2026 Volume 42 Issue 3
2026, 42(3):
Abstract:
2026, 42(3): 100165
doi: 10.1016/j.actphy.2025.100165
Abstract:
Integrating photocatalytic cofactor regeneration with enzymatic cascades enables sustainable CO2 valorization but faces challenges like limited hydrogen sources and homogeneous mediator and photogenerated holes-induced enzyme deactivation. This study demonstrates that the low oxidation potential of L-ascorbic acid (L-AA) can enhance proton supply and promote the formation of[Cp*Rh(bpy)H]+ intermediates. Only 0.26 mg (≈ 0.12 mmol L-1)[Cp*Rh(bpy)Cl]Cl can achieve efficient/selective reduced nicotinamide adenine dinucleotide (NADH) regeneration, which is more than twice as effective as the typical sacrificial agent triethanolamine (TEOA). A novel strategy was developed via electrostatic self-assembly of [Cp*Rh(bpy)H2O]2+ onto CdIn2S4 microsphere photocatalysts. This innovative integration physically separated free mediators and photogenerated holes from enzymes, effectively suppressing enzyme deactivation through spatial compartmentalization. The optimal integrated photocatalytic system achieved 90% NADH regeneration efficiency within 40 min of 420 nm light irradiation, outperforming previously reported systems. When coupled with formate dehydrogenase (FDH), the integrated system achieved formic acid generation rates of 443.5 μmol g-1 h-1 (one light-dark cycle) and 202.7 μmol g-1 h-1 (continuous light), representing 1.2- and 3.2-fold improvements over free mediator systems, respectively. This study provides an efficient and sustainable new strategy for light driven coenzyme regeneration and enzyme catalyzed CO2 synthesis of high value-added chemicals.
Integrating photocatalytic cofactor regeneration with enzymatic cascades enables sustainable CO2 valorization but faces challenges like limited hydrogen sources and homogeneous mediator and photogenerated holes-induced enzyme deactivation. This study demonstrates that the low oxidation potential of L-ascorbic acid (L-AA) can enhance proton supply and promote the formation of[Cp*Rh(bpy)H]+ intermediates. Only 0.26 mg (≈ 0.12 mmol L-1)[Cp*Rh(bpy)Cl]Cl can achieve efficient/selective reduced nicotinamide adenine dinucleotide (NADH) regeneration, which is more than twice as effective as the typical sacrificial agent triethanolamine (TEOA). A novel strategy was developed via electrostatic self-assembly of [Cp*Rh(bpy)H2O]2+ onto CdIn2S4 microsphere photocatalysts. This innovative integration physically separated free mediators and photogenerated holes from enzymes, effectively suppressing enzyme deactivation through spatial compartmentalization. The optimal integrated photocatalytic system achieved 90% NADH regeneration efficiency within 40 min of 420 nm light irradiation, outperforming previously reported systems. When coupled with formate dehydrogenase (FDH), the integrated system achieved formic acid generation rates of 443.5 μmol g-1 h-1 (one light-dark cycle) and 202.7 μmol g-1 h-1 (continuous light), representing 1.2- and 3.2-fold improvements over free mediator systems, respectively. This study provides an efficient and sustainable new strategy for light driven coenzyme regeneration and enzyme catalyzed CO2 synthesis of high value-added chemicals.
2026, 42(3): 100166
doi: 10.1016/j.actphy.2025.100166
Abstract:
Addressing the global energy and environmental crisis necessitates the development of sustainable photocatalytic technologies capable of efficiently converting biomass into high-value chemicals and clean fuels. In this study, we develop a novel one-dimensional/two-dimensional (1D/2D) In2O3/ZnIn2S4S-scheme heterojunction photocatalyst through in situ growth process. This rationally designed architecture combines rod-like In2O3 with sheet-like ZnIn2S4 nanosheets, facilitating directional charge transport and providing a high density of active sites. Consequently, the optimized In2O3/ZnIn2S4 heterojunction achieved a 5-hydroxymethylfurfural (HMF) conversion rate of 81.6% with a high selectivity of 78.2% toward 2,5-diformylfuran (DFF) and 2,5-furandicarboxylic acid (FDCA). Furthermore, it exhibited a hydrogen (H2) evolution rate of 257.69 μmol g-1 h-1 under 420 nm LED irradiation. These results demonstrate the efficacy of S-scheme heterojunctions in enabling spatial charge separation and boosting photocatalytic activity, offering a promising strategy for solar-driven biomass valorization and sustainable H2 production.
