work identified 26a as a potent ferroptosis inducer targeting glutathione peroxidase 4 (GPX4), yet its selectivity and safety needed improvement. In this study, we designed a series of hybrid molecules by integrating the privileged fragment of 26a with the known GPX4 inhibitor ML210. Subsequent structural modifications led to the discovery of XW19, a novel structural scaffold exhibiting GPX4 inhibitory activity. XW19 demonstrated enhanced ferroptosis-inducing potency and highly selectivity (selectivity index (SI) = 1200) as well as inhibitory effects against oral cancer (half maximal inhibitory concentration (IC50) values ranging from 0.71 µmol/L to 2.39 µmol/L). Cellular thermal shift assay (CETSA) confirmed the strong binding affinity of XW19 with GPX4. Notably, XW19 exhibited significant tumor suppression and an improved safety profile in a nude mouse model bearing Cal27 ectopic xenografts, positioning XW19 as a promising therapeutic candidate for oral cancer treatment.
2026, 37(9): 112069
doi: 10.1016/j.cclet.2025.112069
Abstract:
Bioassay- and molecular network-guided isolation of the extract from Hypericum monogynum led to the identification of five polycyclic polyprenylated acylphloroglucinol (PPAP) derivatives, including a previously unreported bis-seco compound, hypermonane A (HMA, 1). HMA possesses a unique 3/6-5/6/5 pentacyclic scaffold, characterized by C-1/C-2 and C-2/C-3 bond cleavage. In addition to HMA, four structurally related biosynthetic analogs (2–5) were also obtained. Its structure was elucidated using computer-assisted structure elucidation (CASE) software and gauge-independent atomic orbital (GIAO)-based nuclear magnetic resonance (NMR) calculations. The absolute configuration of 1 was determined through comparison of experimental and calculated electronic circular dichroism (ECD) spectra. Biological investigations revealed that HMA potently inhibited aortic valve calcification by simultaneously suppressing osteogenic differentiation (runt-related transcription factor 2/alkaline phosphatase, RUNX2/ALP) and extracellular matrix remodeling (collagen type Ⅰ alpha 1 chain/a disintegrin and metalloproteinase with thrombospondin motif 4, COL1A1/ADAMTS4). Moreover, in a murine model of calcific aortic valve disease (CAVD), HMA significantly attenuated pathological aortic valve calcification. These findings highlight HMA as a promising lead compound for the development of anti-CAVD therapeutics.
Bioassay- and molecular network-guided isolation of the extract from Hypericum monogynum led to the identification of five polycyclic polyprenylated acylphloroglucinol (PPAP) derivatives, including a previously unreported bis-seco compound, hypermonane A (HMA, 1). HMA possesses a unique 3/6-5/6/5 pentacyclic scaffold, characterized by C-1/C-2 and C-2/C-3 bond cleavage. In addition to HMA, four structurally related biosynthetic analogs (2–5) were also obtained. Its structure was elucidated using computer-assisted structure elucidation (CASE) software and gauge-independent atomic orbital (GIAO)-based nuclear magnetic resonance (NMR) calculations. The absolute configuration of 1 was determined through comparison of experimental and calculated electronic circular dichroism (ECD) spectra. Biological investigations revealed that HMA potently inhibited aortic valve calcification by simultaneously suppressing osteogenic differentiation (runt-related transcription factor 2/alkaline phosphatase, RUNX2/ALP) and extracellular matrix remodeling (collagen type Ⅰ alpha 1 chain/a disintegrin and metalloproteinase with thrombospondin motif 4, COL1A1/ADAMTS4). Moreover, in a murine model of calcific aortic valve disease (CAVD), HMA significantly attenuated pathological aortic valve calcification. These findings highlight HMA as a promising lead compound for the development of anti-CAVD therapeutics.
2026, 37(9): 112071
doi: 10.1016/j.cclet.2025.112071
Abstract:
Microneedles (MNs) represent a rapidly evolving transdermal drug delivery method, with ongoing development efforts focused on overcoming challenges such as limited drug loading and pore occlusion. Herein, we report dissolvable MNs vaccine with excellent drug loading as well as other positive features that make it an ideal delivery carrier in tumor immunotherapy. This study employs a biodegradable polydopamine-based nano-delivery system to co-encapsulate both Toll-like receptor 7/8 agonist resiquimod (R848) and ovalbumin (OVA) antigens, which are subsequently incorporated into MN patches to achieve synergistic photothermal-immunotherapeutic effects. The MN vaccine targets tumor sites via transdermal administration, exhibiting significant therapeutic efficacy by enabling deep tissue drug release and maintaining prolonged therapeutic levels for at least 3 days. The MN tips are rapidly degraded under photothermal action to release R848 and OVA, can effectively polarizes the tumor-associated macrophages to M1-type macrophages and activate dendritic cells to enhance immune response in vivo, thereby, the MN vaccines have shown excellent efficacy and good safety, resulting in a sufficient and persistent anti-tumor cellular immune response with potent tumor immunotherapeutic efficacy. In brief, this study demonstrates that MN administration successfully delivers polydopamine-based nanotherapeutics to tumor sites and validates their anti-tumor efficacy.
Microneedles (MNs) represent a rapidly evolving transdermal drug delivery method, with ongoing development efforts focused on overcoming challenges such as limited drug loading and pore occlusion. Herein, we report dissolvable MNs vaccine with excellent drug loading as well as other positive features that make it an ideal delivery carrier in tumor immunotherapy. This study employs a biodegradable polydopamine-based nano-delivery system to co-encapsulate both Toll-like receptor 7/8 agonist resiquimod (R848) and ovalbumin (OVA) antigens, which are subsequently incorporated into MN patches to achieve synergistic photothermal-immunotherapeutic effects. The MN vaccine targets tumor sites via transdermal administration, exhibiting significant therapeutic efficacy by enabling deep tissue drug release and maintaining prolonged therapeutic levels for at least 3 days. The MN tips are rapidly degraded under photothermal action to release R848 and OVA, can effectively polarizes the tumor-associated macrophages to M1-type macrophages and activate dendritic cells to enhance immune response in vivo, thereby, the MN vaccines have shown excellent efficacy and good safety, resulting in a sufficient and persistent anti-tumor cellular immune response with potent tumor immunotherapeutic efficacy. In brief, this study demonstrates that MN administration successfully delivers polydopamine-based nanotherapeutics to tumor sites and validates their anti-tumor efficacy.
2026, 37(9): 112072
doi: 10.1016/j.cclet.2025.112072
Abstract:
Natural material-based hydrogels have emerged as ideal candidates for serving as infected wound dressings relying on the extracellular matrix-like microstructure, biocompatibility and the supplying of the wet healing microenvironment. Nevertheless, these hydrogels suffer from limitations including the weak mechanical property, poor water retention ability and inadequate antibacterial property. Herein, we develop a stratum corneum-inspired all-natural-based biogel dressing by directly incorporating natural moisturizing factor (NMF) into gelatin/chitosan quaternary ammonium salt (QCS) hydrogels without necessitating any chemical modification. The sodium pyrrolidone carboxylic acid (PCA-Na, an NMF compound) equipping carboxyl groups forms the ionic crosslink with gelatin containing protonated amino groups and QCS involving quaternary ammonium groups by electrostatic interaction, leading to a significant melioration in the mechanical strength of the biogel. The highly hydrophilic PCA-Na contributes to form additional hydrogen bonds and heighten resistance to dehydration of the biogel, mimicking the role of NMF in the stratum corneum. The excellent broad-spectrum antibacterial property, temperature-controlled reversible fluid-gel transition property and complete degradability are also gathered. A Staphylococcus aureus-infected full-thickness wound repair experiment manifests that our biogel effectively promotes infected wound healing by inhibiting inflammatory factors, facilitating formation of the granulation tissue and angiogenesis. This work paves a valuable way for designing multifunctional natural material-based hydrogel dressings.
Natural material-based hydrogels have emerged as ideal candidates for serving as infected wound dressings relying on the extracellular matrix-like microstructure, biocompatibility and the supplying of the wet healing microenvironment. Nevertheless, these hydrogels suffer from limitations including the weak mechanical property, poor water retention ability and inadequate antibacterial property. Herein, we develop a stratum corneum-inspired all-natural-based biogel dressing by directly incorporating natural moisturizing factor (NMF) into gelatin/chitosan quaternary ammonium salt (QCS) hydrogels without necessitating any chemical modification. The sodium pyrrolidone carboxylic acid (PCA-Na, an NMF compound) equipping carboxyl groups forms the ionic crosslink with gelatin containing protonated amino groups and QCS involving quaternary ammonium groups by electrostatic interaction, leading to a significant melioration in the mechanical strength of the biogel. The highly hydrophilic PCA-Na contributes to form additional hydrogen bonds and heighten resistance to dehydration of the biogel, mimicking the role of NMF in the stratum corneum. The excellent broad-spectrum antibacterial property, temperature-controlled reversible fluid-gel transition property and complete degradability are also gathered. A Staphylococcus aureus-infected full-thickness wound repair experiment manifests that our biogel effectively promotes infected wound healing by inhibiting inflammatory factors, facilitating formation of the granulation tissue and angiogenesis. This work paves a valuable way for designing multifunctional natural material-based hydrogel dressings.
2026, 37(9): 112125
doi: 10.1016/j.cclet.2025.112125
Abstract:
Nanozymes have demonstrated significant potential as robust enzyme-mimicking catalysts due to their high stability, low cost and easy preparation. However, achieving precise enantioselective control of nanozymes remains a significant challenge. In this study, the supramolecular chiral nanozymes were engineered by integrating supramolecular chiral polyaniline (P/M-PANI) scaffolds with platinum-nickel nanoparticles (Pt-Nix NPs). The resulting P/M-PANI@Pt-Nix nanozymes exhibited high catalytic activity toward the oxidation of 3,4-dihydroxy-S/R-phenylalanine (S/R-DOPA). Moreover, systematic modulation of the Pt/Ni atomic ratio in Pt-Nix NPs enabled precise regulation of interfacial interactions and chiral transfer effects, thereby optimizing enantioselectivity. Density functional theory (DFT) calculations further revealed that the distinct adsorption energies of DOPA and its oxidation products on Pt-Nix surfaces directly correlated with the observed catalytic efficiency trends. This work demonstrated that compositional tuning of catalytic centers is an effective strategy for manipulating both catalytic efficiency and enantioselectivity, providing valuable insights for the rational design of smart supramolecular chiral nanozymes.
Nanozymes have demonstrated significant potential as robust enzyme-mimicking catalysts due to their high stability, low cost and easy preparation. However, achieving precise enantioselective control of nanozymes remains a significant challenge. In this study, the supramolecular chiral nanozymes were engineered by integrating supramolecular chiral polyaniline (P/M-PANI) scaffolds with platinum-nickel nanoparticles (Pt-Nix NPs). The resulting P/M-PANI@Pt-Nix nanozymes exhibited high catalytic activity toward the oxidation of 3,4-dihydroxy-S/R-phenylalanine (S/R-DOPA). Moreover, systematic modulation of the Pt/Ni atomic ratio in Pt-Nix NPs enabled precise regulation of interfacial interactions and chiral transfer effects, thereby optimizing enantioselectivity. Density functional theory (DFT) calculations further revealed that the distinct adsorption energies of DOPA and its oxidation products on Pt-Nix surfaces directly correlated with the observed catalytic efficiency trends. This work demonstrated that compositional tuning of catalytic centers is an effective strategy for manipulating both catalytic efficiency and enantioselectivity, providing valuable insights for the rational design of smart supramolecular chiral nanozymes.
2026, 37(9): 112126
doi: 10.1016/j.cclet.2025.112126
Abstract:
The construction of lanthanide nanoclusters that are stable in aqueous solution is challenging, which has led to a sluggish application in the field of bioimaging. Herein, a chelating ligand protection strategy was used to construct nonanuclear lanthanide clusters (Ln9, Ln = Eu, Dy, and Gd) that is stable in aqueous solution. The first fluorescence imaging performance of lanthanide clusters targeting mitochondrial organelles was achieved, with colocalization coefficients of up to 0.96 (MCF-7) and 0.93 (MDA-MB-231) with commercial mitochondrial dyes, respectively. Eu9 can be rapidly taken up by zebrafish and shows excellent fluorescence imaging results, demonstrating its excellent in vivo imaging performance. In addition, the longitudinal and transverse relaxation rates r1 and r2 of Gd9 with highly aggregated Gd(Ⅲ) ions are 39.42 and 50.58 mmol L−1 s−1, respectively, showing great application potential as a new and efficient T1-weighted nanocluster-based magnetic resonance imaging contrast agents.
The construction of lanthanide nanoclusters that are stable in aqueous solution is challenging, which has led to a sluggish application in the field of bioimaging. Herein, a chelating ligand protection strategy was used to construct nonanuclear lanthanide clusters (Ln9, Ln = Eu, Dy, and Gd) that is stable in aqueous solution. The first fluorescence imaging performance of lanthanide clusters targeting mitochondrial organelles was achieved, with colocalization coefficients of up to 0.96 (MCF-7) and 0.93 (MDA-MB-231) with commercial mitochondrial dyes, respectively. Eu9 can be rapidly taken up by zebrafish and shows excellent fluorescence imaging results, demonstrating its excellent in vivo imaging performance. In addition, the longitudinal and transverse relaxation rates r1 and r2 of Gd9 with highly aggregated Gd(Ⅲ) ions are 39.42 and 50.58 mmol L−1 s−1, respectively, showing great application potential as a new and efficient T1-weighted nanocluster-based magnetic resonance imaging contrast agents.
2026, 37(9): 112133
doi: 10.1016/j.cclet.2025.112133
Abstract:
The meta-selective trifluoromethylation of pyridines has remained a significant challenge due to the inherent electronic constraints of the aromatic system. This study developed a novel dearomatization-rearomatization strategy based on 1,4-dihydropyridinephosphonate intermediates, which underwent copper-catalyzed regioselective C–CF3 bond formation with Togni Ⅱ reagent followed by DABCO-promoted rearomatization, achieving highly regioselective meta-C-H trifluoromethylation of pyridine derivatives. This approach accommodated mostly meta-substituted pyridine substrates and enabled late-stage meta-C-H trifluoromethylation of pharmaceutical molecules containing pyridine motifs.
The meta-selective trifluoromethylation of pyridines has remained a significant challenge due to the inherent electronic constraints of the aromatic system. This study developed a novel dearomatization-rearomatization strategy based on 1,4-dihydropyridinephosphonate intermediates, which underwent copper-catalyzed regioselective C–CF3 bond formation with Togni Ⅱ reagent followed by DABCO-promoted rearomatization, achieving highly regioselective meta-C-H trifluoromethylation of pyridine derivatives. This approach accommodated mostly meta-substituted pyridine substrates and enabled late-stage meta-C-H trifluoromethylation of pharmaceutical molecules containing pyridine motifs.
2026, 37(9): 112157
doi: 10.1016/j.cclet.2025.112157
Abstract:
Inherently chiral calix[4]arenes (ICCs) represent a unique class of chiral macrocyclic arenes, which hold significant potentials in chiral recognition, sensing, and asymmetric catalysis. However, accessing these distinct chiral molecules poses notable challenges, with their catalytic enantioselective synthesis being largely underdeveloped. Herein, we report an efficient enantioselective synthesis of ICCs using an asymmetric C-H brominative desymmetrization strategy. Utilizing the chiral phosphoric acid-catalyzed asymmetric electrophilic aromatic ortho-bromination reaction of phenol, we successfully broke the symmetry of prochiral calix[4]arenes, which resulted in the formation of various 1,3-bis-phenyl rings-substituted ICCs with good yields and high enantioselectivities. Moreover, the asymmetric di-bromination of bis-phenol-containing prochiral calix[4]arenes was demonstrated, yielding ICCs featuring three or even four rings displaying various modifications with high enantioselectivity. Leveraging the versatility of the introduced bromide handle and the phenolic hydroxyl group in the ICC products, a range of derivatizations were performed to produce diverse ICC derivatives, one of which exhibited notable chiroptical properties, highlighting the significance of this method.
Inherently chiral calix[4]arenes (ICCs) represent a unique class of chiral macrocyclic arenes, which hold significant potentials in chiral recognition, sensing, and asymmetric catalysis. However, accessing these distinct chiral molecules poses notable challenges, with their catalytic enantioselective synthesis being largely underdeveloped. Herein, we report an efficient enantioselective synthesis of ICCs using an asymmetric C-H brominative desymmetrization strategy. Utilizing the chiral phosphoric acid-catalyzed asymmetric electrophilic aromatic ortho-bromination reaction of phenol, we successfully broke the symmetry of prochiral calix[4]arenes, which resulted in the formation of various 1,3-bis-phenyl rings-substituted ICCs with good yields and high enantioselectivities. Moreover, the asymmetric di-bromination of bis-phenol-containing prochiral calix[4]arenes was demonstrated, yielding ICCs featuring three or even four rings displaying various modifications with high enantioselectivity. Leveraging the versatility of the introduced bromide handle and the phenolic hydroxyl group in the ICC products, a range of derivatizations were performed to produce diverse ICC derivatives, one of which exhibited notable chiroptical properties, highlighting the significance of this method.
2026, 37(9): 112189
doi: 10.1016/j.cclet.2025.112189
Abstract:
The variable oxidation states of nickel catalysts play an essential yet elusive role in reductive coupling reactions, wherein the rapid conversion of nickel species with different oxidation states into NiⅠ has been recognized as a crucial factor in controlling the catalytic turnover and inhibiting side reactions. Beyond the popular strategies for reductive (re)generation of NiⅠ species, spontaneous comproportionation of Ni0 and NiⅡ species can form NiⅠ during catalysis, which is an approach holding great promises yet still relatively underexplored in catalysis. Herein, we transform the intermolecular comproportionation into an entropically more favorable intramolecular pathway by taking advantage of a tetradentate nitrogen ligand (dppn), which effectively brings two catalytic Ni centers in close proximity. This strategy enables ready generation of catalytically active NiⅠ species for reductive diarylation of dienes with aryl iodides using Mn as the terminal reductant. Mechanistic studies reveal that the dppn ligand facilitates the assembly of a dinickel complex, where one nickel acts as the catalytic site for oxidative addition and coupling while the other nickel functions as an electron reservoir. The intramolecular comproportionation pathway establishes a robust strategy for accessing the often fleeting and elusive NiⅠ intermediates critical in forging C–C bonds in the reductive coupling reactions.