Addressing the global energy and environmental crisis necessitates the development of sustainable photocatalytic technologies capable of efficiently converting biomass into high-value chemicals and clean fuels. In this study, we develop a novel one-dimensional/two-dimensional (1D/2D) In2O3/ZnIn2S4S-scheme heterojunction photocatalyst through in situ growth process. This rationally designed architecture combines rod-like In2O3 with sheet-like ZnIn2S4 nanosheets, facilitating directional charge transport and providing a high density of active sites. Consequently, the optimized In2O3/ZnIn2S4 heterojunction achieved a 5-hydroxymethylfurfural (HMF) conversion rate of 81.6% with a high selectivity of 78.2% toward 2,5-diformylfuran (DFF) and 2,5-furandicarboxylic acid (FDCA). Furthermore, it exhibited a hydrogen (H2) evolution rate of 257.69 μmol g-1 h-1 under 420 nm LED irradiation. These results demonstrate the efficacy of S-scheme heterojunctions in enabling spatial charge separation and boosting photocatalytic activity, offering a promising strategy for solar-driven biomass valorization and sustainable H2 production.
2026, 42(3): 100172
doi: 10.1016/j.actphy.2025.100172
Abstract:
Solar-driven oxygen reduction for H2O2 production offers a green, efficient, and environmentally friendly alternative to the conventional industrial anthraquinone process and direct H2/O2 synthesis. In this study, through targeted crystal facet engineering, a hydrogen-bonded organic framework (HOF) was selectively anchored onto the (010) facet of BiVO4, forming an S-scheme heterojunction where the HOF is the reducing side and oxygen reduction occurs to produce H2O2. This configuration significantly enhanced the H2O2 yield to 555 μmol g-1 h-1, representing a ~37% improvement compared to randomly contacted HOF/BiVO4 systems. In situ Kelvin probe force microscopy (KPFM) revealed the formation of an intrinsic electric field between the (110) and (010) facets of pristine BiVO4, with the (010) facet becoming electron-rich under illumination. Further investigation of the HOF/BiVO4 (010) material, where HOF is directionally anchored to the (010) facet of BiVO4, demonstrated the establishment of an additional built-in electric field between the two components. Thus, we propose a novel HOF/BiVO4(010) photocatalytic material featuring dual built-in electric fields in the heterojunctions, which significantly promote the dual directed charge transfer in the different facets of single crystal BiVO4 and the interface of the S-scheme heterojunction. In situ X-ray Photoelectron Spectroscopy (XPS) further confirmed the S-scheme heterojunction electron transfer mechanism. By introducing electron scavengers and hole trappers, we conclusively verified that the heterojunction-mediated photocatalytic process follows a two-electron Oxygen Reduction Reaction (ORR) pathway. Electron Paramagnetic Resonance (EPR) spectroscopy detected the presence of superoxide radicals (∙O2-), indicating that the ORR proceeds via an indirect two-electron transfer mechanism. The synergistic effects of the dual built-in electric fields, S-scheme heterojunction structure, and two-electron ORR pathway collectively contribute to the superior photocatalytic performance of this system.