The variable oxidation states of nickel catalysts play an essential yet elusive role in reductive coupling reactions, wherein the rapid conversion of nickel species with different oxidation states into NiⅠ has been recognized as a crucial factor in controlling the catalytic turnover and inhibiting side reactions. Beyond the popular strategies for reductive (re)generation of NiⅠ species, spontaneous comproportionation of Ni0 and NiⅡ species can form NiⅠ during catalysis, which is an approach holding great promises yet still relatively underexplored in catalysis. Herein, we transform the intermolecular comproportionation into an entropically more favorable intramolecular pathway by taking advantage of a tetradentate nitrogen ligand (dppn), which effectively brings two catalytic Ni centers in close proximity. This strategy enables ready generation of catalytically active NiⅠ species for reductive diarylation of dienes with aryl iodides using Mn as the terminal reductant. Mechanistic studies reveal that the dppn ligand facilitates the assembly of a dinickel complex, where one nickel acts as the catalytic site for oxidative addition and coupling while the other nickel functions as an electron reservoir. The intramolecular comproportionation pathway establishes a robust strategy for accessing the often fleeting and elusive NiⅠ intermediates critical in forging C–C bonds in the reductive coupling reactions.
2026, 37(9): 112190
doi: 10.1016/j.cclet.2025.112190
Abstract:
A three-step cascade artificial light-harvesting system was constructed by the supramolecular assembly of cation-pillar[5]arene (CP5), tetraphenylethene-sulfonate (TPESF), 4,7-di(2-thienyl)-2,1,3-benzothiadiazole (DBT), sulforhodamine 101 (SR101) and chlorin e6 (Ce6). Inspired by the aggregate state in nanoparticles, CP5-TPESF nanoparticles emitted significant blue fluorescence as FRET donors because of TPESF's AIE effect. Due to the donor emission overlapping the acceptors' absorption, a three-step sequential energy transfer process was successfully constructed in CP5-TPESF-DBT-SR101-Ce6 nanoparticles, which achieved the significant energy transfer efficiency of 87% and antenna effect of 30.8. Benefitting to three-step cascade light-harvesting process and energy transfer to Ce6, Ce6* was excited to release 1O2 in CP5-TPESF-DBT-SR101-Ce6 nanoparticles, which was used as efficient photooxidation catalyst to realize the photooxidation reaction of 4-(methylthio)toluene to 4-(methylsulfinyl)toluene. Notably, the photooxidation yield of CP5-TPESF-DBT-SR101-Ce6 LHS was significantly improved to 89%, suggesting potential in converting solar energy to chemical energy storage.
A three-step cascade artificial light-harvesting system was constructed by the supramolecular assembly of cation-pillar[5]arene (CP5), tetraphenylethene-sulfonate (TPESF), 4,7-di(2-thienyl)-2,1,3-benzothiadiazole (DBT), sulforhodamine 101 (SR101) and chlorin e6 (Ce6). Inspired by the aggregate state in nanoparticles, CP5-TPESF nanoparticles emitted significant blue fluorescence as FRET donors because of TPESF's AIE effect. Due to the donor emission overlapping the acceptors' absorption, a three-step sequential energy transfer process was successfully constructed in CP5-TPESF-DBT-SR101-Ce6 nanoparticles, which achieved the significant energy transfer efficiency of 87% and antenna effect of 30.8. Benefitting to three-step cascade light-harvesting process and energy transfer to Ce6, Ce6* was excited to release 1O2 in CP5-TPESF-DBT-SR101-Ce6 nanoparticles, which was used as efficient photooxidation catalyst to realize the photooxidation reaction of 4-(methylthio)toluene to 4-(methylsulfinyl)toluene. Notably, the photooxidation yield of CP5-TPESF-DBT-SR101-Ce6 LHS was significantly improved to 89%, suggesting potential in converting solar energy to chemical energy storage.
2026, 37(9): 112198
doi: 10.1016/j.cclet.2025.112198
Abstract:
Selective targeting to the subcellular organelle of cancer cells could provide a novel method to realize precise in situ self-assembly for enhanced therapeutic efficiency. Herein, a series of cationic compounds have been synthesized to investigate their subcellular targeting abilities, we found the amino group functionalized planar cationic molecules could selectively locate in the mitochondria of cancer cells (Pearson's coefficient > 0.9), while in the lysosomes of normal cells (Pearson's coefficient > 0.9). Moreover, due to the intermolecular hydrogen bond, the TPE derivative (TPE-NH2) was selected to investigate the in situ self-assembly behavior with negatively charged molecules in the mitochondria of MB49 cancer cells, which could impair the mitochondrial membrane, leading to the elevated reactive oxygen species (ROS), downregulating glutathione peroxidase 4 (GPX4) protein, and finally resulting in LPO for ferroptosis. Moreover, the aggregation-enhanced ROS generation ability of TPE-NH2 made it an ideal candidate for PDT. Under the white light irradiation, the synergetic ferroptosis could be realized to suppress the cancer cell proliferation. Finally, this in situ self-assembly for synergetic therapy would also be realized in vivo to suppress the tumor growth.
Selective targeting to the subcellular organelle of cancer cells could provide a novel method to realize precise in situ self-assembly for enhanced therapeutic efficiency. Herein, a series of cationic compounds have been synthesized to investigate their subcellular targeting abilities, we found the amino group functionalized planar cationic molecules could selectively locate in the mitochondria of cancer cells (Pearson's coefficient > 0.9), while in the lysosomes of normal cells (Pearson's coefficient > 0.9). Moreover, due to the intermolecular hydrogen bond, the TPE derivative (TPE-NH2) was selected to investigate the in situ self-assembly behavior with negatively charged molecules in the mitochondria of MB49 cancer cells, which could impair the mitochondrial membrane, leading to the elevated reactive oxygen species (ROS), downregulating glutathione peroxidase 4 (GPX4) protein, and finally resulting in LPO for ferroptosis. Moreover, the aggregation-enhanced ROS generation ability of TPE-NH2 made it an ideal candidate for PDT. Under the white light irradiation, the synergetic ferroptosis could be realized to suppress the cancer cell proliferation. Finally, this in situ self-assembly for synergetic therapy would also be realized in vivo to suppress the tumor growth.
2026, 37(9): 112199
doi: 10.1016/j.cclet.2025.112199
Abstract:
Cycloparaphenylenes (CPPs) and related carbon nanohoops have garnered significant research interest owing to their unique optoelectronic properties, charge transport characteristics, and host-guest chemistry. Nevertheless, the development of heteroatom-doped carbon nanorings, particularly nitrogen-doped (N-doped) systems, remains limited, and systematic investigations of their host-guest interactions are still scarce. In this work, we present the synthesis of a series of size-controlled aza[10]CPP derivatives designed as optimal hosts for fullerene C60 encapsulation. The acid-responsive optical properties of these N-doped nanorings were thoroughly examined through absorption and fluorescence spectroscopy. Furthermore, we experimentally evaluated and theoretically analyzed the variations in their binding affinities toward C60, elucidating key structural factors that govern supramolecular complexation, including π-π stacking interactions, geometric adaptability, and charge distribution. These findings would provide new insights for advancing strained nanohoop systems in supramolecular chemistry and organic electronic applications.
Cycloparaphenylenes (CPPs) and related carbon nanohoops have garnered significant research interest owing to their unique optoelectronic properties, charge transport characteristics, and host-guest chemistry. Nevertheless, the development of heteroatom-doped carbon nanorings, particularly nitrogen-doped (N-doped) systems, remains limited, and systematic investigations of their host-guest interactions are still scarce. In this work, we present the synthesis of a series of size-controlled aza[10]CPP derivatives designed as optimal hosts for fullerene C60 encapsulation. The acid-responsive optical properties of these N-doped nanorings were thoroughly examined through absorption and fluorescence spectroscopy. Furthermore, we experimentally evaluated and theoretically analyzed the variations in their binding affinities toward C60, elucidating key structural factors that govern supramolecular complexation, including π-π stacking interactions, geometric adaptability, and charge distribution. These findings would provide new insights for advancing strained nanohoop systems in supramolecular chemistry and organic electronic applications.
2026, 37(9): 112200
doi: 10.1016/j.cclet.2025.112200
Abstract:
Electrosynthesis has emerged as a powerful and sustainable strategy in organic chemistry, with growing applications in carbohydrate synthesis. Herein, we report an electrochemical method for the regio- and stereo-selective O-glycosylation of exo-glycals with a wide range of substrates under mild conditions. This approach employs simple setup in an undivided cell with KOTf as electrolyte, facilitating the efficient synthesis of bioactive O-glycosides in good yields and with exclusive α-selectivity. The reaction exhibits broad substrate compatibility, accommodating both sugar- and non-sugar-based acceptors, including complex natural products and pharmaceuticals. Furthermore, gram-scale reactions proceed without loss of efficiency or stereocontrol, underscoring the practicality of this method. Mechanistic studies suggest a radical cation-based pathway. This strategy provides a robust and scalable platform for O-glycosides synthesis.
Electrosynthesis has emerged as a powerful and sustainable strategy in organic chemistry, with growing applications in carbohydrate synthesis. Herein, we report an electrochemical method for the regio- and stereo-selective O-glycosylation of exo-glycals with a wide range of substrates under mild conditions. This approach employs simple setup in an undivided cell with KOTf as electrolyte, facilitating the efficient synthesis of bioactive O-glycosides in good yields and with exclusive α-selectivity. The reaction exhibits broad substrate compatibility, accommodating both sugar- and non-sugar-based acceptors, including complex natural products and pharmaceuticals. Furthermore, gram-scale reactions proceed without loss of efficiency or stereocontrol, underscoring the practicality of this method. Mechanistic studies suggest a radical cation-based pathway. This strategy provides a robust and scalable platform for O-glycosides synthesis.
2026, 37(9): 112201
doi: 10.1016/j.cclet.2025.112201
Abstract:
Skeletal transformations of heteroaromatic compounds via endocyclic bond cleavage have emerged as powerful tools in modern organic synthesis. Nonetheless, selective cleavage of the C2−N1 bond in indoles without the assistance of metal reagents or additives remains highly challenging, owing to the strong aromatic stabilization and intrinsic bond strength of the indole framework. Herein, we present a distinctive dimerization of C3-substituted indolyl vinyl isonitriles that proceeds through a sequential "head-to-head" cross-coupling, pyridannulation, and C2−N1 bond cleavage cascade. This transformation not only disrupts the indole core but also forges a new pyridine ring, thereby providing a metal-free and efficient route to highly functionalized 1-(2-pyridyl)-β-carbolines. Notably, an oxidative aromatic dimerization of C3- and C2-substituted heteroaryl vinyl isonitriles was developed, providing a modular route to bis-β-carbolines, bis-γ-carbolines, and their chalcogen analogues.
Skeletal transformations of heteroaromatic compounds via endocyclic bond cleavage have emerged as powerful tools in modern organic synthesis. Nonetheless, selective cleavage of the C2−N1 bond in indoles without the assistance of metal reagents or additives remains highly challenging, owing to the strong aromatic stabilization and intrinsic bond strength of the indole framework. Herein, we present a distinctive dimerization of C3-substituted indolyl vinyl isonitriles that proceeds through a sequential "head-to-head" cross-coupling, pyridannulation, and C2−N1 bond cleavage cascade. This transformation not only disrupts the indole core but also forges a new pyridine ring, thereby providing a metal-free and efficient route to highly functionalized 1-(2-pyridyl)-β-carbolines. Notably, an oxidative aromatic dimerization of C3- and C2-substituted heteroaryl vinyl isonitriles was developed, providing a modular route to bis-β-carbolines, bis-γ-carbolines, and their chalcogen analogues.
2026, 37(9): 112221
doi: 10.1016/j.cclet.2025.112221
Abstract:
Constructing high-contrast mechanochromic luminescent (MCL) materials with a wide range of emission color variations remains challenging. Herein, a host-guest strategy is proposed to optimize molecular MCL behavior. Two pyridinium-functionalized carbazole derivatives only exhibit a slight red-shifted fluorescence under mechanical stimulation. By forming host-guest complexes with cucurbit[n]urils (CB[n]s, n = 8 or 10), the complexes demonstrate more significant fluorescence wavelength changes after grinding. Mechanistic studies reveal that the crystallization and CB[n]’s confinement effect, synergistically induce more twisted molecular conformations and facilitate the planarization of guests under mechanical stimulation. Moreover, the host-guest complexes also exhibit outstanding MCL property in the polyvinyl alcohol (PVA) film. This strategy is both conceptually and synthetically simple and provides a promising method for preparing high-contrast MCL materials.
Constructing high-contrast mechanochromic luminescent (MCL) materials with a wide range of emission color variations remains challenging. Herein, a host-guest strategy is proposed to optimize molecular MCL behavior. Two pyridinium-functionalized carbazole derivatives only exhibit a slight red-shifted fluorescence under mechanical stimulation. By forming host-guest complexes with cucurbit[n]urils (CB[n]s, n = 8 or 10), the complexes demonstrate more significant fluorescence wavelength changes after grinding. Mechanistic studies reveal that the crystallization and CB[n]’s confinement effect, synergistically induce more twisted molecular conformations and facilitate the planarization of guests under mechanical stimulation. Moreover, the host-guest complexes also exhibit outstanding MCL property in the polyvinyl alcohol (PVA) film. This strategy is both conceptually and synthetically simple and provides a promising method for preparing high-contrast MCL materials.
Water-dispersible cyclen-based porous organic polymers for CO2 direct air capture and photoreduction
2026, 37(9): 112222
doi: 10.1016/j.cclet.2025.112222
Abstract:
Porous organic polymers (POPs) are promising candidates for CO2 capture and conversion, yet the integration of direct air capture (DAC) and in situ conversion presents a fundamental challenge. Here, we report six novel water-dispersible cyclen-based POPs for efficient atmospheric CO2 capture and photoreduction. The resulting POPs (POP-1~6) exhibit exceptional aqueous-phase CO2 uptake (264–569 mg/g) with DAC capacities reaching 11–49 mg g−1 d−1. When integrated with an iron porphyrin catalyst (Fe-P) and a ruthenium-based photosensitizer, these POPs enable efficient photocatalytic atmospheric CO2-to-CO conversion with rates of 1.4–4.5 µmol g−1 h−1 and a yield up to 93% in water. These findings provide valuable insights for the further exploration of POP materials for atmospheric CO2 capture and photoreduction.
Porous organic polymers (POPs) are promising candidates for CO2 capture and conversion, yet the integration of direct air capture (DAC) and in situ conversion presents a fundamental challenge. Here, we report six novel water-dispersible cyclen-based POPs for efficient atmospheric CO2 capture and photoreduction. The resulting POPs (POP-1~6) exhibit exceptional aqueous-phase CO2 uptake (264–569 mg/g) with DAC capacities reaching 11–49 mg g−1 d−1. When integrated with an iron porphyrin catalyst (Fe-P) and a ruthenium-based photosensitizer, these POPs enable efficient photocatalytic atmospheric CO2-to-CO conversion with rates of 1.4–4.5 µmol g−1 h−1 and a yield up to 93% in water. These findings provide valuable insights for the further exploration of POP materials for atmospheric CO2 capture and photoreduction.
2026, 37(9): 112296
doi: 10.1016/j.cclet.2025.112296
Abstract:
The development of novel catalysts with both robust activity and long-term stability is significant but remains a critical challenge for the degradation of emerging pollutants. Herein, CoSe nanocrystal-embedded amorphous carbon (CoSe/MC) was rationally designed and synthesized via an in situ selenization strategy. Interestingly, the unique hierarchical architecture featuring CoSe nanocrystal cores and carbon shells simultaneously exposes abundant accessible active sites and enhances stability during the Fenton-like process. Under ambient conditions, CoSe/MC achieves 97% tetracycline (TC) degradation within 2 min, with a rate constant of 3.74 × 10–2 s-1, which is 7.3-fold faster than Co3O4/C. Furthermore, CoSe/MC exhibits remarkable versatility across a wide pH range (3–11), various water sources (e.g., river/lake water), and diverse pollutants (e.g., antibiotics/dyes). Continuous-flow tests confirm long-term stability (>95% efficiency over 300 min) with negligible metal leaching (<0.1 mg/L Co). Mechanistic studies reveal a synergistic radical/non-radical pathway dominated by 1O2 generation, validated by EPR spectroscopy and quenching experiments. Density functional theory (DFT) calculations further elucidate the key role of CoSe in activating PMS by elongating O–O bonds considerably and accelerating electron transfer, which synergistically promotes O–O cleavage and the generation of reactive oxygen species during TC degradation.
The development of novel catalysts with both robust activity and long-term stability is significant but remains a critical challenge for the degradation of emerging pollutants. Herein, CoSe nanocrystal-embedded amorphous carbon (CoSe/MC) was rationally designed and synthesized via an in situ selenization strategy. Interestingly, the unique hierarchical architecture featuring CoSe nanocrystal cores and carbon shells simultaneously exposes abundant accessible active sites and enhances stability during the Fenton-like process. Under ambient conditions, CoSe/MC achieves 97% tetracycline (TC) degradation within 2 min, with a rate constant of 3.74 × 10–2 s-1, which is 7.3-fold faster than Co3O4/C. Furthermore, CoSe/MC exhibits remarkable versatility across a wide pH range (3–11), various water sources (e.g., river/lake water), and diverse pollutants (e.g., antibiotics/dyes). Continuous-flow tests confirm long-term stability (>95% efficiency over 300 min) with negligible metal leaching (<0.1 mg/L Co). Mechanistic studies reveal a synergistic radical/non-radical pathway dominated by 1O2 generation, validated by EPR spectroscopy and quenching experiments. Density functional theory (DFT) calculations further elucidate the key role of CoSe in activating PMS by elongating O–O bonds considerably and accelerating electron transfer, which synergistically promotes O–O cleavage and the generation of reactive oxygen species during TC degradation.
2026, 37(9): 112313
doi: 10.1016/j.cclet.2025.112313
Abstract:
The structure of photocatalysts largely determines the selectivity of CO2 conversion products in CO2 photoreduction reaction, while it is dynamic during the photoreaction. Therefore, how the dynamic structure affecting photoactivity deserves further investigation. Herein, with defective oxygen vacancies BiOCl/C3N5 nanosheets heterojunction (BiO1-xCl/C3N5) as model photocatalyst, the structure dynamic evolution in CO2 photoreduction reaction and its influence on the CO2-to-CO directional conversion were investigated. Specially, in BiO1-xCl/C3N5, the exposed Bi atoms adjected oxygen vacancies interacted with N atoms of C3N5 via the strong electrostatic effect, resulting in the shrinking crystalline structures. Once illuminated, the photogenerated electrons enriched on Bi active sites, which further strengthened the interfacial interaction between BiO1-xCl and C3N5 to a quasi-bonding state. The resulting changes in electronic structure destroyed the linear structure of CO2 molecule pre-adsorbed on Bi sites, accompanying with transformation of Bi atom valence states and heterostructure restoration. As a result, the *CO2 molecule activation and *CO intermediate desorption barrier energies both reduced, promoting the CO2-to-CO directional conversion with a CO evolution rate of 207.3 μmol g−1 h−1. This work demonstrated the importance of studying the structural dynamics evolution in photoreactions, which may be beneficial for future photocatalyst design.
The structure of photocatalysts largely determines the selectivity of CO2 conversion products in CO2 photoreduction reaction, while it is dynamic during the photoreaction. Therefore, how the dynamic structure affecting photoactivity deserves further investigation. Herein, with defective oxygen vacancies BiOCl/C3N5 nanosheets heterojunction (BiO1-xCl/C3N5) as model photocatalyst, the structure dynamic evolution in CO2 photoreduction reaction and its influence on the CO2-to-CO directional conversion were investigated. Specially, in BiO1-xCl/C3N5, the exposed Bi atoms adjected oxygen vacancies interacted with N atoms of C3N5 via the strong electrostatic effect, resulting in the shrinking crystalline structures. Once illuminated, the photogenerated electrons enriched on Bi active sites, which further strengthened the interfacial interaction between BiO1-xCl and C3N5 to a quasi-bonding state. The resulting changes in electronic structure destroyed the linear structure of CO2 molecule pre-adsorbed on Bi sites, accompanying with transformation of Bi atom valence states and heterostructure restoration. As a result, the *CO2 molecule activation and *CO intermediate desorption barrier energies both reduced, promoting the CO2-to-CO directional conversion with a CO evolution rate of 207.3 μmol g−1 h−1. This work demonstrated the importance of studying the structural dynamics evolution in photoreactions, which may be beneficial for future photocatalyst design.
2026, 37(9): 112407
doi: 10.1016/j.cclet.2026.112407
Abstract:
Thrombin can participate in many physiological and pathological processes so that its sensitive determination is important in diagnostic and pharmaceutical fields. The content of hirudin in leech is a key criterion for determining the quality of leech. In this work, a dual-modal biosensor was constructed based on fluorescence resonance energy transfer between UCNPs and Cy5 via a thrombin-responsive peptide as a linker. Thrombin cleaved the peptide and Cy5 released, leading to the fluorescence recovery of UCNPs at a specific wavelength, which enabled the successful ratiometric fluorescence detection of thrombin. Simultaneously, Cy5 in the supernatant allowed a colorimetric detection. Hirudin inhibited the activity of thrombin, causing the intensity reduction of the corresponding fluorescence and absorbance signals. The linear ranges of the fluorescence and colorimetric detection for thrombin were 10−9 ~ 10−4 U/mL with a detection limit of 1.15 × 10−10 U/mL and 0.0025–5 U/mL with a detection limit of 1.12 × 10−3 U/mL, respectively. The linear ranges of the fluorescence and colorimetric detection for hirudin were 10−8–10−4 U/mL with a detection limit of 6.026 × 10−9 U/mL and 0.005–5 U/mL with a detection limit of 2.82 × 10−3 U/mL, respectively. This developed biosensor was further applied to the detection of anti-thrombin components in leech extract and the results showed that it had an excellent analytical performance, indicating this dual-modal biosensor provided a new specific and sensitive method for the detection of anti-thrombin components in practical sample, which is significant in quality evaluation of traditional Chinese medicine.
Thrombin can participate in many physiological and pathological processes so that its sensitive determination is important in diagnostic and pharmaceutical fields. The content of hirudin in leech is a key criterion for determining the quality of leech. In this work, a dual-modal biosensor was constructed based on fluorescence resonance energy transfer between UCNPs and Cy5 via a thrombin-responsive peptide as a linker. Thrombin cleaved the peptide and Cy5 released, leading to the fluorescence recovery of UCNPs at a specific wavelength, which enabled the successful ratiometric fluorescence detection of thrombin. Simultaneously, Cy5 in the supernatant allowed a colorimetric detection. Hirudin inhibited the activity of thrombin, causing the intensity reduction of the corresponding fluorescence and absorbance signals. The linear ranges of the fluorescence and colorimetric detection for thrombin were 10−9 ~ 10−4 U/mL with a detection limit of 1.15 × 10−10 U/mL and 0.0025–5 U/mL with a detection limit of 1.12 × 10−3 U/mL, respectively. The linear ranges of the fluorescence and colorimetric detection for hirudin were 10−8–10−4 U/mL with a detection limit of 6.026 × 10−9 U/mL and 0.005–5 U/mL with a detection limit of 2.82 × 10−3 U/mL, respectively. This developed biosensor was further applied to the detection of anti-thrombin components in leech extract and the results showed that it had an excellent analytical performance, indicating this dual-modal biosensor provided a new specific and sensitive method for the detection of anti-thrombin components in practical sample, which is significant in quality evaluation of traditional Chinese medicine.
2026, 37(9): 112409
doi: 10.1016/j.cclet.2026.112409
Abstract:
At present, the practical application of photocatalysis is still limited by poor charge carrier separation efficiency. The incorporation of a piezoelectric polarization field is an effective strategy to enhance the photogenerated charge transport rate and strengthen the photocatalytic activity. In this work, a NaNbO3/AgI (NBO/AgI) heterojunction was fabricated for the efficient piezo-photocatalytic degradation of sulfamethoxazole (SMZ). 91.6% of SMZ was degraded within 30 min, which far surpasses degradation under individual photocatalysis or piezocatalysis. Density functional theory (DFT) calculations reveal that electron cloud interactions form interfacial cascade channels at the NBO/AgI heterojunction interface, facilitating charge transport. Meanwhile, the piezoelectric polarization field promotes the separation and migration of photogenerated charges, inducing high-efficiency piezo-photocatalytic performance. The piezo-photocatalytic mechanism was explored by electron paramagnetic resonance, piezo-response force microscopy. Intermediate analysis confirmed the degradation pathways and reduced ecological risks of intermediates. This study provides new insights for the design of piezo-photocatalytic materials, as well as a fresh perspective on the treatment of pollutants in wastewater.
At present, the practical application of photocatalysis is still limited by poor charge carrier separation efficiency. The incorporation of a piezoelectric polarization field is an effective strategy to enhance the photogenerated charge transport rate and strengthen the photocatalytic activity. In this work, a NaNbO3/AgI (NBO/AgI) heterojunction was fabricated for the efficient piezo-photocatalytic degradation of sulfamethoxazole (SMZ). 91.6% of SMZ was degraded within 30 min, which far surpasses degradation under individual photocatalysis or piezocatalysis. Density functional theory (DFT) calculations reveal that electron cloud interactions form interfacial cascade channels at the NBO/AgI heterojunction interface, facilitating charge transport. Meanwhile, the piezoelectric polarization field promotes the separation and migration of photogenerated charges, inducing high-efficiency piezo-photocatalytic performance. The piezo-photocatalytic mechanism was explored by electron paramagnetic resonance, piezo-response force microscopy. Intermediate analysis confirmed the degradation pathways and reduced ecological risks of intermediates. This study provides new insights for the design of piezo-photocatalytic materials, as well as a fresh perspective on the treatment of pollutants in wastewater.
2026, 37(9): 112410
doi: 10.1016/j.cclet.2026.112410
Abstract:
Traditional carbon-based catalysts often suffer from limited catalytic activity and stability in peroxymonosulfate (PMS) activation for pollutant degradation. In this study, a Si–O doped layered carbonaceous catalyst (Si/C@PDA) was synthesized using natural vermiculite as the hard template, enabling the efficient PMS activation for ultrafast degradation of tetracycline (TC) (kobs-TC = 0.228 min–1). The Si/C@PDA/PMS system demonstrated strong resistance to environmental matrix interference by enhanced singlet oxygen (1O2) generation and electron transfer processes (ETP). The experimental and density functional theory results prove that the Si–O site induced the cleavage of adsorbed PMS to promote the generation of 1O2 through the self-decomposition of peroxymonosulfate anion radical (SO5•–) and the disproportionation of superoxide radical (O2•–). Meanwhile, the Si–O site also served as the electron transfer bridge facilitating electron migration from the pollutants to the Si/C@PDA/PMS*. In addition, the Si/C@PDA/PMS system integrated with membrane filtration technology achieved continuous degradation of TC with nearly 100% removal efficiency under a low oxidant dosage (0.1 mmol/L PMS). This work underscores the pivotal role of Si–O doping in modulating active sites to selectively promote nonradical pathways, thereby promoting effective pollutant degradation in complex water matrices and offering strategic insights for developing nonradical-dominated carbon-based catalysts.
Traditional carbon-based catalysts often suffer from limited catalytic activity and stability in peroxymonosulfate (PMS) activation for pollutant degradation. In this study, a Si–O doped layered carbonaceous catalyst (Si/C@PDA) was synthesized using natural vermiculite as the hard template, enabling the efficient PMS activation for ultrafast degradation of tetracycline (TC) (kobs-TC = 0.228 min–1). The Si/C@PDA/PMS system demonstrated strong resistance to environmental matrix interference by enhanced singlet oxygen (1O2) generation and electron transfer processes (ETP). The experimental and density functional theory results prove that the Si–O site induced the cleavage of adsorbed PMS to promote the generation of 1O2 through the self-decomposition of peroxymonosulfate anion radical (SO5•–) and the disproportionation of superoxide radical (O2•–). Meanwhile, the Si–O site also served as the electron transfer bridge facilitating electron migration from the pollutants to the Si/C@PDA/PMS*. In addition, the Si/C@PDA/PMS system integrated with membrane filtration technology achieved continuous degradation of TC with nearly 100% removal efficiency under a low oxidant dosage (0.1 mmol/L PMS). This work underscores the pivotal role of Si–O doping in modulating active sites to selectively promote nonradical pathways, thereby promoting effective pollutant degradation in complex water matrices and offering strategic insights for developing nonradical-dominated carbon-based catalysts.
2026, 37(9): 112412
doi: 10.1016/j.cclet.2026.112412
Abstract:
A novel in-situ method for creating a CO2-responsive switchable deep eutectic solvent (SDES) was developed for the homogeneous liquid-liquid microextraction (HLLME) of 18 polychlorinated biphenyls (PCBs) compounds from water samples. Following extraction, the compounds were separated and analyzed by gas chromatography-triple quadrupole tandem mass spectrometry (GC–MS/MS). Diethanolamine (DEA) was employed as the hydrogen bond acceptor (HBA), while 3-methoxyphenol (3-MP) served as the hydrogen bond donor (HBD). The in-situ formed CO2-responsive SDES was used as the extractant, representing a green alternative to traditional toxic organic reagents. Under ideal extraction conditions, a strong linear relationship was established over the concentration range of 0.1–100 ng/mL. The limits of detection (LODs) and quantification (LOQs) were found to be between 0.001–0.040 ng/mL and 0.004–0.134 ng/mL. The preconcentration factors (PFs) varied from 49 to 76, while both intra-day and inter-day precision (RSDs) remained under 6.8%. Ultimately, the method proved successful in detecting 18 PCBs in environmental water samples, with satisfactory recovery rates. These results demonstrate that the method is not only green and sustainable, but also exhibits excellent methodological performance, rendering it highly promising for applications in the field of HLLME.
A novel in-situ method for creating a CO2-responsive switchable deep eutectic solvent (SDES) was developed for the homogeneous liquid-liquid microextraction (HLLME) of 18 polychlorinated biphenyls (PCBs) compounds from water samples. Following extraction, the compounds were separated and analyzed by gas chromatography-triple quadrupole tandem mass spectrometry (GC–MS/MS). Diethanolamine (DEA) was employed as the hydrogen bond acceptor (HBA), while 3-methoxyphenol (3-MP) served as the hydrogen bond donor (HBD). The in-situ formed CO2-responsive SDES was used as the extractant, representing a green alternative to traditional toxic organic reagents. Under ideal extraction conditions, a strong linear relationship was established over the concentration range of 0.1–100 ng/mL. The limits of detection (LODs) and quantification (LOQs) were found to be between 0.001–0.040 ng/mL and 0.004–0.134 ng/mL. The preconcentration factors (PFs) varied from 49 to 76, while both intra-day and inter-day precision (RSDs) remained under 6.8%. Ultimately, the method proved successful in detecting 18 PCBs in environmental water samples, with satisfactory recovery rates. These results demonstrate that the method is not only green and sustainable, but also exhibits excellent methodological performance, rendering it highly promising for applications in the field of HLLME.
2026, 37(9): 112434
doi: 10.1016/j.cclet.2026.112434
Abstract:
Cyanuric acid (CA), a stable triazine-based compound widely used in chlorinated disinfectants, has emerged as a recalcitrant contaminant frequently detected in aquatic environments. Due to its high chemical stability and electron-deficient structure, CA resists degradation by conventional oxidative processes. Here, a tandem UV/sulfite (SF)-based photochemical reduction-electrochemical oxidation (EO) process was developed to achieve complete mineralization of CA. Hydrated electrons generated in the UV/SF process efficiently induce triazine ring-opening, while EO further oxidizes the resulting intermediates. Density functional theory calculations and quenching experiments revealed that CA exhibits high activation barriers toward direct oxidation by •OH and SO4•−, explaining their limited reactivity. In contrast, direct electron transfer to the boron-doped diamond (BDD) anode dominates CA degradation in the EO process, albeit with sluggish kinetics due to the high oxidation potential. The tandem system effectively lowers the oxidative energy barrier via reductive fragmentation. Moreover, the UV/SF-EO process demonstrated reliable and effective performance in natural waters and industrial effluents. This study not only highlights the synergistic benefits of coupling reduction and oxidation for the treatment of persistent organic pollutants but also provides mechanistic insight into CA degradation pathways, offering a promising strategy for mitigating CA pollution in complex water environments.
Cyanuric acid (CA), a stable triazine-based compound widely used in chlorinated disinfectants, has emerged as a recalcitrant contaminant frequently detected in aquatic environments. Due to its high chemical stability and electron-deficient structure, CA resists degradation by conventional oxidative processes. Here, a tandem UV/sulfite (SF)-based photochemical reduction-electrochemical oxidation (EO) process was developed to achieve complete mineralization of CA. Hydrated electrons generated in the UV/SF process efficiently induce triazine ring-opening, while EO further oxidizes the resulting intermediates. Density functional theory calculations and quenching experiments revealed that CA exhibits high activation barriers toward direct oxidation by •OH and SO4•−, explaining their limited reactivity. In contrast, direct electron transfer to the boron-doped diamond (BDD) anode dominates CA degradation in the EO process, albeit with sluggish kinetics due to the high oxidation potential. The tandem system effectively lowers the oxidative energy barrier via reductive fragmentation. Moreover, the UV/SF-EO process demonstrated reliable and effective performance in natural waters and industrial effluents. This study not only highlights the synergistic benefits of coupling reduction and oxidation for the treatment of persistent organic pollutants but also provides mechanistic insight into CA degradation pathways, offering a promising strategy for mitigating CA pollution in complex water environments.
Engineering amorphous MOF with P–Fe–O sites for robust electro-Fenton degradation of micropollutants
2026, 37(9): 112442
doi: 10.1016/j.cclet.2026.112442
Abstract:
Iron-based metal-organic frameworks (MOFs) stand out as promising catalysts for heterogeneous electro-Fenton (HEF) treatment of micropollutants, yet their performance is often constrained by the limited accessibility of active sites and sluggish electron transfer. Herein, a facile phosphine-assisted amorphization strategy was proposed to convert crystalline MIL-88B(Fe) into a P-coordinated amorphous counterpart (aMIL-88B(Fe)-P) featuring abundant asymmetric P–Fe–O moieties. The amorphous architecture ensures abundant exposure of active sites and enhanced mass transport, while the asymmetric coordination environment upshifts the Fe d-band center toward the Fermi level, thereby lowering the energy barrier for H2O2 activation. Notably, the aMIL-88B(Fe)-P-catalyzed EF system attained complete naproxen removal within 90 min, with a pseudo-first-order kinetic rate constant of 0.038 min-1, outperforming all comparative trials and many reported HEF systems. Moreover, the system demonstrated broad-spectrum micropollutant removal, favorable catalyst reusability, and remarkable scalability in a flow-through electrochemical device, confirming strong practical applicability. This work highlights the potential of combining structural amorphization with precise coordination engineering to fully unlock the catalytic potential of MOFs for advanced EF applications.
Iron-based metal-organic frameworks (MOFs) stand out as promising catalysts for heterogeneous electro-Fenton (HEF) treatment of micropollutants, yet their performance is often constrained by the limited accessibility of active sites and sluggish electron transfer. Herein, a facile phosphine-assisted amorphization strategy was proposed to convert crystalline MIL-88B(Fe) into a P-coordinated amorphous counterpart (aMIL-88B(Fe)-P) featuring abundant asymmetric P–Fe–O moieties. The amorphous architecture ensures abundant exposure of active sites and enhanced mass transport, while the asymmetric coordination environment upshifts the Fe d-band center toward the Fermi level, thereby lowering the energy barrier for H2O2 activation. Notably, the aMIL-88B(Fe)-P-catalyzed EF system attained complete naproxen removal within 90 min, with a pseudo-first-order kinetic rate constant of 0.038 min-1, outperforming all comparative trials and many reported HEF systems. Moreover, the system demonstrated broad-spectrum micropollutant removal, favorable catalyst reusability, and remarkable scalability in a flow-through electrochemical device, confirming strong practical applicability. This work highlights the potential of combining structural amorphization with precise coordination engineering to fully unlock the catalytic potential of MOFs for advanced EF applications.
2026, 37(9): 112443
doi: 10.1016/j.cclet.2026.112443
Abstract:
The effective FeⅡ/FeⅢ cycling and rapid activation of oxidants are the key problems that expand the application of iron-based Fenton-like reaction in water purification. Herein, bamboo-like Fe-Mo bimetallic catalysts (FeMo@CNT) were prepared to activate peroxydisulfate (PDS) for organic pollutants removal. FeMo@CNT/PDS system can completely degrade bisphenol (BPA) within 30 min (kobs = 0.444 min-1, which was 17.1 times that of Fe@CNT/PDS system). Results showed that singlet oxygen (1O2) and sulfate radical (SO4•-) were dominant reactive oxygen species in FeMo@CNT/PDS/BPA system, where 1O2 was derived from superoxide radical (O2•-) oxidized by SO4•-. Mo species in FeMo@CNT/PDS system could accelerate the O–O breaking in PDS and reduce the energy barrier of 1O2 production, thus achieving the increase of both SO4•- and 1O2. Meanwhile, FeMo@CNT/PDS system exhibited good catalytic activity with wide pH and multiple environmental substrates. The high oxidation performance after 23 h in dynamic experiments further demonstrated the stability of this system. And the toxicity of the original pollutants was further declined, indicating that the FeMo@CNT/PDS system was ecologically friendly. This work provides new insights for solving hindered FeⅡ/FeⅢ cycle and proves a new mechanism of 1O2 generation in SR-AOPs.