Solar-driven oxygen reduction for H2O2 production offers a green, efficient, and environmentally friendly alternative to the conventional industrial anthraquinone process and direct H2/O2 synthesis. In this study, through targeted crystal facet engineering, a hydrogen-bonded organic framework (HOF) was selectively anchored onto the (010) facet of BiVO4, forming an S-scheme heterojunction where the HOF is the reducing side and oxygen reduction occurs to produce H2O2. This configuration significantly enhanced the H2O2 yield to 555 μmol g-1 h-1, representing a ~37% improvement compared to randomly contacted HOF/BiVO4 systems. In situ Kelvin probe force microscopy (KPFM) revealed the formation of an intrinsic electric field between the (110) and (010) facets of pristine BiVO4, with the (010) facet becoming electron-rich under illumination. Further investigation of the HOF/BiVO4 (010) material, where HOF is directionally anchored to the (010) facet of BiVO4, demonstrated the establishment of an additional built-in electric field between the two components. Thus, we propose a novel HOF/BiVO4(010) photocatalytic material featuring dual built-in electric fields in the heterojunctions, which significantly promote the dual directed charge transfer in the different facets of single crystal BiVO4 and the interface of the S-scheme heterojunction. In situ X-ray Photoelectron Spectroscopy (XPS) further confirmed the S-scheme heterojunction electron transfer mechanism. By introducing electron scavengers and hole trappers, we conclusively verified that the heterojunction-mediated photocatalytic process follows a two-electron Oxygen Reduction Reaction (ORR) pathway. Electron Paramagnetic Resonance (EPR) spectroscopy detected the presence of superoxide radicals (∙O2-), indicating that the ORR proceeds via an indirect two-electron transfer mechanism. The synergistic effects of the dual built-in electric fields, S-scheme heterojunction structure, and two-electron ORR pathway collectively contribute to the superior photocatalytic performance of this system.
2026, 42(3): 100181
doi: 10.1016/j.actphy.2025.100181
Abstract:
In this study, we explore the potential of the Ruddlesden-Popper (RP)-type bilayer manganite LaSr2Mn2O6.96 as an intercalation-based cathode material for all-solid-state fluoride ion batteries (FIBs). Structural changes of LaSr2Mn2O6.96 during fluoride intercalation and de-intercalation were analyzed via ex situ X-ray diffraction, revealing that F- insertion induces the formation of three distinct tetragonal phases. To understand the complex behavior of these phases, we examined the changes in the Mn oxidation state and coordination environment using X-ray absorption spectroscopy and magnetic measurements. Under stack pressure (20 kN), electrochemical cycling of LaSr2Mn2O6.96 in the potential range of 1 V to -1 V exhibited a continuous increase in specific capacity from capacity of ~30 mAh g-1 to ~68 mAh g-1 over 200 cycles, with ~99% coulombic efficiency and no signs of capacity fading. This makes the bilayer manganite LaSr2Mn2O6.96 a promising candidate for a cycling stable cathode for all-solid-state FIBs, especially under the application of stack pressure.
In this study, we explore the potential of the Ruddlesden-Popper (RP)-type bilayer manganite LaSr2Mn2O6.96 as an intercalation-based cathode material for all-solid-state fluoride ion batteries (FIBs). Structural changes of LaSr2Mn2O6.96 during fluoride intercalation and de-intercalation were analyzed via ex situ X-ray diffraction, revealing that F- insertion induces the formation of three distinct tetragonal phases. To understand the complex behavior of these phases, we examined the changes in the Mn oxidation state and coordination environment using X-ray absorption spectroscopy and magnetic measurements. Under stack pressure (20 kN), electrochemical cycling of LaSr2Mn2O6.96 in the potential range of 1 V to -1 V exhibited a continuous increase in specific capacity from capacity of ~30 mAh g-1 to ~68 mAh g-1 over 200 cycles, with ~99% coulombic efficiency and no signs of capacity fading. This makes the bilayer manganite LaSr2Mn2O6.96 a promising candidate for a cycling stable cathode for all-solid-state FIBs, especially under the application of stack pressure.
2026, 42(3): 100184
doi: 10.1016/j.actphy.2025.100184
Abstract:
Photocatalysis of H2O2 production using O2 and water is a cost-effective and environmental process, but developing high-performance photocatalysts is still a challenge. Herein, a WO3@polymer S-scheme photocatalyst was synthesized by in situ growing the Schiff-base polymer, tris-(4-aminophenyl)amine (TAPA)-terephthaldicarboxaldehyde (PDA) (labeled as TP) on the surface of WO3 nanofibers (WO3@TP) at room temperature. The obtained WO3@TP S-scheme heterojunction exhibited rapid carrier separation ability and short photogenerated carriers transfer distance. The optimal WO3@TP composite (WT-10) realized the H2O2evolution rate of 3242 μmol g-1 h-1, which was 137.3 and 4.6-fold higher than bare WO3 and TP, respectively. The combination of advanced characterizations regarding in situ irradiated X-ray photoelectron spectroscopy (ISI-XPS), theoretical calculation, and femtosecond transient absorption spectroscopy (fs-TAS) validates the charge transfer mechanism within the WO3@TP S-scheme heterojunction. The occurrence of a dual-channel pathway (O2 reduction reaction (ORR) and water oxidation reaction (WOR) within the reaction system has been confirmed via electron paramagnetic resonance (EPR) and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), thereby contributing to the highly efficient H2O2 evolution. This study not only gives an in-depth understanding of the ultrafast charge migration behavior in S-scheme heterojunction but also offers the rational design of inorganic@organic photocatalysts applied to solar-driven H2O2 production.