The effective FeⅡ/FeⅢ cycling and rapid activation of oxidants are the key problems that expand the application of iron-based Fenton-like reaction in water purification. Herein, bamboo-like Fe-Mo bimetallic catalysts (FeMo@CNT) were prepared to activate peroxydisulfate (PDS) for organic pollutants removal. FeMo@CNT/PDS system can completely degrade bisphenol (BPA) within 30 min (kobs = 0.444 min-1, which was 17.1 times that of Fe@CNT/PDS system). Results showed that singlet oxygen (1O2) and sulfate radical (SO4•-) were dominant reactive oxygen species in FeMo@CNT/PDS/BPA system, where 1O2 was derived from superoxide radical (O2•-) oxidized by SO4•-. Mo species in FeMo@CNT/PDS system could accelerate the O–O breaking in PDS and reduce the energy barrier of 1O2 production, thus achieving the increase of both SO4•- and 1O2. Meanwhile, FeMo@CNT/PDS system exhibited good catalytic activity with wide pH and multiple environmental substrates. The high oxidation performance after 23 h in dynamic experiments further demonstrated the stability of this system. And the toxicity of the original pollutants was further declined, indicating that the FeMo@CNT/PDS system was ecologically friendly. This work provides new insights for solving hindered FeⅡ/FeⅢ cycle and proves a new mechanism of 1O2 generation in SR-AOPs.
2026, 37(9): 112449
doi: 10.1016/j.cclet.2026.112449
Abstract:
Genetically encoded sensors have been extensively utilized for the analysis of biomarkers. However, their applications remain limited by the scarcity of analyte-binding proteins or peptides and the challenges associated with translating analyte recognition into a quantifiable signal. Herein, we report a novel class of activable chimeric sensors that harness bioluminescent resonance energy transfer (BRET) between nanoluciferase proteins and fluorescent small-molecule probes. We demonstrated that the responsiveness of these hybrid sensors can be significantly enhanced by modulating the electrostatic surface potential of the fusion protein in the vicinity of the recognition site. As proof of concept, we engineered two chimeric bioluminescent sensors, Bp7-pH and Bp7-NO, for the detection of pH and nitric oxide (NO), respectively. Both sensors exhibited strong BRET signal modulation upon exposure to their target analytes, leading to distinct and quantifiable shifts in luminescence color. Importantly, we successfully applied these sensors for field-deployable imaging of pH and NO dynamics in a murine wound infection model. Given the vast array of existing fluorescent molecular sensors, the detection targets of these chimeric bioluminescent sensors can be easily modified by altering the recognition moieties. Collectively, this work establishes a generalizable and tunable design strategy for developing highly sensitive chimeric bioluminescent sensors, with broad applicability in physiological and pathological monitoring.
Genetically encoded sensors have been extensively utilized for the analysis of biomarkers. However, their applications remain limited by the scarcity of analyte-binding proteins or peptides and the challenges associated with translating analyte recognition into a quantifiable signal. Herein, we report a novel class of activable chimeric sensors that harness bioluminescent resonance energy transfer (BRET) between nanoluciferase proteins and fluorescent small-molecule probes. We demonstrated that the responsiveness of these hybrid sensors can be significantly enhanced by modulating the electrostatic surface potential of the fusion protein in the vicinity of the recognition site. As proof of concept, we engineered two chimeric bioluminescent sensors, Bp7-pH and Bp7-NO, for the detection of pH and nitric oxide (NO), respectively. Both sensors exhibited strong BRET signal modulation upon exposure to their target analytes, leading to distinct and quantifiable shifts in luminescence color. Importantly, we successfully applied these sensors for field-deployable imaging of pH and NO dynamics in a murine wound infection model. Given the vast array of existing fluorescent molecular sensors, the detection targets of these chimeric bioluminescent sensors can be easily modified by altering the recognition moieties. Collectively, this work establishes a generalizable and tunable design strategy for developing highly sensitive chimeric bioluminescent sensors, with broad applicability in physiological and pathological monitoring.
2026, 37(9): 112450
doi: 10.1016/j.cclet.2026.112450
Abstract:
How to precisely discriminate homologous microRNA sequences from each other has always been a big challenge. Herein, we proposed an artificial mismatch-assisted Cas12a crRNA splicing mechanism that enables completely interference-free discrimination of homologous microRNAs with single-nucleotide resolution. Specifically, a truncated crRNA (tcrRNA) can recover its ability to activate Cas12a trans-cleavage activity when spliced with a miRNA. Since the miRNA splicing region itself is relatively short, rationally tuning the tcrRNA splicing length can render the proposed system with high sensitivity for base-variation discrimination. More importantly, we innovatively introduced an extra artificial mismatch in the miRNA splicing region, which enables the system to distinguish single-nucleotide variants in an interference-free manner. In this way, only the perfectly matched target miRNA can trigger the complete assembly of the spliced crRNA to active Cas12a, while non-target RNAs even with a single-base mismatch cannot. This mechanism ensures that the target miRNA can be accurately hooked even in the presence of a large excess of non-target homologous RNAs (100-fold). The discrimination capability of the proposed method has been proven by achieving the interference-free discrimination of the members within the let-7 family, which can hardly be achieved by conventional hybridization-based amplification methods. This work fully taps into the potential of the Cas12a system in interference-free homologous miRNA discrimination, offering a new tool for precise RNA analysis in molecular diagnostics.
How to precisely discriminate homologous microRNA sequences from each other has always been a big challenge. Herein, we proposed an artificial mismatch-assisted Cas12a crRNA splicing mechanism that enables completely interference-free discrimination of homologous microRNAs with single-nucleotide resolution. Specifically, a truncated crRNA (tcrRNA) can recover its ability to activate Cas12a trans-cleavage activity when spliced with a miRNA. Since the miRNA splicing region itself is relatively short, rationally tuning the tcrRNA splicing length can render the proposed system with high sensitivity for base-variation discrimination. More importantly, we innovatively introduced an extra artificial mismatch in the miRNA splicing region, which enables the system to distinguish single-nucleotide variants in an interference-free manner. In this way, only the perfectly matched target miRNA can trigger the complete assembly of the spliced crRNA to active Cas12a, while non-target RNAs even with a single-base mismatch cannot. This mechanism ensures that the target miRNA can be accurately hooked even in the presence of a large excess of non-target homologous RNAs (100-fold). The discrimination capability of the proposed method has been proven by achieving the interference-free discrimination of the members within the let-7 family, which can hardly be achieved by conventional hybridization-based amplification methods. This work fully taps into the potential of the Cas12a system in interference-free homologous miRNA discrimination, offering a new tool for precise RNA analysis in molecular diagnostics.
2026, 37(9): 112487
doi: 10.1016/j.cclet.2026.112487
Abstract:
Cataracts, particularly diabetic cataracts (DC), represent a significant cause of blindness, exacerbated by diabetes mellitus. Monitoring intracellular pH (pHi) in human lens epithelial cells (HLECs) provides valuable insights into the pathogenesis of DC. This study introduces a novel phenol-armed flavylium-based fluorescent probe (FpH-2) for real-time pH monitoring in HLECs. The probe is facilely prepared to offer a reversible and highly sensitive fluorescence response to pH changes, with a pKa value of 6.66. The probe’s efficacy was demonstrated through its ability to monitor pH elevation under high glucose conditions, simulating diabetic stress. The study further investigates the effects of various clinical drugs on pH regulation in HLECs, offering new perspectives for managing DC. The findings suggest that pHi serves as a critical parameter for investigating DC pathophysiology and pharmacology, offering potential for advancing early diagnostic and therapeutic strategies.
Cataracts, particularly diabetic cataracts (DC), represent a significant cause of blindness, exacerbated by diabetes mellitus. Monitoring intracellular pH (pHi) in human lens epithelial cells (HLECs) provides valuable insights into the pathogenesis of DC. This study introduces a novel phenol-armed flavylium-based fluorescent probe (FpH-2) for real-time pH monitoring in HLECs. The probe is facilely prepared to offer a reversible and highly sensitive fluorescence response to pH changes, with a pKa value of 6.66. The probe’s efficacy was demonstrated through its ability to monitor pH elevation under high glucose conditions, simulating diabetic stress. The study further investigates the effects of various clinical drugs on pH regulation in HLECs, offering new perspectives for managing DC. The findings suggest that pHi serves as a critical parameter for investigating DC pathophysiology and pharmacology, offering potential for advancing early diagnostic and therapeutic strategies.
2026, 37(9): 112521
doi: 10.1016/j.cclet.2026.112521
Abstract:
Inspired by natural photosynthesis, visible-light-driven carboxylation of carbon dioxide for the synthesis of value-added chemicals has attracted considerable attention. However, the current limitation in carboxylation lies in the narrow absorption range of the photocatalysts used. These photocatalysts are predominantly activated by blue light, limiting the utilization of most of the solar light. Herein, we employed the organic dye N,N-bis(2,6-diisopropylphenyl)perylene-3,4,9,10-bis(dicarboximide) (PDI), along with its single-electron-reduced state PDI•− through consecutive photoinduced electron transfer (ConPET), effectively absorbs panchromatic solar spectrum for photocatalytic dicarboxylation. Mechanistic investigations using femtosecond time-resolved transient absorption (fs-TA) spectroscopy unequivocally identified the excited state of the singly reduced species, PDI•−*, rather than the doubly reduced form, as the key intermediate responsible for the reductive activation of alkenes. Furthermore, efficient solar-driven carboxylation of CO2 was successfully demonstrated under natural sunlight irradiation, underscoring the practical potential of this photocatalytic system.
Inspired by natural photosynthesis, visible-light-driven carboxylation of carbon dioxide for the synthesis of value-added chemicals has attracted considerable attention. However, the current limitation in carboxylation lies in the narrow absorption range of the photocatalysts used. These photocatalysts are predominantly activated by blue light, limiting the utilization of most of the solar light. Herein, we employed the organic dye N,N-bis(2,6-diisopropylphenyl)perylene-3,4,9,10-bis(dicarboximide) (PDI), along with its single-electron-reduced state PDI•− through consecutive photoinduced electron transfer (ConPET), effectively absorbs panchromatic solar spectrum for photocatalytic dicarboxylation. Mechanistic investigations using femtosecond time-resolved transient absorption (fs-TA) spectroscopy unequivocally identified the excited state of the singly reduced species, PDI•−*, rather than the doubly reduced form, as the key intermediate responsible for the reductive activation of alkenes. Furthermore, efficient solar-driven carboxylation of CO2 was successfully demonstrated under natural sunlight irradiation, underscoring the practical potential of this photocatalytic system.
2026, 37(9): 112540
doi: 10.1016/j.cclet.2026.112540
Abstract:
Zinc anode as one of the most promising energy storage materials for aqueous zinc-ion batteries (AZIBs), suffer from significant degradation in cycle life and Coulombic efficiency (CE) due to uncontrolled dendrite growth and H2O-induced side reactions. In this work, we propose a nonionic dual-additive (gelatin, urea, abbreviated as GU) strategy that utilizes the dual hydrogen bond (H-bond) network H2O-locking structure. Due to the H-bond reinforcement effect introduced by the GU additive, the energy barrier for H-bond breaking and reconfiguration is elevated, effectively impeding the rapid proton shuttling between H2O molecules. It can induce the preferred growth of the (002) crystal plane by adsorbing onto other crystal planes, thereby achieving a dendrite-free zinc anode. Thus, the stability and reversibility of the zinc anode have improved significantly. The symmetrical cells stably cycled for more than 2100 h at 2.0 mA/cm2@1.0 mA/cm2, and the ZnCu asymmetric cells cycled for 1600 times at 5 mA/cm2@1 mAh/cm2 with an average CE of 99.4%. The full cells matched with the PANI cathode cycled more than 3500 times at 1 A/g. The work provides a new strategy for regulating the interfacial chemistry of zinc anodes to achieve highly stable high-performance zinc batteries.
Zinc anode as one of the most promising energy storage materials for aqueous zinc-ion batteries (AZIBs), suffer from significant degradation in cycle life and Coulombic efficiency (CE) due to uncontrolled dendrite growth and H2O-induced side reactions. In this work, we propose a nonionic dual-additive (gelatin, urea, abbreviated as GU) strategy that utilizes the dual hydrogen bond (H-bond) network H2O-locking structure. Due to the H-bond reinforcement effect introduced by the GU additive, the energy barrier for H-bond breaking and reconfiguration is elevated, effectively impeding the rapid proton shuttling between H2O molecules. It can induce the preferred growth of the (002) crystal plane by adsorbing onto other crystal planes, thereby achieving a dendrite-free zinc anode. Thus, the stability and reversibility of the zinc anode have improved significantly. The symmetrical cells stably cycled for more than 2100 h at 2.0 mA/cm2@1.0 mA/cm2, and the ZnCu asymmetric cells cycled for 1600 times at 5 mA/cm2@1 mAh/cm2 with an average CE of 99.4%. The full cells matched with the PANI cathode cycled more than 3500 times at 1 A/g. The work provides a new strategy for regulating the interfacial chemistry of zinc anodes to achieve highly stable high-performance zinc batteries.
2026, 37(9): 112618
doi: 10.1016/j.cclet.2026.112618
Abstract:
Lipid droplets (LDs) serve as central hubs for lipid synthesis, storage, and mobilization, with their biological functions largely governed by the composition of neutral lipid cores. Although in situ probing of LD polarity has emerged as a promising strategy to decode compositional remodeling, probes capable of resolving the subtle and narrowly distributed polarity variations within LD interiors remain scarce. Here we report a phenylethynyl-bridged naphthalimide probe (TS-N) that enables sensitive decoding of LD polarity in living cells. Introduction of a conjugated phenylethynyl spacer significantly increases the intramolecular charge-transfer distance (dCT = 3.561 Å), resulting in enhanced solvatochromic responsiveness with an emission shift exceeding 220 nm across solvent polarity gradients. The probe exhibits a high polarity sensitivity of 14.5 nm per unit, enabling detection of subtle dielectric variations within weakly polar LD interiors. TS-N selectively targets LDs and supports long-term super-resolution imaging of dynamic processes, including LD fusion and mitochondria-LD interactions. Importantly, quantitative in situ fluorescence spectral analysis reveals that TS-N can resolve metabolic perturbation-induced polarity fluctuations at the single-droplet level and correlate dielectric changes with droplet size remodeling. This strategy integrates structural imaging with compositional decoding, providing a powerful tool for investigating LD metabolic heterogeneity and organelle interactions in living cells.
Lipid droplets (LDs) serve as central hubs for lipid synthesis, storage, and mobilization, with their biological functions largely governed by the composition of neutral lipid cores. Although in situ probing of LD polarity has emerged as a promising strategy to decode compositional remodeling, probes capable of resolving the subtle and narrowly distributed polarity variations within LD interiors remain scarce. Here we report a phenylethynyl-bridged naphthalimide probe (TS-N) that enables sensitive decoding of LD polarity in living cells. Introduction of a conjugated phenylethynyl spacer significantly increases the intramolecular charge-transfer distance (dCT = 3.561 Å), resulting in enhanced solvatochromic responsiveness with an emission shift exceeding 220 nm across solvent polarity gradients. The probe exhibits a high polarity sensitivity of 14.5 nm per unit, enabling detection of subtle dielectric variations within weakly polar LD interiors. TS-N selectively targets LDs and supports long-term super-resolution imaging of dynamic processes, including LD fusion and mitochondria-LD interactions. Importantly, quantitative in situ fluorescence spectral analysis reveals that TS-N can resolve metabolic perturbation-induced polarity fluctuations at the single-droplet level and correlate dielectric changes with droplet size remodeling. This strategy integrates structural imaging with compositional decoding, providing a powerful tool for investigating LD metabolic heterogeneity and organelle interactions in living cells.
2026, 37(9): 112633
doi: 10.1016/j.cclet.2026.112633
Abstract:
The pursuit of high color purity in next-generation displays has spurred intense interest in multiple-resonance thermally activated delayed fluorescence (MR-TADF) emitters, which combine narrowband emission with high exciton utilization efficiency. However, the intricate relationship between molecular structure and photophysical properties renders rational design highly challenging. Herein, we present an integrated computational framework that unifies automated data extraction, de novo molecular generation and multi-property prediction for the targeted discovery of MR-TADF materials. Our approach leverages large-language-model-based literature mining and chemical structure recognition to construct a curated dataset (MR585), which guides a Transformer-based variational autoencoder for generative molecular design. Machine learning models trained on this dataset achieve test-set R2 values of 0.692 for predicting the singlet-triplet energy gap (ΔEST) and 0.788 for full width at half maximum (FWHM). From the generated candidates, we identify 15 structurally novel emitters with ΔEST values of 0.13–0.33 eV and narrow FWHMs of 26.2–46.6 nm. Theoretical analysis further reveals that two sulphur-containing BCzBN derivatives exhibit enhanced spin-orbit coupling, accelerated reverse intersystem crossing and reduced efficiency roll-off compared to their parent structures. This work establishes a comprehensive AI-driven platform that bridges automated knowledge extraction with generative chemistry, offering an efficient and scalable pathway towards high-performance narrowband emitters.
The pursuit of high color purity in next-generation displays has spurred intense interest in multiple-resonance thermally activated delayed fluorescence (MR-TADF) emitters, which combine narrowband emission with high exciton utilization efficiency. However, the intricate relationship between molecular structure and photophysical properties renders rational design highly challenging. Herein, we present an integrated computational framework that unifies automated data extraction, de novo molecular generation and multi-property prediction for the targeted discovery of MR-TADF materials. Our approach leverages large-language-model-based literature mining and chemical structure recognition to construct a curated dataset (MR585), which guides a Transformer-based variational autoencoder for generative molecular design. Machine learning models trained on this dataset achieve test-set R2 values of 0.692 for predicting the singlet-triplet energy gap (ΔEST) and 0.788 for full width at half maximum (FWHM). From the generated candidates, we identify 15 structurally novel emitters with ΔEST values of 0.13–0.33 eV and narrow FWHMs of 26.2–46.6 nm. Theoretical analysis further reveals that two sulphur-containing BCzBN derivatives exhibit enhanced spin-orbit coupling, accelerated reverse intersystem crossing and reduced efficiency roll-off compared to their parent structures. This work establishes a comprehensive AI-driven platform that bridges automated knowledge extraction with generative chemistry, offering an efficient and scalable pathway towards high-performance narrowband emitters.