Photocatalysis of H2O2 production using O2 and water is a cost-effective and environmental process, but developing high-performance photocatalysts is still a challenge. Herein, a WO3@polymer S-scheme photocatalyst was synthesized by in situ growing the Schiff-base polymer, tris-(4-aminophenyl)amine (TAPA)-terephthaldicarboxaldehyde (PDA) (labeled as TP) on the surface of WO3 nanofibers (WO3@TP) at room temperature. The obtained WO3@TP S-scheme heterojunction exhibited rapid carrier separation ability and short photogenerated carriers transfer distance. The optimal WO3@TP composite (WT-10) realized the H2O2evolution rate of 3242 μmol g-1 h-1, which was 137.3 and 4.6-fold higher than bare WO3 and TP, respectively. The combination of advanced characterizations regarding in situ irradiated X-ray photoelectron spectroscopy (ISI-XPS), theoretical calculation, and femtosecond transient absorption spectroscopy (fs-TAS) validates the charge transfer mechanism within the WO3@TP S-scheme heterojunction. The occurrence of a dual-channel pathway (O2 reduction reaction (ORR) and water oxidation reaction (WOR) within the reaction system has been confirmed via electron paramagnetic resonance (EPR) and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), thereby contributing to the highly efficient H2O2 evolution. This study not only gives an in-depth understanding of the ultrafast charge migration behavior in S-scheme heterojunction but also offers the rational design of inorganic@organic photocatalysts applied to solar-driven H2O2 production.
2026, 42(3): 100194
doi: 10.1016/j.actphy.2025.100194
Abstract:
In the rapidly evolving field of photovoltaic technology, self-assembled monolayers (SAMs) have become essential hole-selective layers (HSLs) for inverted perovskite solar cells (PSCs). SAMs not only determine interfacial hole extraction but also significantly influence the film quality of the atop perovskite layers, consequently affecting the efficiency and stability of perovskite solar cells. Among various SAMs, carbazole-based SAMs, exemplified by 4PACZ, have emerged as prominent due to their electron-rich characteristics, making them some of the most prevalent HSLs in modern inverted PSCs. Nevertheless, 4PACZ exhibits significant limitations: one major issue is its limited molecular dipole, which leads to insufficient energy level alignment between the treated substrate and the perovskite, causing substantial interfacial energy loss. Another critical challenge is the flat structure of the carbazole unit, which often promotes molecular stacking, resulting in incomplete substrate coverage and non-uniform film formation, thereby compromising both device performance and stability. In this study, we designed a novel SAM based on a polycyclic aromatic hydrocarbon derivative, (4-(8H-dinaphtho[2,3-c:2',3'-g]carbazol-8-yl)butyl)phosphonic acid (4PADNC), with the aim of optimizing hole transport in inverted PSCs. This SAM incorporates the structurally extended dinaphtho[2,3-c:2',3'-g]carbazole (DNC) as the functional terminal group, replacing the single carbazole unit in the traditional material 4PACZ. The key structural difference is that the DNC group provides a significantly expanded π-conjugated skeleton and enhanced electron-rich characteristics. These features not only greatly enhance hole extraction and transport at the interface but also induce a significant increase in the molecular dipole moment, which is crucial for effectively adjusting the work function of ITO, ensuring proper alignment with the perovskite layer. Additionally, there is an intramolecular dihedral angle of approximately 34.62° in the DNC unit at the core of 4PADNC. This non-planar configuration contrasts sharply with the planar carbazole structure. The larger dihedral angle effectively suppresses excessive π-π stacking between molecules, which not only aids in forming a denser and more ordered molecular layer on the ITO surface but also provides a more favorable and defect-free substrate for the growth of the upper perovskite. With these upgrades, the inverted PSCs based on 4PADNC achieved a PCE as high as 24.32%, compared to 22.89% for the control devices based on 4PACZ. Furthermore, the 4PADNC-based devices also exhibited superior thermal stability and operational stability.