2026, 37(9): 112638
doi: 10.1016/j.cclet.2026.112638
Abstract:
Dual-atom catalysts (DACs) show great potential for boosting reaction kinetics and diversifying active sites via the synergistic effects of two metal atoms. However, the influence of intermetallic interactions on catalytic performance remains underexplored. Herein, we report a Cu/Ni dual-atom catalyst anchored on N-doped carbon (Cu/Ni-N-C) for the electrochemical CO2 reduction reaction (CO2RR). Advanced experimental and theoretical approaches, including X-ray absorption fine structure (XAFS) analysis and density functional theory (DFT) calculations, were employed to systematically investigate the mechanism of intermetallic interactions. Experimental results demonstrate that the monometallic Cu-N-C catalyst achieves a maximum CO Faradaic efficiency (FE) of 38.35% at -1 V vs. RHE, with a non-negligible CH4 FE of 21.89% at -1.4 V vs. RHE. In contrast, the Cu0.5Ni0.5–N-C catalyst exhibits significantly enhanced performance for CO formation, reaching a high CO FE of 96.78% with partial current density of 24.80 mA/cm2 and a negligible CH4 formation. The reason for this selectivity shift is that Ni atoms within the Cu-Ni diatomic pairs in the Cu/Ni-N-C catalyst attract the electron cloud of Cu atoms. This reduces the electron cloud density near Cu atoms, and thus weakens the adsorption of CO2RR intermediates on Cu sites. DFT calculations further reveal that charge regulation between Cu and Ni is the key to the improved CO selectivity: electron-deficient Cu atoms act as O-terminal adsorption sites to bind the oxygen atoms of CO2, while electron-enriched Ni atoms serve as C-terminal adsorption sites to anchor the carbon atoms. This asymmetric adsorption mode promotes CO2 polarization and activation, narrows the HOMO-LUMO band gap for efficient electron transfer, and reduces the thermodynamic barrier for *COOH intermediate formation (ΔG = 1.78 eV vs. 2.52 eV for Cu-N-C). Additionally, the shortened Ni-C bond (1.921 Å vs. 2.207 Å for Cu-N-C) and elongated C–OH bond (1.388 Å vs. 1.376 Å for Cu-N-C) in *COOH on Cu0.5Ni0.5–N-C further favor CO generation. This work provides new insights into the precise design of DACs by regulating intermetallic interactions, advancing their industrial applications in CO2RR.
Dual-atom catalysts (DACs) show great potential for boosting reaction kinetics and diversifying active sites via the synergistic effects of two metal atoms. However, the influence of intermetallic interactions on catalytic performance remains underexplored. Herein, we report a Cu/Ni dual-atom catalyst anchored on N-doped carbon (Cu/Ni-N-C) for the electrochemical CO2 reduction reaction (CO2RR). Advanced experimental and theoretical approaches, including X-ray absorption fine structure (XAFS) analysis and density functional theory (DFT) calculations, were employed to systematically investigate the mechanism of intermetallic interactions. Experimental results demonstrate that the monometallic Cu-N-C catalyst achieves a maximum CO Faradaic efficiency (FE) of 38.35% at -1 V vs. RHE, with a non-negligible CH4 FE of 21.89% at -1.4 V vs. RHE. In contrast, the Cu0.5Ni0.5–N-C catalyst exhibits significantly enhanced performance for CO formation, reaching a high CO FE of 96.78% with partial current density of 24.80 mA/cm2 and a negligible CH4 formation. The reason for this selectivity shift is that Ni atoms within the Cu-Ni diatomic pairs in the Cu/Ni-N-C catalyst attract the electron cloud of Cu atoms. This reduces the electron cloud density near Cu atoms, and thus weakens the adsorption of CO2RR intermediates on Cu sites. DFT calculations further reveal that charge regulation between Cu and Ni is the key to the improved CO selectivity: electron-deficient Cu atoms act as O-terminal adsorption sites to bind the oxygen atoms of CO2, while electron-enriched Ni atoms serve as C-terminal adsorption sites to anchor the carbon atoms. This asymmetric adsorption mode promotes CO2 polarization and activation, narrows the HOMO-LUMO band gap for efficient electron transfer, and reduces the thermodynamic barrier for *COOH intermediate formation (ΔG = 1.78 eV vs. 2.52 eV for Cu-N-C). Additionally, the shortened Ni-C bond (1.921 Å vs. 2.207 Å for Cu-N-C) and elongated C–OH bond (1.388 Å vs. 1.376 Å for Cu-N-C) in *COOH on Cu0.5Ni0.5–N-C further favor CO generation. This work provides new insights into the precise design of DACs by regulating intermetallic interactions, advancing their industrial applications in CO2RR.
2026, 37(9): 112788
doi: 10.1016/j.cclet.2026.112788
Abstract:
Commercialization of rechargeable lithium–sulfur batteries (LSBs) is severely hindered by the "shuttle effect" and their sluggish electrochemical kinetics. Herein, highly matched NbN/TiN heterocrystals with nanosize (< 5 nm) uniformly dispersed within in hollow porous N–doped carbon microspheres (NbN/TiN@N–C) was designed. DFT calculations and electrochemical tests demonstrate the remarkable improvement in anchoring lithium polysulfides (LiPSs) and sulfur redox kinetics. Specifically, the hollow porous frameworks can physically confine LiPSs and effectively alleviate volume changes, and simultaneously the immobilized NbN/TiN nanocrystals can strongly interact with LiPSs by the dual–chemical adsorption that the formation of Nb–S and Ti–S bonds. The nanosized NbN/TiN heterocrystals and their clusters induce maximum reaction surface and numerous activity sites. Significantly, the heterocrystals, based on high lattice matching and stable built–in electric field, endows smooth channels for Li+ diffusion and maximum electron transfer ability to catalysts. The LSBs with NbN/TiN@N–C separator delivers ultralong cycling stability that sustained 545.5 mAh/g with only 0.056% capacity decay per cycle over 1000 cycles at 2 C and high rate performance with 663.7 mAh/g at 10 C. This work provides a novel insight for regulating LiPSs through highly matched binary heterogeneous catalyst to advance the industrial application of LSBs.
Commercialization of rechargeable lithium–sulfur batteries (LSBs) is severely hindered by the "shuttle effect" and their sluggish electrochemical kinetics. Herein, highly matched NbN/TiN heterocrystals with nanosize (< 5 nm) uniformly dispersed within in hollow porous N–doped carbon microspheres (NbN/TiN@N–C) was designed. DFT calculations and electrochemical tests demonstrate the remarkable improvement in anchoring lithium polysulfides (LiPSs) and sulfur redox kinetics. Specifically, the hollow porous frameworks can physically confine LiPSs and effectively alleviate volume changes, and simultaneously the immobilized NbN/TiN nanocrystals can strongly interact with LiPSs by the dual–chemical adsorption that the formation of Nb–S and Ti–S bonds. The nanosized NbN/TiN heterocrystals and their clusters induce maximum reaction surface and numerous activity sites. Significantly, the heterocrystals, based on high lattice matching and stable built–in electric field, endows smooth channels for Li+ diffusion and maximum electron transfer ability to catalysts. The LSBs with NbN/TiN@N–C separator delivers ultralong cycling stability that sustained 545.5 mAh/g with only 0.056% capacity decay per cycle over 1000 cycles at 2 C and high rate performance with 663.7 mAh/g at 10 C. This work provides a novel insight for regulating LiPSs through highly matched binary heterogeneous catalyst to advance the industrial application of LSBs.
2026, 37(9): 112790
doi: 10.1016/j.cclet.2026.112790
Abstract:
This study identifies and characterises a previously unknown diterpene synthase, SjJS, from the acidophilic actinomycete Streptacidiphilus jiangxiensis. Genome mining and heterologous expression demonstrated that Streptacidiphilus jiangxiensis Jiangxidiene Synthase (SjJS) accepts both farnesyl pyrophosphate (FPP) and geranylgeranyl pyrophosphate (GGPP) as substrates to produce a diverse terpene profile, including two new diterpenes, jiangxidiene A (1) and B (2). Comprehensive 13C-labelling experiments combined with computational analyses delineated its intricate cyclisation mechanism and revealed two possible pathways. Structure-guided mutagenesis enabled the accumulation of key intermediate-derived products, jiangxienols A–D (4, 7, 8, and 10), thereby allowing a clear differentiation between the two proposed cyclisation pathways and leading to the formation of several additional diterpenes. In addition, a cytochrome P450 encoded adjacent to the sjjs gene was shown to oxidise jiangxidiene A (1), the major diterpene product, yielding jiangxienoide B (12) and jiangxienol E (13). Further cytotoxicity assays were performed for the isolated compounds, among which jiangxidiene A (1) gave the lowest half maximal inhibitory concentration (IC50) values (15–20 µg/mL) against the tested human cancer cell lines.
This study identifies and characterises a previously unknown diterpene synthase, SjJS, from the acidophilic actinomycete Streptacidiphilus jiangxiensis. Genome mining and heterologous expression demonstrated that Streptacidiphilus jiangxiensis Jiangxidiene Synthase (SjJS) accepts both farnesyl pyrophosphate (FPP) and geranylgeranyl pyrophosphate (GGPP) as substrates to produce a diverse terpene profile, including two new diterpenes, jiangxidiene A (1) and B (2). Comprehensive 13C-labelling experiments combined with computational analyses delineated its intricate cyclisation mechanism and revealed two possible pathways. Structure-guided mutagenesis enabled the accumulation of key intermediate-derived products, jiangxienols A–D (4, 7, 8, and 10), thereby allowing a clear differentiation between the two proposed cyclisation pathways and leading to the formation of several additional diterpenes. In addition, a cytochrome P450 encoded adjacent to the sjjs gene was shown to oxidise jiangxidiene A (1), the major diterpene product, yielding jiangxienoide B (12) and jiangxienol E (13). Further cytotoxicity assays were performed for the isolated compounds, among which jiangxidiene A (1) gave the lowest half maximal inhibitory concentration (IC50) values (15–20 µg/mL) against the tested human cancer cell lines.
2026, 37(9): 112813
doi: 10.1016/j.cclet.2026.112813
Abstract:
Lycibarbarspermidines represent a major class of bioactive components in wolfberry (the fruit of Lycium barbarum), consisting of di-phenylpropionyl spermidines and their glucosides. While the molecular basis underlying their glycodiversity was clarified in our previous work, the biosynthesis of di-phenylpropionyl spermidine core structure remains elusive. In particular, the acyltransferase responsible for conjugating dihydrocaffeoyl, one of the dominant phenylpropionyl moieties, is still unidentified. Herein, two N-hydroxycinnamoyltransferases (LbSCT1/2) from wolfberry were identified, which not only catalyze the conjugation of spermidine with caffeoyl-CoA, but also exhibit high catalytic activity toward dihydrocaffeoyl-CoA. Notably, LbSCT2 catalyzes monoacylation, whereas LbSCT1 enables sequential diacylation. Together with caffeoyl-CoA double bond reductase (LbDBR2), LbSCT1/2 accomplish the biosynthesis of lycibarbarspermidine Ⅰ-Ⅳ. Furthermore, LbSCT1 efficiently catalyzes the biosynthesis of kukoamine B, a major bioactive component from Lycii Cortex (the root bark of Lycium species). Crystal structural and mutagenic investigations elucidated the catalytic mechanisms underlying the selectivity of LbSCT1/2 for spermidine mono- and diacylation. This study establishes the complete biosynthesis of lycibarbarspermidines and provides valuable enzymatic tools for diversifying phenylpropionyl compounds.
Lycibarbarspermidines represent a major class of bioactive components in wolfberry (the fruit of Lycium barbarum), consisting of di-phenylpropionyl spermidines and their glucosides. While the molecular basis underlying their glycodiversity was clarified in our previous work, the biosynthesis of di-phenylpropionyl spermidine core structure remains elusive. In particular, the acyltransferase responsible for conjugating dihydrocaffeoyl, one of the dominant phenylpropionyl moieties, is still unidentified. Herein, two N-hydroxycinnamoyltransferases (LbSCT1/2) from wolfberry were identified, which not only catalyze the conjugation of spermidine with caffeoyl-CoA, but also exhibit high catalytic activity toward dihydrocaffeoyl-CoA. Notably, LbSCT2 catalyzes monoacylation, whereas LbSCT1 enables sequential diacylation. Together with caffeoyl-CoA double bond reductase (LbDBR2), LbSCT1/2 accomplish the biosynthesis of lycibarbarspermidine Ⅰ-Ⅳ. Furthermore, LbSCT1 efficiently catalyzes the biosynthesis of kukoamine B, a major bioactive component from Lycii Cortex (the root bark of Lycium species). Crystal structural and mutagenic investigations elucidated the catalytic mechanisms underlying the selectivity of LbSCT1/2 for spermidine mono- and diacylation. This study establishes the complete biosynthesis of lycibarbarspermidines and provides valuable enzymatic tools for diversifying phenylpropionyl compounds.
2026, 37(9): 112824
doi: 10.1016/j.cclet.2026.112824
Abstract:
The direct hydroalkenylation of alkenes represents the most straightforward method for constructing C(sp2)-C(sp3) bonds. However, controlling chemo- and regioselectivity between two different alkenes remains a fundamental challenge. Herein, we developed a cobalt-catalyzed system to regioselectively ligate electron-deficient alkenes with electron-rich alkenes. The in-situ generated CoⅢ-H activate electron-deficient alkenes through a Markovnikov or anti-Markovnikov manner, to form linear or branched alkylcobalt species as key intermediate, which can successfully achieve regiodivergent hydroalkenylation of acrylates and analogs. The method demonstrates a broad substrate scope and functional group compatibility. Origin of regioselectivity control by the cobalt catalyst has been elucidated through mechanistic studies and density functional theory (DFT) calculations.
The direct hydroalkenylation of alkenes represents the most straightforward method for constructing C(sp2)-C(sp3) bonds. However, controlling chemo- and regioselectivity between two different alkenes remains a fundamental challenge. Herein, we developed a cobalt-catalyzed system to regioselectively ligate electron-deficient alkenes with electron-rich alkenes. The in-situ generated CoⅢ-H activate electron-deficient alkenes through a Markovnikov or anti-Markovnikov manner, to form linear or branched alkylcobalt species as key intermediate, which can successfully achieve regiodivergent hydroalkenylation of acrylates and analogs. The method demonstrates a broad substrate scope and functional group compatibility. Origin of regioselectivity control by the cobalt catalyst has been elucidated through mechanistic studies and density functional theory (DFT) calculations.
2026, 37(9): 112846
doi: 10.1016/j.cclet.2026.112846
Abstract:
Pancreatic cancer (PCa) is highly aggressive and resistant to conventional therapies due to its dense stroma and immunosuppressive microenvironment. To overcome these barriers, we engineered dextran-coated copper peroxide-doxorubicin nanoclusters (DCPD NCs) that enabled ultrasound (US)-augmented chemodynamic therapy (CDT) and chemotherapy. In the acidic tumor microenvironment, DCPD NCs disassemble and co-release Cu2+, doxorubicin, and self-supplied H2O2. Cu2+ depletes glutathione (GSH) and catalyzes H2O2 to generate •OH with US (1.5 fold higher than that without US). Under US treatment, DCPD NCs not only increased the permeability of Panc02 tumor spheroids, but also increased intracellular reactive oxygen species by 2.1 times, depleted GSH by up to 25.2%, and induced lipid peroxidation. This nanoplatform works synergistically to induce potent immunogenic cell death. In both subcutaneous and orthotopic PCa mice models, this nanoplatform demonstrated remarkable therapeutic effects. The tumor weights of mice treated with DCPD NCs + US were significantly reduced by 91.8% and 85.7% vs. controls, with robust calreticulin (CRT) exposure and HMGB1 translocation in tumors. This work establishes an US augmented and self-reinforcing nanoplatform that overcomes stromal and metabolic barriers in PCa, providing a synergistic strategy for catalytic immunotherapy.
Pancreatic cancer (PCa) is highly aggressive and resistant to conventional therapies due to its dense stroma and immunosuppressive microenvironment. To overcome these barriers, we engineered dextran-coated copper peroxide-doxorubicin nanoclusters (DCPD NCs) that enabled ultrasound (US)-augmented chemodynamic therapy (CDT) and chemotherapy. In the acidic tumor microenvironment, DCPD NCs disassemble and co-release Cu2+, doxorubicin, and self-supplied H2O2. Cu2+ depletes glutathione (GSH) and catalyzes H2O2 to generate •OH with US (1.5 fold higher than that without US). Under US treatment, DCPD NCs not only increased the permeability of Panc02 tumor spheroids, but also increased intracellular reactive oxygen species by 2.1 times, depleted GSH by up to 25.2%, and induced lipid peroxidation. This nanoplatform works synergistically to induce potent immunogenic cell death. In both subcutaneous and orthotopic PCa mice models, this nanoplatform demonstrated remarkable therapeutic effects. The tumor weights of mice treated with DCPD NCs + US were significantly reduced by 91.8% and 85.7% vs. controls, with robust calreticulin (CRT) exposure and HMGB1 translocation in tumors. This work establishes an US augmented and self-reinforcing nanoplatform that overcomes stromal and metabolic barriers in PCa, providing a synergistic strategy for catalytic immunotherapy.
2026, 37(9): 112945
doi: 10.1016/j.cclet.2026.112945
Abstract:
Seawater electrolysis, utilizing coastal resources, holds great promise as a sustainable method for hydrogen production. However, the efficiency of seawater electrolysis is limited by anode catalysts with high overpotentials (η) and short lifespans, due to chloride-induced side reactions. In this study, we introduce sodium alginate (SA) modified NiFe layered double hydroxide nanosheets on Ni foam (SA@NiFe LDH/NF) as a highly efficient and stable electrocatalyst for long-term alkaline seawater oxidation. Our SA@NiFe LDH/NF needs a low η of 362 mV to reach 1000 mA/cm2, outperforming the unmodified NiFe LDH/NF (425 mV). Furthermore, it maintains continuous electrolysis for 1600 h at current densities of 500 and 1000 mA/cm2. In situ Raman spectroscopy reveals that the SA protective layer not only facilitates NiOOH formation but also establishes a dense electrostatic network via carboxyl groups, which repels chloride ions and ensures stable seawater oxidation. This work presents a promising strategy for developing durable, high-performance anodes and highlights the potential of natural polysaccharide coatings for enhancing anode corrosion resistance during the seawater electrolysis process.