In the rapidly evolving field of photovoltaic technology, self-assembled monolayers (SAMs) have become essential hole-selective layers (HSLs) for inverted perovskite solar cells (PSCs). SAMs not only determine interfacial hole extraction but also significantly influence the film quality of the atop perovskite layers, consequently affecting the efficiency and stability of perovskite solar cells. Among various SAMs, carbazole-based SAMs, exemplified by 4PACZ, have emerged as prominent due to their electron-rich characteristics, making them some of the most prevalent HSLs in modern inverted PSCs. Nevertheless, 4PACZ exhibits significant limitations: one major issue is its limited molecular dipole, which leads to insufficient energy level alignment between the treated substrate and the perovskite, causing substantial interfacial energy loss. Another critical challenge is the flat structure of the carbazole unit, which often promotes molecular stacking, resulting in incomplete substrate coverage and non-uniform film formation, thereby compromising both device performance and stability. In this study, we designed a novel SAM based on a polycyclic aromatic hydrocarbon derivative, (4-(8H-dinaphtho[2,3-c:2',3'-g]carbazol-8-yl)butyl)phosphonic acid (4PADNC), with the aim of optimizing hole transport in inverted PSCs. This SAM incorporates the structurally extended dinaphtho[2,3-c:2',3'-g]carbazole (DNC) as the functional terminal group, replacing the single carbazole unit in the traditional material 4PACZ. The key structural difference is that the DNC group provides a significantly expanded π-conjugated skeleton and enhanced electron-rich characteristics. These features not only greatly enhance hole extraction and transport at the interface but also induce a significant increase in the molecular dipole moment, which is crucial for effectively adjusting the work function of ITO, ensuring proper alignment with the perovskite layer. Additionally, there is an intramolecular dihedral angle of approximately 34.62° in the DNC unit at the core of 4PADNC. This non-planar configuration contrasts sharply with the planar carbazole structure. The larger dihedral angle effectively suppresses excessive π-π stacking between molecules, which not only aids in forming a denser and more ordered molecular layer on the ITO surface but also provides a more favorable and defect-free substrate for the growth of the upper perovskite. With these upgrades, the inverted PSCs based on 4PADNC achieved a PCE as high as 24.32%, compared to 22.89% for the control devices based on 4PACZ. Furthermore, the 4PADNC-based devices also exhibited superior thermal stability and operational stability.
2026, 42(3): 100198
doi: 10.1016/j.actphy.2025.100198
Abstract:
Phosphorescent inks based on carbon nanodots (CNDs) offer an environmentally friendly and low-cost alternative for persistent visibility and time-delayed information retrieval. However, current matrix-dependent phosphorescent CNDs suffer from poor processability and limited substrate compatibility, hindering their application in scalable, high-resolution invisible printing. Here, we report water-soluble phosphorescent CND inks that enable high-resolution, environmentally stable, and invisible printing. The triplet excitons in CNDs are stabilized by spatial confinement during printing, resulting in bright and long-lived phosphorescence. The phosphorescent CND inks enable invisible yet high-fidelity printing of complex textual patterns with micrometer resolution (2480 × 3508 dpi, ~100 μm feature size), supporting font sizes down to 5 pt and line widths as thin as 0.05 pt across five types of paper substrates. The printed patterns exhibit over 98.7% accuracy across approximately 8.7 million pixels, demonstrating excellent fidelity. Based on these excellent invisible printing properties, a 200-page wordless book using phosphorescent CND inks was demonstrated. This work presents a scalable, low-cost, and high-resolution platform for phosphorescent ink printing, marking a significant advance in invisible printing technology.
Phosphorescent inks based on carbon nanodots (CNDs) offer an environmentally friendly and low-cost alternative for persistent visibility and time-delayed information retrieval. However, current matrix-dependent phosphorescent CNDs suffer from poor processability and limited substrate compatibility, hindering their application in scalable, high-resolution invisible printing. Here, we report water-soluble phosphorescent CND inks that enable high-resolution, environmentally stable, and invisible printing. The triplet excitons in CNDs are stabilized by spatial confinement during printing, resulting in bright and long-lived phosphorescence. The phosphorescent CND inks enable invisible yet high-fidelity printing of complex textual patterns with micrometer resolution (2480 × 3508 dpi, ~100 μm feature size), supporting font sizes down to 5 pt and line widths as thin as 0.05 pt across five types of paper substrates. The printed patterns exhibit over 98.7% accuracy across approximately 8.7 million pixels, demonstrating excellent fidelity. Based on these excellent invisible printing properties, a 200-page wordless book using phosphorescent CND inks was demonstrated. This work presents a scalable, low-cost, and high-resolution platform for phosphorescent ink printing, marking a significant advance in invisible printing technology.
2026, 42(3): 100200
doi: 10.1016/j.actphy.2025.100200
Abstract:
With prospects for high energy density and safety, all-solid-state lithium-ion batteries (ASSLBs) with lithium-rich manganese-based materials (LRMs) are exploited as next-generation energy storage systems. However, the severe interfacial degradations with halide solid electrolytes (SEs) caused by the irreversible oxygen release remain to be urgently solved. In this work, we synthesized Cr-substituted LRMs with high capacity and stability. The reversible redox of Cr3+/Cr6+ contributes to an enhanced capacity, accompanied by the reversible migration of Cr6+ ions between octahedral and tetrahedral sites, effectively maintaining the structural stability of LRMs. Meanwhile, the strong Cr–O bond can stabilize the lattice oxygen, establish a stable cathode/electrolyte interface, and alleviate the voltage decay. Therefore, the ASSBs with LRMs-Cr0.1 cathode and halide electrolyte show an excellent cycling stability with 0.065% capacity decay per cycle for 500 cycles at 0.5C. Notably, the LRMs-Cr0.1//Li21Si5@Si/C full cell exhibits outstanding long-term cyclability over 1000 cycles with nearly 100% capacity retention at 0.3C, corresponding to an energy density of 413.11 Wh kg-1. This work provides guidance for developing high energy-density solid-state batteries.
With prospects for high energy density and safety, all-solid-state lithium-ion batteries (ASSLBs) with lithium-rich manganese-based materials (LRMs) are exploited as next-generation energy storage systems. However, the severe interfacial degradations with halide solid electrolytes (SEs) caused by the irreversible oxygen release remain to be urgently solved. In this work, we synthesized Cr-substituted LRMs with high capacity and stability. The reversible redox of Cr3+/Cr6+ contributes to an enhanced capacity, accompanied by the reversible migration of Cr6+ ions between octahedral and tetrahedral sites, effectively maintaining the structural stability of LRMs. Meanwhile, the strong Cr–O bond can stabilize the lattice oxygen, establish a stable cathode/electrolyte interface, and alleviate the voltage decay. Therefore, the ASSBs with LRMs-Cr0.1 cathode and halide electrolyte show an excellent cycling stability with 0.065% capacity decay per cycle for 500 cycles at 0.5C. Notably, the LRMs-Cr0.1//Li21Si5@Si/C full cell exhibits outstanding long-term cyclability over 1000 cycles with nearly 100% capacity retention at 0.3C, corresponding to an energy density of 413.11 Wh kg-1. This work provides guidance for developing high energy-density solid-state batteries.
2026, 42(3): 100170
doi: 10.1016/j.actphy.2025.100170
Abstract:
In response to the growing demand for renewable energy, rechargeable batteries, such as lithium-ion batteries, are finding increasingly widespread applications in energy storage and daily life. Currently, the pursuit of batteries with high specific energy and enhanced safety is constrained by limitations in the electrolyte bulk and interfacial reactions. Consequently, modulating the electrolyte and its interphases is key to overcoming current bottlenecks and developing next-generation batteries. As an emerging nanomaterial, the rich surface functional groups and dopable sites of carbon dots (CDs) enable them to simultaneously regulate bulk ion dynamics and interface stability through surface chemistry design, showcasing immense potential in addressing the critical challenges in electrolytes. This review systematically summarizes the cutting-edge applications of CDs in electrolytes for lithium-ion, sodium-ion, and zinc-ion batteries. It introduces the structural characteristics, classification, and synthesis methods of CDs, and outlines their multifaceted roles as additives in liquid electrolytes, fillers in solid-state electrolytes, and interfacial regulators for solid composite electrolytes. A special focus is placed on elucidating the mechanisms of CDs in regulating ion deposition, constructing functionalized interfacial layers, and optimizing the electrolyte microenvironment. Finally, this review discusses the challenges and future outlook for CDs in electrolyte engineering, aiming to provide new perspectives and theoretical support for the design of battery systems with high specific energy and high safety.
In response to the growing demand for renewable energy, rechargeable batteries, such as lithium-ion batteries, are finding increasingly widespread applications in energy storage and daily life. Currently, the pursuit of batteries with high specific energy and enhanced safety is constrained by limitations in the electrolyte bulk and interfacial reactions. Consequently, modulating the electrolyte and its interphases is key to overcoming current bottlenecks and developing next-generation batteries. As an emerging nanomaterial, the rich surface functional groups and dopable sites of carbon dots (CDs) enable them to simultaneously regulate bulk ion dynamics and interface stability through surface chemistry design, showcasing immense potential in addressing the critical challenges in electrolytes. This review systematically summarizes the cutting-edge applications of CDs in electrolytes for lithium-ion, sodium-ion, and zinc-ion batteries. It introduces the structural characteristics, classification, and synthesis methods of CDs, and outlines their multifaceted roles as additives in liquid electrolytes, fillers in solid-state electrolytes, and interfacial regulators for solid composite electrolytes. A special focus is placed on elucidating the mechanisms of CDs in regulating ion deposition, constructing functionalized interfacial layers, and optimizing the electrolyte microenvironment. Finally, this review discusses the challenges and future outlook for CDs in electrolyte engineering, aiming to provide new perspectives and theoretical support for the design of battery systems with high specific energy and high safety.
2026, 42(3): 100188
doi: 10.1016/j.actphy.2025.100188
Abstract:
Phase, which refers to the long-range ordered atomic arrangement, is one of the key parameters to determine the physicochemical properties and functions of nanomaterials. Recently, phase engineering of nanomaterials (PEN) has emerged as a promising research direction in materials science, since precise control over atomic arrangements enables the synthesis of nanomaterials with unconventional phases that are different from their thermodynamically stable counterparts, resulting in unique physicochemical properties. Therefore, PEN provides a new strategy for developing novel functional nanomaterials to enhance their performance in various applications. This review focuses on PEN strategies for preparing novel noble metals and transition metal dichalcogenides (TMDs) with unconventional phases. It provides a comprehensive summary of crucial synthetic methods, such as direct synthesis and phase transformation, demonstrates their phase-dependent properties and catalytic performance, and highlights the significant impact of phase on the functions and applications of nanomaterials. Finally, we discuss the challenges and future directions for PEN, including in-depth studies on synthetic mechanisms, effective strategies to improve the stability of unconventional-phase nanomaterials, and innovative AI-aided structural design. These efforts aim to provide theoretical and technical guidance on both fundamental research and practical applications in the field of PEN.
Phase, which refers to the long-range ordered atomic arrangement, is one of the key parameters to determine the physicochemical properties and functions of nanomaterials. Recently, phase engineering of nanomaterials (PEN) has emerged as a promising research direction in materials science, since precise control over atomic arrangements enables the synthesis of nanomaterials with unconventional phases that are different from their thermodynamically stable counterparts, resulting in unique physicochemical properties. Therefore, PEN provides a new strategy for developing novel functional nanomaterials to enhance their performance in various applications. This review focuses on PEN strategies for preparing novel noble metals and transition metal dichalcogenides (TMDs) with unconventional phases. It provides a comprehensive summary of crucial synthetic methods, such as direct synthesis and phase transformation, demonstrates their phase-dependent properties and catalytic performance, and highlights the significant impact of phase on the functions and applications of nanomaterials. Finally, we discuss the challenges and future directions for PEN, including in-depth studies on synthetic mechanisms, effective strategies to improve the stability of unconventional-phase nanomaterials, and innovative AI-aided structural design. These efforts aim to provide theoretical and technical guidance on both fundamental research and practical applications in the field of PEN.
2026, 42(3): 100192
doi: 10.1016/j.actphy.2025.100192
Abstract:
2026, 42(3): 100205
doi: 10.1016/j.actphy.2025.100205
Abstract:
Login In