Seawater electrolysis, utilizing coastal resources, holds great promise as a sustainable method for hydrogen production. However, the efficiency of seawater electrolysis is limited by anode catalysts with high overpotentials (η) and short lifespans, due to chloride-induced side reactions. In this study, we introduce sodium alginate (SA) modified NiFe layered double hydroxide nanosheets on Ni foam (SA@NiFe LDH/NF) as a highly efficient and stable electrocatalyst for long-term alkaline seawater oxidation. Our SA@NiFe LDH/NF needs a low η of 362 mV to reach 1000 mA/cm2, outperforming the unmodified NiFe LDH/NF (425 mV). Furthermore, it maintains continuous electrolysis for 1600 h at current densities of 500 and 1000 mA/cm2. In situ Raman spectroscopy reveals that the SA protective layer not only facilitates NiOOH formation but also establishes a dense electrostatic network via carboxyl groups, which repels chloride ions and ensures stable seawater oxidation. This work presents a promising strategy for developing durable, high-performance anodes and highlights the potential of natural polysaccharide coatings for enhancing anode corrosion resistance during the seawater electrolysis process.
2026, 37(9): 111387
doi: 10.1016/j.cclet.2025.111387
Abstract:
Solid-state zinc-air batteries (SZABs) and solid-state zinc-ion batteries (SZIBs) exhibit significant potential for applications in flexible electronic devices, due to zinc's abundance, enhanced safety, high theoretical energy density, and eco-friendliness. Recently, various SZABs and SZIBs utilizing advanced solid-state electrolytes (SEs) and cathodes have been developed. However, the conductivity of the cathode, as well as the construction of active sites and ion transport pathways during charging and discharging, require further investigation. Additionally, the electrolyte plays a critical role in solid-state batteries, directly impacting the output performance of the battery, cycling stability, and operational lifespan. Thus, the development of high-quality electrolytes alongside efficient and stable electrodes is essential for the large-scale application of solid-state batteries. This review examines the working principles and assembly processes of SZABs and SZIBs and summarizes the superior properties of various cathodes and electrolytes, thereby offering new perspectives for advancing high-performance SZABs and SZIBs.
Solid-state zinc-air batteries (SZABs) and solid-state zinc-ion batteries (SZIBs) exhibit significant potential for applications in flexible electronic devices, due to zinc's abundance, enhanced safety, high theoretical energy density, and eco-friendliness. Recently, various SZABs and SZIBs utilizing advanced solid-state electrolytes (SEs) and cathodes have been developed. However, the conductivity of the cathode, as well as the construction of active sites and ion transport pathways during charging and discharging, require further investigation. Additionally, the electrolyte plays a critical role in solid-state batteries, directly impacting the output performance of the battery, cycling stability, and operational lifespan. Thus, the development of high-quality electrolytes alongside efficient and stable electrodes is essential for the large-scale application of solid-state batteries. This review examines the working principles and assembly processes of SZABs and SZIBs and summarizes the superior properties of various cathodes and electrolytes, thereby offering new perspectives for advancing high-performance SZABs and SZIBs.
2026, 37(9): 111389
doi: 10.1016/j.cclet.2025.111389
Abstract:
Piezoelectric materials can efficiently convert widely available mechanical energy to usable electrical energy or chemical energy, which represent a type of promising sustainable materials and is worth being extensively explored. Covalent organic frameworks (COFs), with their finely tunable structures and properties, have emerged as exciting materials for piezoelectric applications. This review aims to discuss the strategy for enhanced piezoelectric properties of COFs and the applications of COFs in the piezoelectric field, including piezocatalysis and piezoelectric nanogenerators. Then, the effect of pressure on the structure of COFs is introduced, which may provide new perspectives for the design of COFs in piezoelectricity. The review concludes that COFs offer a versatile platform for developing advanced piezoelectric materials, with potential in wide range of applications. The insights provided in this review are hoped to guide the direction of future research in the field of COF-based piezoelectric materials.
Piezoelectric materials can efficiently convert widely available mechanical energy to usable electrical energy or chemical energy, which represent a type of promising sustainable materials and is worth being extensively explored. Covalent organic frameworks (COFs), with their finely tunable structures and properties, have emerged as exciting materials for piezoelectric applications. This review aims to discuss the strategy for enhanced piezoelectric properties of COFs and the applications of COFs in the piezoelectric field, including piezocatalysis and piezoelectric nanogenerators. Then, the effect of pressure on the structure of COFs is introduced, which may provide new perspectives for the design of COFs in piezoelectricity. The review concludes that COFs offer a versatile platform for developing advanced piezoelectric materials, with potential in wide range of applications. The insights provided in this review are hoped to guide the direction of future research in the field of COF-based piezoelectric materials.
2026, 37(9): 111489
doi: 10.1016/j.cclet.2025.111489
Abstract:
MXene and metal-organic frame (MOFs) are emerging as transformative materials in the field of energy storage and conversion. While MXene excel in conductivity, tunable surface chemistry, and flexibility, MOFs bring complementary benefits with their tunable porosity and structural versatility, enabling the design of hybrid systems with enhanced functionalities. However, challenges such as material stability, structural integrity, and ink formulation must be addressed to fully integrate these materials into 3D printing technologies. This review elucidates cutting-edge material design frameworks for MXene- and MOF-integrated 3D-printed architectures, emphasizing their transformative roles in advancing energy storage/conversion systems. We provide a systematic evaluation of additive manufacturing compatibility and multidisciplinary optimization strategies spanning ink rheology, hierarchical structure engineering, and interfacial electrochemistry to enhance device performance metrics. Additionally, by analyzing the key advantages and limitations of MXene- and MOF-based materials, we examine their role in overcoming current challenges in electrochemical energy storage devices. Finally, we provide insights into future prospects, presenting a roadmap for integrating MXene and MOFs into scalable 3D printing technologies, which will enable breakthroughs in sustainable and high-performance energy devices.
MXene and metal-organic frame (MOFs) are emerging as transformative materials in the field of energy storage and conversion. While MXene excel in conductivity, tunable surface chemistry, and flexibility, MOFs bring complementary benefits with their tunable porosity and structural versatility, enabling the design of hybrid systems with enhanced functionalities. However, challenges such as material stability, structural integrity, and ink formulation must be addressed to fully integrate these materials into 3D printing technologies. This review elucidates cutting-edge material design frameworks for MXene- and MOF-integrated 3D-printed architectures, emphasizing their transformative roles in advancing energy storage/conversion systems. We provide a systematic evaluation of additive manufacturing compatibility and multidisciplinary optimization strategies spanning ink rheology, hierarchical structure engineering, and interfacial electrochemistry to enhance device performance metrics. Additionally, by analyzing the key advantages and limitations of MXene- and MOF-based materials, we examine their role in overcoming current challenges in electrochemical energy storage devices. Finally, we provide insights into future prospects, presenting a roadmap for integrating MXene and MOFs into scalable 3D printing technologies, which will enable breakthroughs in sustainable and high-performance energy devices.
2026, 37(9): 111865
doi: 10.1016/j.cclet.2025.111865
Abstract:
Molecular oxygen (O2) activation offers a sustainable pathway for environmental remediation by generating reactive oxygen species (ROS), yet challenges in efficiency, stability, and scalability hinder its practical application. This review systematically explores recent advances in integrated (photo)electrocatalytic systems, where synergistic coupling of photonic and electrical energy inputs overcomes spin-forbidden barriers in molecular O2 activation. Emphasis is placed on nanoscale catalyst engineering, including alloy, carbon-based materials, and single-atom catalysts, to precisely regulate ROS generation via electronic structure design and targeted electron transfer. Parallel innovations in reactor design, such as flow-by and flow-through (photo)electrodes, are analyzed for their role in enhancing mass transport, increasing ROS yields, and ensuring operational durability. Integrating fundamental insights with system engineering, the review provides a roadmap for advancing energy-efficient (photo)electrocatalytic platforms, highlighting their transformative potential in ROS-mediated environmental technologies.
Molecular oxygen (O2) activation offers a sustainable pathway for environmental remediation by generating reactive oxygen species (ROS), yet challenges in efficiency, stability, and scalability hinder its practical application. This review systematically explores recent advances in integrated (photo)electrocatalytic systems, where synergistic coupling of photonic and electrical energy inputs overcomes spin-forbidden barriers in molecular O2 activation. Emphasis is placed on nanoscale catalyst engineering, including alloy, carbon-based materials, and single-atom catalysts, to precisely regulate ROS generation via electronic structure design and targeted electron transfer. Parallel innovations in reactor design, such as flow-by and flow-through (photo)electrodes, are analyzed for their role in enhancing mass transport, increasing ROS yields, and ensuring operational durability. Integrating fundamental insights with system engineering, the review provides a roadmap for advancing energy-efficient (photo)electrocatalytic platforms, highlighting their transformative potential in ROS-mediated environmental technologies.
2026, 37(9): 111888
doi: 10.1016/j.cclet.2025.111888
Abstract:
The active ingredients components of traditional Chinese medicine (TCM) can naturally create supramolecular structures like nanoparticles and micelles with well-defined functions through a dynamic assembly mechanism driven by noncovalent bonding interactions. In recent years, numerous studies have found that the supramolecular self-assemblies of TCM, which are also known as Chinese medicine supramolecules (CMS), exhibit better efficacy, higher bioavailability, and synergistic effects. In vivo fate analysis is a roadblock to revealing the active mechanisms of CMS. This review focuses on the in vivo dynamic biological fate of herbal self-assemblies and systematically elucidates their delivery characteristics in absorption barrier penetration, biofilm transport, and tissue-specific distribution. Meanwhile, this review summarizes the progress in applying cutting-edge detection techniques for tracking supramolecular behavior in vivo, including fluorescent labeling, isotope tracing, and multimodal imaging. By summarizing the existing research results, we aim to construct a systematic research framework for the in vivo behaviors of Chinese medicine self-assemblies and explore feasible analysis paths for Chinese medicine formulations.
The active ingredients components of traditional Chinese medicine (TCM) can naturally create supramolecular structures like nanoparticles and micelles with well-defined functions through a dynamic assembly mechanism driven by noncovalent bonding interactions. In recent years, numerous studies have found that the supramolecular self-assemblies of TCM, which are also known as Chinese medicine supramolecules (CMS), exhibit better efficacy, higher bioavailability, and synergistic effects. In vivo fate analysis is a roadblock to revealing the active mechanisms of CMS. This review focuses on the in vivo dynamic biological fate of herbal self-assemblies and systematically elucidates their delivery characteristics in absorption barrier penetration, biofilm transport, and tissue-specific distribution. Meanwhile, this review summarizes the progress in applying cutting-edge detection techniques for tracking supramolecular behavior in vivo, including fluorescent labeling, isotope tracing, and multimodal imaging. By summarizing the existing research results, we aim to construct a systematic research framework for the in vivo behaviors of Chinese medicine self-assemblies and explore feasible analysis paths for Chinese medicine formulations.
2026, 37(9): 111900
doi: 10.1016/j.cclet.2025.111900
Abstract:
The pervasive inflammatory response orchestrates every stage of tumor initiation and progression, not only serving as a catalyst for tumorigenesis but also as a nurturing environment for malignant growth. Within this intricate microenvironment teeming with cancer cells, immune cells, and stromal cells, a continuous exchange of inflammatory signals mediated by exosomes, small membrane-bound vesicles guide the development of the proinflammatory tumor microenvironment (TME). In this review, we delve into the intricate dialogue mechanisms among tumor cells, resident immune cells and stromal cells, scrutinizing the roles of exosomes derived from both tumor cells and other resident cells in shaping the inflammatory milieu. Anti-tumor therapies harnessing the diverse compositions and effects of exosomes have unveiled novel strategies for combating tumor malignancy.
The pervasive inflammatory response orchestrates every stage of tumor initiation and progression, not only serving as a catalyst for tumorigenesis but also as a nurturing environment for malignant growth. Within this intricate microenvironment teeming with cancer cells, immune cells, and stromal cells, a continuous exchange of inflammatory signals mediated by exosomes, small membrane-bound vesicles guide the development of the proinflammatory tumor microenvironment (TME). In this review, we delve into the intricate dialogue mechanisms among tumor cells, resident immune cells and stromal cells, scrutinizing the roles of exosomes derived from both tumor cells and other resident cells in shaping the inflammatory milieu. Anti-tumor therapies harnessing the diverse compositions and effects of exosomes have unveiled novel strategies for combating tumor malignancy.
2026, 37(9): 111956
doi: 10.1016/j.cclet.2025.111956
Abstract:
Breast cancer (BRCA) is a multifaceted and extremely diverse condition, with conventional diagnostic and therapeutic methods encountering considerable obstacles. With the increasing amount of medical data and the ongoing development of computer technologies, artificial intelligence (AI) has become widely used in BRCA medication research and clinical decision-making. Specifically, AI helps anticipate therapy responses, makes it easier to choose the best treatment regimens based on the molecular and pathological features of tumors, and allows for more accurate risk assessments for BRCA. AI is also essential to drug development, including the identification and prediction of novel therapeutic targets, the screening and prediction of compound structures, the repurposing of existing drugs, and the creation of combination treatments. From static assessments based on molecular subtypes to dynamic tracking of disease development, AI’s role in BRCA diagnosis and therapy has changed throughout time. It has transitioned from experience-based therapeutic approaches to data-driven clinical decision-making. In addition to improving patients’ quality of life, this shift is essential to turning cancer therapy into a "prevention-prediction-personalized" paradigm. This review article thoroughly examines the developments in AI applications for important fields such as molecular subtype identification, metastasis and recurrence prediction, BRCA risk stratification, and the creation of new medications. It delves deeper into current technological constraints and clinical translation pathways, emphasizing the need for advances in clinical applicability and technical standardization through tactics like large-scale multi-center clinical trials, innovative cross-modal data integration, and algorithmic architecture optimization.
Breast cancer (BRCA) is a multifaceted and extremely diverse condition, with conventional diagnostic and therapeutic methods encountering considerable obstacles. With the increasing amount of medical data and the ongoing development of computer technologies, artificial intelligence (AI) has become widely used in BRCA medication research and clinical decision-making. Specifically, AI helps anticipate therapy responses, makes it easier to choose the best treatment regimens based on the molecular and pathological features of tumors, and allows for more accurate risk assessments for BRCA. AI is also essential to drug development, including the identification and prediction of novel therapeutic targets, the screening and prediction of compound structures, the repurposing of existing drugs, and the creation of combination treatments. From static assessments based on molecular subtypes to dynamic tracking of disease development, AI’s role in BRCA diagnosis and therapy has changed throughout time. It has transitioned from experience-based therapeutic approaches to data-driven clinical decision-making. In addition to improving patients’ quality of life, this shift is essential to turning cancer therapy into a "prevention-prediction-personalized" paradigm. This review article thoroughly examines the developments in AI applications for important fields such as molecular subtype identification, metastasis and recurrence prediction, BRCA risk stratification, and the creation of new medications. It delves deeper into current technological constraints and clinical translation pathways, emphasizing the need for advances in clinical applicability and technical standardization through tactics like large-scale multi-center clinical trials, innovative cross-modal data integration, and algorithmic architecture optimization.
2026, 37(9): 111969
doi: 10.1016/j.cclet.2025.111969
Abstract:
Glycopolymers with a brush architecture that are immobilized on material surfaces can mimic the natural glycoconjugates found on cell surfaces, with potential biomedical applications including antimicrobial, anticoagulation, anti-nonspecific adhesion, cellular communication and protein purification. To facilitate the clinical translation and applications of glyco-engineered materials, it is essential to achieve a comprehensive understanding of synthetic strategies and surface-immobilization techniques from a holistic perspective. This review highlights recent advances in the covalent immobilization of glycopolymer chains onto materials through methods like surface-initiated polymerization and interfacial coupling reactions. It provides a detailed summary of the synthetic routes for reactive glycopolymers and interfaces, as well as the technologies used for immobilization on various surfaces, including plastics, metals, silica materials, carbon materials, and living cells. The challenges and opportunities for the future development of glycopolymer-engineered materials and interfaces are also discussed. We believe that this review can serve as a valuable resource for researchers interested in the interdisciplinary field of glycoscience and materials.
Glycopolymers with a brush architecture that are immobilized on material surfaces can mimic the natural glycoconjugates found on cell surfaces, with potential biomedical applications including antimicrobial, anticoagulation, anti-nonspecific adhesion, cellular communication and protein purification. To facilitate the clinical translation and applications of glyco-engineered materials, it is essential to achieve a comprehensive understanding of synthetic strategies and surface-immobilization techniques from a holistic perspective. This review highlights recent advances in the covalent immobilization of glycopolymer chains onto materials through methods like surface-initiated polymerization and interfacial coupling reactions. It provides a detailed summary of the synthetic routes for reactive glycopolymers and interfaces, as well as the technologies used for immobilization on various surfaces, including plastics, metals, silica materials, carbon materials, and living cells. The challenges and opportunities for the future development of glycopolymer-engineered materials and interfaces are also discussed. We believe that this review can serve as a valuable resource for researchers interested in the interdisciplinary field of glycoscience and materials.
2026, 37(9): 111983
doi: 10.1016/j.cclet.2025.111983
Abstract:
Venous thrombosis (VT) is defined by the formation of a blood clot within a vein, leading to partial or complete obstruction of blood flow. This condition may result in severe sequelae, including chronic thromboembolic pulmonary hypertension and post-thrombotic syndrome. As a multifactorial and episodic disorder, VT constitutes a significant contributor to global morbidity and mortality. In this review, we first seek to provide a comprehensive understanding of the intricate pathophysiological mechanisms underlying VT. Next, the diagnostic challenges posed by the nonspecific nature of clinical signs and symptoms were explored, offering an overview of current strategies aimed at enhancing diagnostic accuracy. Furthermore, treatment modalities for VT, primarily consisting of anticoagulation therapy, along with thrombolysis or surgical intervention when indicated, are discussed in detail. Considering the urgent need for safer and more effective therapeutic options, the development of nanoparticle-based drug delivery systems (DDS) capable of specific sites of thrombosis is crucial. Thus, this review further examines recent advancements in DDS for the treatment of VT. Finally, we will evaluate the prospects and significant challenges currently facing the field, offering a comprehensive overview of the research and treatment of VT.
Venous thrombosis (VT) is defined by the formation of a blood clot within a vein, leading to partial or complete obstruction of blood flow. This condition may result in severe sequelae, including chronic thromboembolic pulmonary hypertension and post-thrombotic syndrome. As a multifactorial and episodic disorder, VT constitutes a significant contributor to global morbidity and mortality. In this review, we first seek to provide a comprehensive understanding of the intricate pathophysiological mechanisms underlying VT. Next, the diagnostic challenges posed by the nonspecific nature of clinical signs and symptoms were explored, offering an overview of current strategies aimed at enhancing diagnostic accuracy. Furthermore, treatment modalities for VT, primarily consisting of anticoagulation therapy, along with thrombolysis or surgical intervention when indicated, are discussed in detail. Considering the urgent need for safer and more effective therapeutic options, the development of nanoparticle-based drug delivery systems (DDS) capable of specific sites of thrombosis is crucial. Thus, this review further examines recent advancements in DDS for the treatment of VT. Finally, we will evaluate the prospects and significant challenges currently facing the field, offering a comprehensive overview of the research and treatment of VT.
2026, 37(9): 111993
doi: 10.1016/j.cclet.2025.111993
Abstract:
Lymph nodes (LNs), as specialized secondary lymphoid organs with highly organized micro-architecture containing various immune cells, play a pivotal role in antigen presentation and immune cell activation. Compared to traditional immunotherapy delivery methods, LN-targeted delivery demonstrates greater effectiveness in modulating the immunosuppressive environment within tumor-draining lymph nodes (TDLNs), thereby activating anti-cancer immunity, and reducing potential systemic side effects. This review summarizes various types of LN-targeted nanoparticles (NPs) and factors influencing targeting efficiency as well as outlining recent advances in LN-targeted immunotherapeutic agents. It is expected that this review will provide a comprehensive understanding of the current research landscape and emerging trends in this field, offering guidance for future studies.
Lymph nodes (LNs), as specialized secondary lymphoid organs with highly organized micro-architecture containing various immune cells, play a pivotal role in antigen presentation and immune cell activation. Compared to traditional immunotherapy delivery methods, LN-targeted delivery demonstrates greater effectiveness in modulating the immunosuppressive environment within tumor-draining lymph nodes (TDLNs), thereby activating anti-cancer immunity, and reducing potential systemic side effects. This review summarizes various types of LN-targeted nanoparticles (NPs) and factors influencing targeting efficiency as well as outlining recent advances in LN-targeted immunotherapeutic agents. It is expected that this review will provide a comprehensive understanding of the current research landscape and emerging trends in this field, offering guidance for future studies.
2026, 37(9): 112030
doi: 10.1016/j.cclet.2025.112030
Abstract:
Paper and ink serve as important media for cultural inheritance and information transmission. With the development of civilization, the research on functional paper and ink has gradually gained attention. Carbon dots (CDs) have attracted widespread interest due to their excellent photoluminescence (PL) properties, strong ultraviolet (UV) absorption, electrical characteristics, and stability. This review summarizes the functionalization applications of CDs in ink and paper, and their applications progress in paper-based cultural relics conservation. To begin, the preparation methods of CDs are introduced. Subsequently, the PL, light absorption mechanisms, and electrical properties of CDs are discussed from the perspective of structure and classification. Then, we discuss the functional applications of CDs with unique optical or electrical properties in paper and ink, and also present the research progress of CDs in the field of paper conservation. Finally, the research development and potential challenges of CDs are presented. It is believed that in the near future, more properties of CDs will be developed, paving the way for the protection, development, and commercialization of paper and ink materials.
Paper and ink serve as important media for cultural inheritance and information transmission. With the development of civilization, the research on functional paper and ink has gradually gained attention. Carbon dots (CDs) have attracted widespread interest due to their excellent photoluminescence (PL) properties, strong ultraviolet (UV) absorption, electrical characteristics, and stability. This review summarizes the functionalization applications of CDs in ink and paper, and their applications progress in paper-based cultural relics conservation. To begin, the preparation methods of CDs are introduced. Subsequently, the PL, light absorption mechanisms, and electrical properties of CDs are discussed from the perspective of structure and classification. Then, we discuss the functional applications of CDs with unique optical or electrical properties in paper and ink, and also present the research progress of CDs in the field of paper conservation. Finally, the research development and potential challenges of CDs are presented. It is believed that in the near future, more properties of CDs will be developed, paving the way for the protection, development, and commercialization of paper and ink materials.
2026, 37(9): 112058
doi: 10.1016/j.cclet.2025.112058
Abstract:
Probiotics encompass a diverse assortment of biological activities and are widely distributed in barrier organs, which enables them to dynamically modulate multiple physiological processes within the human body. Due to their diminished side effects, a spectrum of probiotic-centric functional formulations has been used as an alternative to traditional anti-inflammatory drugs. Nonetheless, probiotics are intrinsically sensitive to environmental fluctuations, which greatly limits their therapeutic effectiveness. The specific combination of probiotics with nanozymes opens up novel perspectives for resolving this issue. Nanozymes are nanomaterials that exhibit enzyme-like properties, showcasing exceptional catalytic prowess while retaining the distinctive attributes of nanomaterials. The alliance of nanozymes and probiotics demonstrates a significant synergistic effect in the treatment of diseases. On one hand, inherent targeting and metabolic properties of probiotics impart nanozymes with site-selectivity, alongside the capacity to fine-tune the catalytic microenvironment for optimized activity. On the other hand, nanozymes exhibit exceptional catalytic properties that can be leveraged to safeguard probiotics and concurrently bestow new bioactivities, thereby enhancing their therapeutic efficacy. This review underscores the therapeutic potential of nanozyme-enhanced probiotics in regulating reactive oxygen species for the synergetic therapy of various diseases, as well as the challenges associated with the biosafety of such biomimetic functional agents.
Probiotics encompass a diverse assortment of biological activities and are widely distributed in barrier organs, which enables them to dynamically modulate multiple physiological processes within the human body. Due to their diminished side effects, a spectrum of probiotic-centric functional formulations has been used as an alternative to traditional anti-inflammatory drugs. Nonetheless, probiotics are intrinsically sensitive to environmental fluctuations, which greatly limits their therapeutic effectiveness. The specific combination of probiotics with nanozymes opens up novel perspectives for resolving this issue. Nanozymes are nanomaterials that exhibit enzyme-like properties, showcasing exceptional catalytic prowess while retaining the distinctive attributes of nanomaterials. The alliance of nanozymes and probiotics demonstrates a significant synergistic effect in the treatment of diseases. On one hand, inherent targeting and metabolic properties of probiotics impart nanozymes with site-selectivity, alongside the capacity to fine-tune the catalytic microenvironment for optimized activity. On the other hand, nanozymes exhibit exceptional catalytic properties that can be leveraged to safeguard probiotics and concurrently bestow new bioactivities, thereby enhancing their therapeutic efficacy. This review underscores the therapeutic potential of nanozyme-enhanced probiotics in regulating reactive oxygen species for the synergetic therapy of various diseases, as well as the challenges associated with the biosafety of such biomimetic functional agents.
2026, 37(9): 112059
doi: 10.1016/j.cclet.2025.112059
Abstract:
Lipid-based vaccines, such as liposomes, emulsions, and lipid nanoparticles, play a key role in the development of antiviral vaccines due to their unique immunomodulatory properties, capacity to serve as antigen depots, ability to protect antigens, and adjuvant effect. Among the various approved vaccines, the vast majority utilize lipid-based adjuvants and delivery systems, such as AS01, AS03, MF59, and BNT162b2. These formulations establish an inflammatory microenvironment at the injection site, recruit immune cells, and activate innate immune pathways, thereby enhancing the immunogenicity of the antigen. Concurrently, they protect antigens from enzymatic degradation and thereby maintain the stability of antigens. This review comprehensively summarizes approved lipid-based antiviral vaccines, encompassing their composition, structure, and underlying immunological mechanisms. Furthermore, it outlines emerging trends in the development of diverse lipid-based vaccine platforms, including strategies to enhance antigen loading capacity, achieve more precise targeting of antigen-presenting cells, and implement novel combinatorial approaches involving multi-platform and multi-pathway strategies. Finally, the review addresses the prevalent challenges, future development directions, industrial-scale manufacturing considerations, and quality control requirements for lipid-based vaccines, with the aim of advancing this promising field.
Lipid-based vaccines, such as liposomes, emulsions, and lipid nanoparticles, play a key role in the development of antiviral vaccines due to their unique immunomodulatory properties, capacity to serve as antigen depots, ability to protect antigens, and adjuvant effect. Among the various approved vaccines, the vast majority utilize lipid-based adjuvants and delivery systems, such as AS01, AS03, MF59, and BNT162b2. These formulations establish an inflammatory microenvironment at the injection site, recruit immune cells, and activate innate immune pathways, thereby enhancing the immunogenicity of the antigen. Concurrently, they protect antigens from enzymatic degradation and thereby maintain the stability of antigens. This review comprehensively summarizes approved lipid-based antiviral vaccines, encompassing their composition, structure, and underlying immunological mechanisms. Furthermore, it outlines emerging trends in the development of diverse lipid-based vaccine platforms, including strategies to enhance antigen loading capacity, achieve more precise targeting of antigen-presenting cells, and implement novel combinatorial approaches involving multi-platform and multi-pathway strategies. Finally, the review addresses the prevalent challenges, future development directions, industrial-scale manufacturing considerations, and quality control requirements for lipid-based vaccines, with the aim of advancing this promising field.
2026, 37(9): 112062
doi: 10.1016/j.cclet.2025.112062
Abstract:
Ocular diseases are the main cause of vision loss and even blindness, with treatments including topical medications (such as eye drops), intravitreal injections, and surgery. However, the eye’s complex anatomical structure and physiological barriers significantly limit drug bioavailability, affecting therapeutic efficacy. Nanomaterials have shown promise in ophthalmic drug delivery due to their unique properties. Nanomaterials can effectively penetrate ocular barriers to enhance drug permeability and bioavailability. Their ocular penetration can be further optimized by regulating nanoparticle (NP) size and surface properties, thereby prolonging drug residence time on the ocular surface and reducing administration frequency. Additionally, as controlled-release carriers, they enable sustained drug release to extend therapeutic duration and improve treatment efficacy. In addition, some nanomaterials also possess biological activities such as antioxidant, antibacterial and anti-inflammatory, making them a promising therapeutic strategy. This review focuses on the advances in nanomaterials application for ocular diseases, summarizes the mechanisms underlying nanomaterial-based drug delivery, and discusses the current challenges and future research directions, with the aim of providing new insights into the clinical application and translation of nanomaterials in ophthalmology.
Ocular diseases are the main cause of vision loss and even blindness, with treatments including topical medications (such as eye drops), intravitreal injections, and surgery. However, the eye’s complex anatomical structure and physiological barriers significantly limit drug bioavailability, affecting therapeutic efficacy. Nanomaterials have shown promise in ophthalmic drug delivery due to their unique properties. Nanomaterials can effectively penetrate ocular barriers to enhance drug permeability and bioavailability. Their ocular penetration can be further optimized by regulating nanoparticle (NP) size and surface properties, thereby prolonging drug residence time on the ocular surface and reducing administration frequency. Additionally, as controlled-release carriers, they enable sustained drug release to extend therapeutic duration and improve treatment efficacy. In addition, some nanomaterials also possess biological activities such as antioxidant, antibacterial and anti-inflammatory, making them a promising therapeutic strategy. This review focuses on the advances in nanomaterials application for ocular diseases, summarizes the mechanisms underlying nanomaterial-based drug delivery, and discusses the current challenges and future research directions, with the aim of providing new insights into the clinical application and translation of nanomaterials in ophthalmology.
2026, 37(9): 112203
doi: 10.1016/j.cclet.2025.112203
Abstract:
Palladium catalysis is regarded as a significant tool for the construction of carbon-carbon and carbon-heteroatom bond in organic synthesis. Thus the sustainable development of this type of transformations, especially designing properly, clean chemical technology, is of great importance. Recently, water as a reaction medium has been developed in both academic laboratories and in the industry, improving the reaction activity and selectivity of the organic reaction through its own properties (such as polarity, high dielectric constant). This review focuses on palladium-catalysed organic synthesis using water as solvent, summarizing relevant articles published from 2015 to 2025. Meanwhile, mechanistic studies, supported by experimental investigations, are thoroughly reviewed to elucidate the interplay between water and palladium species in facilitating bond-forming processes. Furthermore, practical applications of these aqueous-phase methodologies in the synthesis of complex natural products and pharmaceutical intermediates are showcased, underscoring their potential for scalable and sustainable chemical manufacturing.
Palladium catalysis is regarded as a significant tool for the construction of carbon-carbon and carbon-heteroatom bond in organic synthesis. Thus the sustainable development of this type of transformations, especially designing properly, clean chemical technology, is of great importance. Recently, water as a reaction medium has been developed in both academic laboratories and in the industry, improving the reaction activity and selectivity of the organic reaction through its own properties (such as polarity, high dielectric constant). This review focuses on palladium-catalysed organic synthesis using water as solvent, summarizing relevant articles published from 2015 to 2025. Meanwhile, mechanistic studies, supported by experimental investigations, are thoroughly reviewed to elucidate the interplay between water and palladium species in facilitating bond-forming processes. Furthermore, practical applications of these aqueous-phase methodologies in the synthesis of complex natural products and pharmaceutical intermediates are showcased, underscoring their potential for scalable and sustainable chemical manufacturing.
2026, 37(9): 112408
doi: 10.1016/j.cclet.2026.112408
Abstract:
Direct methanol fuel cell (DMFC) is a clean energy technology that integrates high-efficiency energy conversion with environmental benefits. However, its industrial application is hindered by the sluggish kinetics of the cathode oxygen reduction reaction (ORR). This key scientific challenge has driven diversified advances in high-performance ORR electrocatalysts. This review systematically outlines the reaction mechanisms and ORR pathways in DMFC. Furthermore, it comprehensively summarizes recent advances in multi-scale modification strategies, including methanol tolerance optimization, rational design of active sites, electronic structure tailoring, surface/interface micro-environment engineering, and additional modulation approaches for enhancing ORR performance. Additionally, the mechanisms for enhancing intrinsic catalytic activity are discussed in depth, along with the elucidation of the structure-activity relationship governing catalyst performance in terms of activity, selectivity, and stability. Finally, in light of the critical challenges currently facing DMFC cathode catalysts, future directions and development pathways for catalyst design are proposed.
Direct methanol fuel cell (DMFC) is a clean energy technology that integrates high-efficiency energy conversion with environmental benefits. However, its industrial application is hindered by the sluggish kinetics of the cathode oxygen reduction reaction (ORR). This key scientific challenge has driven diversified advances in high-performance ORR electrocatalysts. This review systematically outlines the reaction mechanisms and ORR pathways in DMFC. Furthermore, it comprehensively summarizes recent advances in multi-scale modification strategies, including methanol tolerance optimization, rational design of active sites, electronic structure tailoring, surface/interface micro-environment engineering, and additional modulation approaches for enhancing ORR performance. Additionally, the mechanisms for enhancing intrinsic catalytic activity are discussed in depth, along with the elucidation of the structure-activity relationship governing catalyst performance in terms of activity, selectivity, and stability. Finally, in light of the critical challenges currently facing DMFC cathode catalysts, future directions and development pathways for catalyst design are proposed.
2026, 37(9): 112411
doi: 10.1016/j.cclet.2026.112411
Abstract:
Although porous carbons (PCs) are promising materials for environmental remediation, their synthesis strategies face high cost, strong device corrosion and severe environmental hazards. This review overviews sustainable organic salt-derived PCs (OAPCs), emphasizing their dual role as activators and self-activators. Meanwhile, six different organic salts are identified for the unique decomposition pathways and activation mechanisms, governing hierarchical porous formation, heteroatom doping, etc. Crucially, the dimensional control of OAPCs from 0D to 3D is min discussed, which favors optimizing ion transport and surface accessibility. The environmental applications of OAPCs are further assessed, proving high potential value in the adsorption, capacitive deionization (CDI), peroxymonosulfate (PMS) activation, electro-Fenton (EF) and microwave absorption. These advancements mainly rely on the tailored morphology and porosity, high conductivity and improved hydrophilicity. Overall, this review provides new insights into sustainable OAPCs, bridging fundamental mechanisms to practical environmental solutions.
Although porous carbons (PCs) are promising materials for environmental remediation, their synthesis strategies face high cost, strong device corrosion and severe environmental hazards. This review overviews sustainable organic salt-derived PCs (OAPCs), emphasizing their dual role as activators and self-activators. Meanwhile, six different organic salts are identified for the unique decomposition pathways and activation mechanisms, governing hierarchical porous formation, heteroatom doping, etc. Crucially, the dimensional control of OAPCs from 0D to 3D is min discussed, which favors optimizing ion transport and surface accessibility. The environmental applications of OAPCs are further assessed, proving high potential value in the adsorption, capacitive deionization (CDI), peroxymonosulfate (PMS) activation, electro-Fenton (EF) and microwave absorption. These advancements mainly rely on the tailored morphology and porosity, high conductivity and improved hydrophilicity. Overall, this review provides new insights into sustainable OAPCs, bridging fundamental mechanisms to practical environmental solutions.
2026, 37(9): 112440
doi: 10.1016/j.cclet.2026.112440
Abstract:
The availability of extensive catalytic data from experiments and computations has facilitated the utilization of machine learning (ML) in developing electrocatalysts for the electrocatalytic nitrogen reduction reaction (eNRR). ML has emerged as an effective paradigm to accelerate the discovery and optimization of eNRR catalysts, leveraging its capabilities in automated processing, interpretation, and prediction of high-performance candidates. Crucially, ML enabled the construction of precise data-driven models, establishing key structure-property relationships between material characteristics (e.g., electronic structure, surface properties) and target catalytic performance (activity, selectivity, stability). This review systematically summarized recent advances in ML for eNRR. ML and deep learning methodologies are examined, focusing on two critical aspects: high-throughput catalyst screening and electrocatalytic process optimization. A critical assessment is provided on the commonalities and challenges in model development, encompassing dataset construction, optimal model selection, and interpretability. Finally, current limitations of ML in eNRR research are discussed and the future perspectives and opportunities for the field are also outlined.
The availability of extensive catalytic data from experiments and computations has facilitated the utilization of machine learning (ML) in developing electrocatalysts for the electrocatalytic nitrogen reduction reaction (eNRR). ML has emerged as an effective paradigm to accelerate the discovery and optimization of eNRR catalysts, leveraging its capabilities in automated processing, interpretation, and prediction of high-performance candidates. Crucially, ML enabled the construction of precise data-driven models, establishing key structure-property relationships between material characteristics (e.g., electronic structure, surface properties) and target catalytic performance (activity, selectivity, stability). This review systematically summarized recent advances in ML for eNRR. ML and deep learning methodologies are examined, focusing on two critical aspects: high-throughput catalyst screening and electrocatalytic process optimization. A critical assessment is provided on the commonalities and challenges in model development, encompassing dataset construction, optimal model selection, and interpretability. Finally, current limitations of ML in eNRR research are discussed and the future perspectives and opportunities for the field are also outlined.
2026, 37(9): 112441
doi: 10.1016/j.cclet.2026.112441
Abstract:
Macroalgae, as the third-generation biomass energy source, is considered the most promising form of renewable energy to replace fossil-based energy resources. Hydrothermal liquefaction (HTL) is a low-carbon conversion technology that transforms macroalgae into liquid biofuels by decomposing and converting macroalgal biomass. This review, based on a summary of recent literature, first outlines the environmental risks associated with macroalgae blooms and highlights the benefits of utilizing hydrothermal liquefaction technology for macroalgae treatment. Subsequently, it elaborates on the key factors influencing the hydrothermal liquefaction of macroalgae, including reaction temperature, reaction time, catalyst type, and solution conditions. The results indicate that bio-oil production and consumption occur concurrently during the hydrothermal liquefaction of macroalgae. As reaction temperature and time increase, the bio-oil yield exhibits a trend of first increasing and then decreasing. When the reaction temperature is excessively high or the reaction time is prolonged, the bio-oil consuming reactions gradually dominate, resulting in reduced bio-oil yields. Compared to homogeneous catalysts, heterogeneous catalysts have garnered greater attention due to their superior catalytic performance and recyclability. The findings demonstrate that mixed solutions are more conducive to bio-oil production than aqueous solutions. Furthermore, this review examines the latest advancements in hydrothermal liquefaction technologies, as well as the elemental migration occurring during the process. The current challenges associated with bio-oils include their high production costs and complex compositions, necessitating further investigation and forming the cornerstone of future research endeavors.
Macroalgae, as the third-generation biomass energy source, is considered the most promising form of renewable energy to replace fossil-based energy resources. Hydrothermal liquefaction (HTL) is a low-carbon conversion technology that transforms macroalgae into liquid biofuels by decomposing and converting macroalgal biomass. This review, based on a summary of recent literature, first outlines the environmental risks associated with macroalgae blooms and highlights the benefits of utilizing hydrothermal liquefaction technology for macroalgae treatment. Subsequently, it elaborates on the key factors influencing the hydrothermal liquefaction of macroalgae, including reaction temperature, reaction time, catalyst type, and solution conditions. The results indicate that bio-oil production and consumption occur concurrently during the hydrothermal liquefaction of macroalgae. As reaction temperature and time increase, the bio-oil yield exhibits a trend of first increasing and then decreasing. When the reaction temperature is excessively high or the reaction time is prolonged, the bio-oil consuming reactions gradually dominate, resulting in reduced bio-oil yields. Compared to homogeneous catalysts, heterogeneous catalysts have garnered greater attention due to their superior catalytic performance and recyclability. The findings demonstrate that mixed solutions are more conducive to bio-oil production than aqueous solutions. Furthermore, this review examines the latest advancements in hydrothermal liquefaction technologies, as well as the elemental migration occurring during the process. The current challenges associated with bio-oils include their high production costs and complex compositions, necessitating further investigation and forming the cornerstone of future research endeavors.
2026, 37(9): 112451
doi: 10.1016/j.cclet.2026.112451
Abstract:
DNAzyme is an artificially created deoxyribonuclease that is produced through in vitro screening. Due to the special properties of DNAzyme, such as catalytic activity, recognition function, excellent thermal stability and flexible designability, it has a broad prospect in constructing biosensors. Many innovative biosensors have been developed by integrating DNAzymes with nanomaterials that exhibit distinct physicochemical properties. This review focuses on the classification and application of DNAzyme-based biosensors, such as RNA-cleavage DNAzyme (8-17, 10-23 DNAzyme), peroxidase mimicking DNAzyme. Finally, some risks and challenges in this field are also discussed.
DNAzyme is an artificially created deoxyribonuclease that is produced through in vitro screening. Due to the special properties of DNAzyme, such as catalytic activity, recognition function, excellent thermal stability and flexible designability, it has a broad prospect in constructing biosensors. Many innovative biosensors have been developed by integrating DNAzymes with nanomaterials that exhibit distinct physicochemical properties. This review focuses on the classification and application of DNAzyme-based biosensors, such as RNA-cleavage DNAzyme (8-17, 10-23 DNAzyme), peroxidase mimicking DNAzyme. Finally, some risks and challenges in this field are also discussed.
2026, 37(9): 112456
doi: 10.1016/j.cclet.2026.112456
Abstract:
Photocatalytic water splitting provides a sustainable approach for converting solar energy into H2. Surface and interfacial engineering has become crucial strategies for enhancing photochemical efficiency and optimizing active sites. This review outlines several primary design strategies, including heteroatom doping (encompassing nonmetal and metal atomic doping), functional group modification, defect engineering, and heterostructure construction. These strategies aim to improve charge separation and surface reaction efficiency. The mechanistic roles of these strategies in metal oxides, sulfides, and carbon nitrides are discussed in terms of band structure tuning, the formation of electron transport pathways, and the modulation of intermediate adsorption energetics. The review examines the synergistic effects of these strategies in enhancing photocatalytic efficiency, stability, and environmental adaptability. Finally, we address future challenges, including interfacial structural stability, in situ characterization of reaction dynamics, and potential applications in sustainable energy systems. We believe that this review will provide insights into developing high-performance photocatalysts for water splitting.
Photocatalytic water splitting provides a sustainable approach for converting solar energy into H2. Surface and interfacial engineering has become crucial strategies for enhancing photochemical efficiency and optimizing active sites. This review outlines several primary design strategies, including heteroatom doping (encompassing nonmetal and metal atomic doping), functional group modification, defect engineering, and heterostructure construction. These strategies aim to improve charge separation and surface reaction efficiency. The mechanistic roles of these strategies in metal oxides, sulfides, and carbon nitrides are discussed in terms of band structure tuning, the formation of electron transport pathways, and the modulation of intermediate adsorption energetics. The review examines the synergistic effects of these strategies in enhancing photocatalytic efficiency, stability, and environmental adaptability. Finally, we address future challenges, including interfacial structural stability, in situ characterization of reaction dynamics, and potential applications in sustainable energy systems. We believe that this review will provide insights into developing high-performance photocatalysts for water splitting.
2026, 37(9): 112510
doi: 10.1016/j.cclet.2026.112510
Abstract:
When a deuterium atom (2H or D) replaces a hydrogen atom (1H) in a reactant molecule, the observed change in the rate (kinetic isotope effect, KIE) or equilibrium (equilibrium isotope effect, EIE) of a chemical reaction is known as a deuterium isotope effect (DIE). Because deuterium is twice as heavy as hydrogen, its zero-point energies (ZPEs), which are the lowest vibrational energies that a bond may have, differ significantly. Due to the obvious advantages of deuterium isotope effects (DIE) in total synthesis and mounting importance of deuterated drugs in pharmaceutical industry, development of synthetic routes to these deuterium-based active drugs via DIE is a challenging and important task. The primary goal of this mini-REVIEW is to demonstrate the novel uses of the DIE effect by placing the D atom at specific locations on drug molecules. This has been shown to serve as a "removable blocking group" to enhance yields and selectivity, while suppressing side reactions in the crucial stages of the complete synthesis of certain drug molecules. This review may be served as a perspective or guide for future study as well as inspire further innovative advancements in the field of total synthesis, and stimulate their applications in the related mechanistic studies.
When a deuterium atom (2H or D) replaces a hydrogen atom (1H) in a reactant molecule, the observed change in the rate (kinetic isotope effect, KIE) or equilibrium (equilibrium isotope effect, EIE) of a chemical reaction is known as a deuterium isotope effect (DIE). Because deuterium is twice as heavy as hydrogen, its zero-point energies (ZPEs), which are the lowest vibrational energies that a bond may have, differ significantly. Due to the obvious advantages of deuterium isotope effects (DIE) in total synthesis and mounting importance of deuterated drugs in pharmaceutical industry, development of synthetic routes to these deuterium-based active drugs via DIE is a challenging and important task. The primary goal of this mini-REVIEW is to demonstrate the novel uses of the DIE effect by placing the D atom at specific locations on drug molecules. This has been shown to serve as a "removable blocking group" to enhance yields and selectivity, while suppressing side reactions in the crucial stages of the complete synthesis of certain drug molecules. This review may be served as a perspective or guide for future study as well as inspire further innovative advancements in the field of total synthesis, and stimulate their applications in the related mechanistic studies.
2026, 37(9): 112631
doi: 10.1016/j.cclet.2026.112631
Abstract:
Silicon is considered as one of the most promising anodes for next-generation lithium-ion batteries (LIBs) due to its high theoretical specific capacity (3579 mAh/g) and abundant natural reserves. Compared to nano silicon, micron silicon offers distinct advantages, including lower specific surface area, reduced interfacial side reactions, higher initial coulombic efficiency, greater tap density, and lower cost, making it highly attractive for practical applications. However, its commercial viability is hindered by severe volume expansion, localized stress accumulation, repeated formation of unstable solid electrolyte interphase (SEI) layers, and electrical disconnection during cycling, which together result in rapid capacity fading and high irreversible capacity loss. Recent advances in electrolyte engineering, particularly interfacial modification strategies, have significantly improved the performance of micron silicon anodes by mitigating these challenges. This review provides an integrated perspective on the application of micron-sized silicon anodes by correlating lithium storage mechanisms, failure behaviors, and electrolyte-electrode interfacial evolution. Based on a systematic discussion of silicon lithiation/delithiation processes and associated structural instability, we clarify how interfacial degradation and irreversible lithium consumption govern the electrochemical performance of micron silicon. Then, electrolyte optimization strategies are critically analyzed, with an explicit comparison between liquid electrolyte regulation and solid-state electrolyte (SSE) design, highlighting their distinct roles in interfacial stabilization, stress accommodation, and cycling durability. From an electrolyte system design standpoint, this review summarizes integrated design principles for improving micron silicon performance and discusses the remaining challenges and opportunities toward their commercial application in high-energy-density battery systems.
Silicon is considered as one of the most promising anodes for next-generation lithium-ion batteries (LIBs) due to its high theoretical specific capacity (3579 mAh/g) and abundant natural reserves. Compared to nano silicon, micron silicon offers distinct advantages, including lower specific surface area, reduced interfacial side reactions, higher initial coulombic efficiency, greater tap density, and lower cost, making it highly attractive for practical applications. However, its commercial viability is hindered by severe volume expansion, localized stress accumulation, repeated formation of unstable solid electrolyte interphase (SEI) layers, and electrical disconnection during cycling, which together result in rapid capacity fading and high irreversible capacity loss. Recent advances in electrolyte engineering, particularly interfacial modification strategies, have significantly improved the performance of micron silicon anodes by mitigating these challenges. This review provides an integrated perspective on the application of micron-sized silicon anodes by correlating lithium storage mechanisms, failure behaviors, and electrolyte-electrode interfacial evolution. Based on a systematic discussion of silicon lithiation/delithiation processes and associated structural instability, we clarify how interfacial degradation and irreversible lithium consumption govern the electrochemical performance of micron silicon. Then, electrolyte optimization strategies are critically analyzed, with an explicit comparison between liquid electrolyte regulation and solid-state electrolyte (SSE) design, highlighting their distinct roles in interfacial stabilization, stress accommodation, and cycling durability. From an electrolyte system design standpoint, this review summarizes integrated design principles for improving micron silicon performance and discusses the remaining challenges and opportunities toward their commercial application in high-energy-density battery systems.
2026, 37(9): 112640
doi: 10.1016/j.cclet.2026.112640
Abstract:
Fluorine substitution has emerged as a cornerstone of modern drug design, profoundly influencing the pharmacological properties of therapeutic agents. Owing to its high electronegativity and small atomic radius, fluorine imparts unique electronic and steric effects that enhance lipophilicity, metabolic stability, binding affinity, and pKa, thereby improving efficacy, bioavailability, and pharmacokinetics. Often referred to as an "enchanted atom", fluorine can decisively alter the trajectory of drug candidates, reducing attrition and increasing clinical success. Within synthetic organic chemistry, the pursuit of novel biologically active compounds is closely tied to monitoring advances in approved pharmaceuticals, with fluorine-containing drugs representing one of the most dynamic areas of innovation. In this review, we profile fourteen new pharmaceuticals approved by the U.S. Food and Drug Administration (FDA) in 2025, including datopotamab deruxtecan, suzetrigine, mirdametinib, avutometinib/defactinib, taletrectinib, sunvozertinib, sebetralstat, rilzabrutinib, imlunestrant, paltusotine, remibrutinib, elinzanetant, ziftomenib, and zoliflodacin. For each compound, we examine the medicinal chemistry discovery, therapeutic application, and FDA approval timeline, with particular emphasis on synthetic strategies and the role of fluorine incorporation. This review aims to provide a timely resource and inspiration for researchers in academia and the pharmaceutical industry, as well as for students engaged in drug design, fluorine chemistry, and medicinal chemistry.
Fluorine substitution has emerged as a cornerstone of modern drug design, profoundly influencing the pharmacological properties of therapeutic agents. Owing to its high electronegativity and small atomic radius, fluorine imparts unique electronic and steric effects that enhance lipophilicity, metabolic stability, binding affinity, and pKa, thereby improving efficacy, bioavailability, and pharmacokinetics. Often referred to as an "enchanted atom", fluorine can decisively alter the trajectory of drug candidates, reducing attrition and increasing clinical success. Within synthetic organic chemistry, the pursuit of novel biologically active compounds is closely tied to monitoring advances in approved pharmaceuticals, with fluorine-containing drugs representing one of the most dynamic areas of innovation. In this review, we profile fourteen new pharmaceuticals approved by the U.S. Food and Drug Administration (FDA) in 2025, including datopotamab deruxtecan, suzetrigine, mirdametinib, avutometinib/defactinib, taletrectinib, sunvozertinib, sebetralstat, rilzabrutinib, imlunestrant, paltusotine, remibrutinib, elinzanetant, ziftomenib, and zoliflodacin. For each compound, we examine the medicinal chemistry discovery, therapeutic application, and FDA approval timeline, with particular emphasis on synthetic strategies and the role of fluorine incorporation. This review aims to provide a timely resource and inspiration for researchers in academia and the pharmaceutical industry, as well as for students engaged in drug design, fluorine chemistry, and medicinal chemistry.
2026, 37(9): 112689
doi: 10.1016/j.cclet.2026.112689
Abstract:
The electrochemical nitrogen reduction reaction (NRR) is widely regarded as a promising sustainable alternative to the energy-intensive Haber-Bosch process for ammonia synthesis. In recent years, a large number of studies have focused on enhancing key NRR performance metrics, particularly Faradaic efficiency and ammonia (NH3) yield rate, leading to notable progress in both areas. Despite these advances, the development of low-cost, high-performance electrocatalysts remains the primary challenge and a major bottleneck to large-scale industrial application. This review summarizes the current understanding of NRR mechanisms and reaction pathways, as well as recent progress in electrochemical cell design, quantitative NH3 detection strategies, and electrocatalyst development. Focusing on electrocatalysts, we provide an overview of the major classes of electrocatalysts including noble metals, transition metals, single-atom systems, metal-organic frameworks, and non-metallic materials. Furthermore, we compare their respective advantages and limitations. Finally, we outline the key challenges and future directions for engineering next-generation electrocatalysts capable of achieving high-efficiency nitrogen fixation.
The electrochemical nitrogen reduction reaction (NRR) is widely regarded as a promising sustainable alternative to the energy-intensive Haber-Bosch process for ammonia synthesis. In recent years, a large number of studies have focused on enhancing key NRR performance metrics, particularly Faradaic efficiency and ammonia (NH3) yield rate, leading to notable progress in both areas. Despite these advances, the development of low-cost, high-performance electrocatalysts remains the primary challenge and a major bottleneck to large-scale industrial application. This review summarizes the current understanding of NRR mechanisms and reaction pathways, as well as recent progress in electrochemical cell design, quantitative NH3 detection strategies, and electrocatalyst development. Focusing on electrocatalysts, we provide an overview of the major classes of electrocatalysts including noble metals, transition metals, single-atom systems, metal-organic frameworks, and non-metallic materials. Furthermore, we compare their respective advantages and limitations. Finally, we outline the key challenges and future directions for engineering next-generation electrocatalysts capable of achieving high-efficiency nitrogen fixation.
2026, 37(9): 112485
doi: 10.1016/j.cclet.2026.112485
Abstract:
Covalent-organic frameworks (COFs) have attracted growing interest as photocatalytic materials for uranium extraction because of their tunable structures and adjustable optoelectronic properties. This perspective summarizes recent progress in COF-based systems for the selective capture and photoreduction of U(Ⅵ), with a focus on molecular design strategies such as band-structure regulation, donor-acceptor framework construction, and interfacial functionalization to improve visible-light utilization and charge separation. Key mechanistic aspects of photoinduced uranium conversion, including electron-transfer pathways, uranium valence evolution, and interfacial reaction kinetics, are discussed. Current challenges, such as uncertainty in reduction products, incomplete mechanistic understanding, and limited cycling stability, are also addressed by highlighting the role of in situ characterization combined with theoretical analysis. Finally, the potential of artificial intelligence-assisted design and the development of macroscopic COF forms, such as aerogels and membranes, are briefly discussed as routes toward practical uranium extraction.
Covalent-organic frameworks (COFs) have attracted growing interest as photocatalytic materials for uranium extraction because of their tunable structures and adjustable optoelectronic properties. This perspective summarizes recent progress in COF-based systems for the selective capture and photoreduction of U(Ⅵ), with a focus on molecular design strategies such as band-structure regulation, donor-acceptor framework construction, and interfacial functionalization to improve visible-light utilization and charge separation. Key mechanistic aspects of photoinduced uranium conversion, including electron-transfer pathways, uranium valence evolution, and interfacial reaction kinetics, are discussed. Current challenges, such as uncertainty in reduction products, incomplete mechanistic understanding, and limited cycling stability, are also addressed by highlighting the role of in situ characterization combined with theoretical analysis. Finally, the potential of artificial intelligence-assisted design and the development of macroscopic COF forms, such as aerogels and membranes, are briefly discussed as routes toward practical uranium extraction.
2026, 37(9): 112780
doi: 10.1016/j.cclet.2026.112780
Abstract:
2026, 37(9): 112910
doi: 10.1016/j.cclet.2026.112910
Abstract:
