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2026 Volume 42 Issue 4
2026, 42(4):
Abstract:
2026, 42(4): 100171
doi: 10.1016/j.actphy.2025.100171
Abstract:
The concurrent production of hydrogen (H2) and high-value products from waste and toxic hydrogen sulfide (H2S) has long been a goal in the field of photocatalytic decomposition of H2S. In this study, the twinned Mn0.5Cd0.5S (T-MCS) was selected for its combination of solid solution and twin structure advantages, significantly promoting the bulk phase separation of CdS-based photocatalysts. Furthermore, the highly conductive nickel disulfide (NiS2) was loaded onto T-MCS to create a NiS2/T-MCS composite photocatalyst that features both a bulk phase S-scheme homojunction and an interface Schottky junction. NiS2 not only introduces a large number of active sites, but also improves the separation of surface charges obviously. Utilizing a 0.1 mol L−1 (M) sodium sulfide (Na2S) and 0.6 M anhydrous sodium sulfite (Na2SO3) solution saturated with H2S as the reaction solution, the 8 wt% NiS2/T-MCS composite achieves a remarkable hydrogen production rate of up to 59.95 mmol h−1 g−1. Fourier Transform Infrared (FTIR) spectroscopy and Ultraviolet-Visible (UV-Vis) spectroscopy confirm that the sulfur compounds in the reaction solution are nearly completely converted into high-value sodium thiosulfate (Na2S2O3). The S2O32− was also quantitatively determined by titration. This work presents a novel solid solution twin crystal-based homojunction and Schottky junction for both the photocatalytic treatment of H2S and the production of Na2S2O3.
The concurrent production of hydrogen (H2) and high-value products from waste and toxic hydrogen sulfide (H2S) has long been a goal in the field of photocatalytic decomposition of H2S. In this study, the twinned Mn0.5Cd0.5S (T-MCS) was selected for its combination of solid solution and twin structure advantages, significantly promoting the bulk phase separation of CdS-based photocatalysts. Furthermore, the highly conductive nickel disulfide (NiS2) was loaded onto T-MCS to create a NiS2/T-MCS composite photocatalyst that features both a bulk phase S-scheme homojunction and an interface Schottky junction. NiS2 not only introduces a large number of active sites, but also improves the separation of surface charges obviously. Utilizing a 0.1 mol L−1 (M) sodium sulfide (Na2S) and 0.6 M anhydrous sodium sulfite (Na2SO3) solution saturated with H2S as the reaction solution, the 8 wt% NiS2/T-MCS composite achieves a remarkable hydrogen production rate of up to 59.95 mmol h−1 g−1. Fourier Transform Infrared (FTIR) spectroscopy and Ultraviolet-Visible (UV-Vis) spectroscopy confirm that the sulfur compounds in the reaction solution are nearly completely converted into high-value sodium thiosulfate (Na2S2O3). The S2O32− was also quantitatively determined by titration. This work presents a novel solid solution twin crystal-based homojunction and Schottky junction for both the photocatalytic treatment of H2S and the production of Na2S2O3.
2026, 42(4): 100175
doi: 10.1016/j.actphy.2025.100175
Abstract:
Addressing the growing challenge of nitrogen oxides (NOx) pollution in the atmosphere requires the development of photocatalysts with both high efficiency and strong selectivity. In this study, a g-C3N4/ZnIn2S4 (CN/ZIS) S-scheme heterojunction photocatalyst was constructed, in which ZnIn2S4 with a hollow tubular morphology was synthesized via a MOF-derived strategy, and g-C3N4 served as an efficient electron transfer platform. The optimized CN/ZIS-0.1 exhibited remarkable photocatalytic efficacy under visible-light radiation, attaining a NO removal efficiency of 67.29%, markedly surpassing that of pristine g-C3N4 (41.41%) and ZIS (27.8%). Additionally, a high NO-to-nitrate selectivity of 77.47% was attained, exceeding that of pristine g-C3N4 (49.01%). The material characterization results revealed that CN/ZIS-0.1 not only has a wider light absorption range but also its unique structure provides more reaction sites. Further photoelectrochemical measurements and DFT simulations confirm that the built-in electric field (BIEF) formed at the CN/ZIS interface facilitates the directional migration of photogenerated electrons towards the g-C3N4 surface, and photogenerated holes migrate towards the surface of ZIS, thereby promoting the generation of key reactive species and enhancing NO adsorption. This work not only demonstrates the potential of constructing S-scheme heterojunctions by coupling MOF-derived hollow structures with two-dimensional semiconductors for NO oxidation, but also offers an effective strategy for developing highly selective NO photocatalysts.
Addressing the growing challenge of nitrogen oxides (NOx) pollution in the atmosphere requires the development of photocatalysts with both high efficiency and strong selectivity. In this study, a g-C3N4/ZnIn2S4 (CN/ZIS) S-scheme heterojunction photocatalyst was constructed, in which ZnIn2S4 with a hollow tubular morphology was synthesized via a MOF-derived strategy, and g-C3N4 served as an efficient electron transfer platform. The optimized CN/ZIS-0.1 exhibited remarkable photocatalytic efficacy under visible-light radiation, attaining a NO removal efficiency of 67.29%, markedly surpassing that of pristine g-C3N4 (41.41%) and ZIS (27.8%). Additionally, a high NO-to-nitrate selectivity of 77.47% was attained, exceeding that of pristine g-C3N4 (49.01%). The material characterization results revealed that CN/ZIS-0.1 not only has a wider light absorption range but also its unique structure provides more reaction sites. Further photoelectrochemical measurements and DFT simulations confirm that the built-in electric field (BIEF) formed at the CN/ZIS interface facilitates the directional migration of photogenerated electrons towards the g-C3N4 surface, and photogenerated holes migrate towards the surface of ZIS, thereby promoting the generation of key reactive species and enhancing NO adsorption. This work not only demonstrates the potential of constructing S-scheme heterojunctions by coupling MOF-derived hollow structures with two-dimensional semiconductors for NO oxidation, but also offers an effective strategy for developing highly selective NO photocatalysts.
2026, 42(4): 100177
doi: 10.1016/j.actphy.2025.100177
Abstract:
The construction of dual built-in electric field (IEF)-driven S-scheme heterojunctions presents a promising strategy to accelerate efficient charge separation and improve charge utilization in photocatalytic H2O2 production. Herein, we report, the construction of a heterojunction based on donor-acceptor covalent organic frameworks (D-A COFs) TpAQ (synthesized from two monomers: 1, 3, 5-triformylphloroglucinol (Tp) and 2, 6-diaminoanthraquinone (AQ)) and ZnIn2S4 (ZIS), realizing a dual IEF-driven S-scheme heterojunction—one from the heterojunction interface and another from D-A interface within D-A COFs. In particular, the optimized TpAQ/ZIS-10 exhibits a significantly higher visible-light driven photocatalytic H2O2 production rate of 2362 μmol g−1 h−1 in pure water than TpAQ and ZIS by utilizing both the oxygen reduction reaction and water oxidation reaction pathways. Furthermore, the experimental results and theoretical calculations revealed that the synergistic effect of dual IEF in TpAQ/ZIS heterojunction significantly facilitates efficient charge carrier transfer and separation. This work provides valuable insight for constructing highly efficient S-scheme heterojunctions with dual IEF.
The construction of dual built-in electric field (IEF)-driven S-scheme heterojunctions presents a promising strategy to accelerate efficient charge separation and improve charge utilization in photocatalytic H2O2 production. Herein, we report, the construction of a heterojunction based on donor-acceptor covalent organic frameworks (D-A COFs) TpAQ (synthesized from two monomers: 1, 3, 5-triformylphloroglucinol (Tp) and 2, 6-diaminoanthraquinone (AQ)) and ZnIn2S4 (ZIS), realizing a dual IEF-driven S-scheme heterojunction—one from the heterojunction interface and another from D-A interface within D-A COFs. In particular, the optimized TpAQ/ZIS-10 exhibits a significantly higher visible-light driven photocatalytic H2O2 production rate of 2362 μmol g−1 h−1 in pure water than TpAQ and ZIS by utilizing both the oxygen reduction reaction and water oxidation reaction pathways. Furthermore, the experimental results and theoretical calculations revealed that the synergistic effect of dual IEF in TpAQ/ZIS heterojunction significantly facilitates efficient charge carrier transfer and separation. This work provides valuable insight for constructing highly efficient S-scheme heterojunctions with dual IEF.
2026, 42(4): 100179
doi: 10.1016/j.actphy.2025.100179
Abstract:
The targeted partial oxidation of toluene to valuable products continues to present a significant hurdle in catalytic science. To address the low efficiency of conventional photocatalysis, we developed a photothermal synergistic strategy by constructing a novel S-scheme CdS/MnO2 heterojunction catalyst. CdS nanoparticles were anchored onto MnO2, a material with intrinsic photothermal activity, forming a compact S-scheme heterojunction. This architecture generates an intrinsic electric field that markedly accelerates the segregation of light-induced charge carriers and inhibits their recombination. Moreover, CdS incorporation modulates the electronic band structure of MnO2, thereby improving product selectivity. Owing to these synergistic effects, the optimized 25% CdS/MnO2 catalyst demonstrated excellent catalytic performance, attaining a toluene oxidation rate of 14.1 mmol g−1 h−1 with an impressive 90% selectivity toward benzyl alcohol and benzaldehyde under an oxygen atmosphere at 150 ℃. Mechanistic investigations via Electron Paramagnetic Resonance and Fourier Transform Infrared Spectroscopy analyses revealed the pivotal role of photothermal synergy in promoting the oxidation process. This work not only provides an effective strategy for designing advanced photothermal heterojunctions but also presents new insights into the selective oxidation of toluene under mild conditions.
The targeted partial oxidation of toluene to valuable products continues to present a significant hurdle in catalytic science. To address the low efficiency of conventional photocatalysis, we developed a photothermal synergistic strategy by constructing a novel S-scheme CdS/MnO2 heterojunction catalyst. CdS nanoparticles were anchored onto MnO2, a material with intrinsic photothermal activity, forming a compact S-scheme heterojunction. This architecture generates an intrinsic electric field that markedly accelerates the segregation of light-induced charge carriers and inhibits their recombination. Moreover, CdS incorporation modulates the electronic band structure of MnO2, thereby improving product selectivity. Owing to these synergistic effects, the optimized 25% CdS/MnO2 catalyst demonstrated excellent catalytic performance, attaining a toluene oxidation rate of 14.1 mmol g−1 h−1 with an impressive 90% selectivity toward benzyl alcohol and benzaldehyde under an oxygen atmosphere at 150 ℃. Mechanistic investigations via Electron Paramagnetic Resonance and Fourier Transform Infrared Spectroscopy analyses revealed the pivotal role of photothermal synergy in promoting the oxidation process. This work not only provides an effective strategy for designing advanced photothermal heterojunctions but also presents new insights into the selective oxidation of toluene under mild conditions.
2026, 42(4): 100189
doi: 10.1016/j.actphy.2025.100189
Abstract:
Lithium ferrate Li5FeO4 is a promising cathode prelithiation additive for lithium-ion batteries, boasting a high theoretical capacity of 867 mAh g−1, which compensates for lithium loss due to solid electrolyte interphase (SEI) formation during the initial cycle. However, its practical application faces significant challenges due to inherent chemical instability. The material is extremely sensitive to air, readily undergoing deleterious side reactions with atmospheric carbon dioxide and moisture to form electrochemically inert Li2CO3 surface layers. This degradation in the atmosphere presents several major issues. It not only substantially reduces active lithium content but also induces severe slurry gelation during electrode manufacturing. In addition, it promotes continuous gas generation and electrolyte decomposition during battery operation, and leads to a significant increase in electrochemical impedance. Previous stabilization attempts via carbon coating or metal doping have shown limited success, often introducing new problems such as capacity reduction or inadequate protection, highlighting the urgent need for a more comprehensive and effective modification method. To address these challenges, this study proposes an efficient Lewis acid-induced regeneration strategy through thermal modification with PF5. This approach effectively removes surface inert impurities and facilitates the in-situ construction of a composite layer of Li3PO4 and LiF on the Li5FeO4 particles. The regenerated Li5FeO4 exhibits excellent dispersion, air stability, and electrolyte interfacial compatibility, effectively suppressing slurry gelation and interfacial side reactions. In comparison with the bare counterpart, the regenerated Li5FeO4 shows a significantly reduced viscosity upon slurry processing and gas generation during high-temperature storage. When 1.5% (wt) regenerated Li5FeO4 is introduced to the LiFePO4 cathode in the full cells, the cathode maintains a high capacity of 135.0 mAh g−1 and a retention rate of 95.3% after 200 cycles. In contrast, the control LiFePO4 cathode without Li5FeO4 only retains 113.7 mAh g−1 with a capacity retention of 92.2%. This approach integrates impurity removal, interfacial stabilization, and performance enhancement of Li5FeO4 into one strategy, which will find extensive applications in long-cycle lithium-ion batteries.
Lithium ferrate Li5FeO4 is a promising cathode prelithiation additive for lithium-ion batteries, boasting a high theoretical capacity of 867 mAh g−1, which compensates for lithium loss due to solid electrolyte interphase (SEI) formation during the initial cycle. However, its practical application faces significant challenges due to inherent chemical instability. The material is extremely sensitive to air, readily undergoing deleterious side reactions with atmospheric carbon dioxide and moisture to form electrochemically inert Li2CO3 surface layers. This degradation in the atmosphere presents several major issues. It not only substantially reduces active lithium content but also induces severe slurry gelation during electrode manufacturing. In addition, it promotes continuous gas generation and electrolyte decomposition during battery operation, and leads to a significant increase in electrochemical impedance. Previous stabilization attempts via carbon coating or metal doping have shown limited success, often introducing new problems such as capacity reduction or inadequate protection, highlighting the urgent need for a more comprehensive and effective modification method. To address these challenges, this study proposes an efficient Lewis acid-induced regeneration strategy through thermal modification with PF5. This approach effectively removes surface inert impurities and facilitates the in-situ construction of a composite layer of Li3PO4 and LiF on the Li5FeO4 particles. The regenerated Li5FeO4 exhibits excellent dispersion, air stability, and electrolyte interfacial compatibility, effectively suppressing slurry gelation and interfacial side reactions. In comparison with the bare counterpart, the regenerated Li5FeO4 shows a significantly reduced viscosity upon slurry processing and gas generation during high-temperature storage. When 1.5% (wt) regenerated Li5FeO4 is introduced to the LiFePO4 cathode in the full cells, the cathode maintains a high capacity of 135.0 mAh g−1 and a retention rate of 95.3% after 200 cycles. In contrast, the control LiFePO4 cathode without Li5FeO4 only retains 113.7 mAh g−1 with a capacity retention of 92.2%. This approach integrates impurity removal, interfacial stabilization, and performance enhancement of Li5FeO4 into one strategy, which will find extensive applications in long-cycle lithium-ion batteries.
2026, 42(4): 100224
doi: 10.1016/j.actphy.2025.100224
Abstract:
Due to the hexagonal structure, thermal stability, and wide bandgap, two-dimensional group-Ⅲ nitrides (h-BN, h-AlN, h-GaN and h-InN) show great promise for electronic and optoelectronic applications. Density functional theory (DFT) and classical molecular dynamics (MD) methods have advantages in calculation accuracy and scale respectively, but they are limited in the application of high-precision large-scale structure and performance research. Herein, we employ deep potential (DP) method to construct a high-precision machine learning potential (MLP) and systematically investigate the lattice dynamics, thermodynamic, mechanical, and thermal transport properties of two-dimensional Group Ⅲ nitrides. The DP method can achieve DFT accuracy in energy and atomic force predictions and accurately reproduce phonon dispersion and thermodynamic functions (free energy, heat capacity, entropy) across the 0–1200 K temperature range. MD simulations of uniaxial tensiles reveal distinct mechanical behavior differences among materials. h-BN exhibits high strength but brittle fracture characteristics, while h-AlN and h-GaN demonstrate good strength and ductility. h-InN shows relatively weak overall mechanical performance. Non-equilibrium MD simulations on thermal conductivity reveal significant length-dependent effects in h-BN and h-AlN, attributed to longer phonon mean free paths. Enhanced phonon scattering in h-GaN and h-InN results in lower thermal conductivities. These findings demonstrate that the DP method combines DFT accuracy with large-scale simulation capabilities can deepen understanding of structures and properties of two-dimensional Group Ⅲ nitrides and provide a computational framework and theoretical foundations for material design and device application.
Due to the hexagonal structure, thermal stability, and wide bandgap, two-dimensional group-Ⅲ nitrides (h-BN, h-AlN, h-GaN and h-InN) show great promise for electronic and optoelectronic applications. Density functional theory (DFT) and classical molecular dynamics (MD) methods have advantages in calculation accuracy and scale respectively, but they are limited in the application of high-precision large-scale structure and performance research. Herein, we employ deep potential (DP) method to construct a high-precision machine learning potential (MLP) and systematically investigate the lattice dynamics, thermodynamic, mechanical, and thermal transport properties of two-dimensional Group Ⅲ nitrides. The DP method can achieve DFT accuracy in energy and atomic force predictions and accurately reproduce phonon dispersion and thermodynamic functions (free energy, heat capacity, entropy) across the 0–1200 K temperature range. MD simulations of uniaxial tensiles reveal distinct mechanical behavior differences among materials. h-BN exhibits high strength but brittle fracture characteristics, while h-AlN and h-GaN demonstrate good strength and ductility. h-InN shows relatively weak overall mechanical performance. Non-equilibrium MD simulations on thermal conductivity reveal significant length-dependent effects in h-BN and h-AlN, attributed to longer phonon mean free paths. Enhanced phonon scattering in h-GaN and h-InN results in lower thermal conductivities. These findings demonstrate that the DP method combines DFT accuracy with large-scale simulation capabilities can deepen understanding of structures and properties of two-dimensional Group Ⅲ nitrides and provide a computational framework and theoretical foundations for material design and device application.
2026, 42(4): 100178
doi: 10.1016/j.actphy.2025.100178
Abstract:
Amid escalating global sustainability pressures and energy-environmental crises, catalytic innovation has reached a pivotal inflection point. Electron spin manipulation emerges as a transformative paradigm, fundamentally rewiring reaction pathways at the quantum level, transcending classical electronic and geometric constraints. This review frames spin-engineered active centers as molecular spin switches, governing orbital symmetry matching, spin-polarized electron transfer, and transition-state energy landscapes. Covering diverse catalytic materials including metal oxides (e.g., Co3O4, Y2Ru2O7), sulfides, alloys, and coordination compounds (e.g., MOF-Co/Cu/Ni), we elucidate how targeted spin-state modulation—achieved via coordination engineering (doping/defect introduction, ligand regulation), valence modulation, size control (quantum confinement), and external stimuli (magnetic coupling)—dynamically tailors d-orbital occupancy to optimize intermediate adsorption and overcome thermodynamic scaling limitations. Critically, these engineered spin configurations mediate accelerated charge-transfer kinetics, thereby expediting rate-determining steps and elevating overall catalytic performance. By integrating advanced spin-sensitive characterization with theoretical calculation, this review summarizes how precisely tailored high- and low-spin states yield unprecedented enhancements in key reactions such as oxygen reduction, CO2 reduction, hydrogen evolution, urea synthesis, and battery-related reactions. The perspective advances an innovation framework where nonequilibrium spin control and spin-coherent catalysis will pioneer next-generation sustainable energy technologies.
Amid escalating global sustainability pressures and energy-environmental crises, catalytic innovation has reached a pivotal inflection point. Electron spin manipulation emerges as a transformative paradigm, fundamentally rewiring reaction pathways at the quantum level, transcending classical electronic and geometric constraints. This review frames spin-engineered active centers as molecular spin switches, governing orbital symmetry matching, spin-polarized electron transfer, and transition-state energy landscapes. Covering diverse catalytic materials including metal oxides (e.g., Co3O4, Y2Ru2O7), sulfides, alloys, and coordination compounds (e.g., MOF-Co/Cu/Ni), we elucidate how targeted spin-state modulation—achieved via coordination engineering (doping/defect introduction, ligand regulation), valence modulation, size control (quantum confinement), and external stimuli (magnetic coupling)—dynamically tailors d-orbital occupancy to optimize intermediate adsorption and overcome thermodynamic scaling limitations. Critically, these engineered spin configurations mediate accelerated charge-transfer kinetics, thereby expediting rate-determining steps and elevating overall catalytic performance. By integrating advanced spin-sensitive characterization with theoretical calculation, this review summarizes how precisely tailored high- and low-spin states yield unprecedented enhancements in key reactions such as oxygen reduction, CO2 reduction, hydrogen evolution, urea synthesis, and battery-related reactions. The perspective advances an innovation framework where nonequilibrium spin control and spin-coherent catalysis will pioneer next-generation sustainable energy technologies.
2026, 42(4): 100191
doi: 10.1016/j.actphy.2025.100191
Abstract:
Circularly polarized luminescence (CPL) has significant application value in fields such as quantum computing, three-dimensional (3D) display, and bioimaging. However, its practical application faces challenges including low dissymmetry factor (g), insufficient quantum yield, poor directionality, and broad emission spectrum. To address these issues, circularly polarized laser technology can significantly enhance CPL performance through stimulated emission amplification and resonant cavity mode selection, achieving circularly polarized light output with high g (close to the theoretical limit of 2), high brightness, narrow linewidth, and strong directionality. Currently, although materials like organic microcrystals and perovskites can realize circularly polarized laser with high g, they still have problems such as complex preparation and poor biocompatibility. In contrast, carbon dots (CDs) have emerged as a highly promising new type of circularly polarized gain medium due to their advantages of simple preparation, low cost, low toxicity, easy modification, and good biocompatibility. This paper systematically reviews the material systems, device types, and application progress of circularly polarized laser, focusing on the advantages of CDs as gain media and their potential in fields such as 3D display, optical communication, information encryption, and biosensing. It also prospects the future development directions and challenges of CDs-based circularly polarized lasers, providing a reference for promoting the practical application process of high-performance circularly polarized laser devices.
Circularly polarized luminescence (CPL) has significant application value in fields such as quantum computing, three-dimensional (3D) display, and bioimaging. However, its practical application faces challenges including low dissymmetry factor (g), insufficient quantum yield, poor directionality, and broad emission spectrum. To address these issues, circularly polarized laser technology can significantly enhance CPL performance through stimulated emission amplification and resonant cavity mode selection, achieving circularly polarized light output with high g (close to the theoretical limit of 2), high brightness, narrow linewidth, and strong directionality. Currently, although materials like organic microcrystals and perovskites can realize circularly polarized laser with high g, they still have problems such as complex preparation and poor biocompatibility. In contrast, carbon dots (CDs) have emerged as a highly promising new type of circularly polarized gain medium due to their advantages of simple preparation, low cost, low toxicity, easy modification, and good biocompatibility. This paper systematically reviews the material systems, device types, and application progress of circularly polarized laser, focusing on the advantages of CDs as gain media and their potential in fields such as 3D display, optical communication, information encryption, and biosensing. It also prospects the future development directions and challenges of CDs-based circularly polarized lasers, providing a reference for promoting the practical application process of high-performance circularly polarized laser devices.
2026, 42(4): 100204
doi: 10.1016/j.actphy.2025.100204
Abstract:
Sulfide-based all-solid-state lithium-ion batteries (ASSLIBs) have emerged as one of the most promising candidates for next-generation energy storage systems owing to their high energy density, wide electrochemical stability window, and intrinsic safety benefits over liquid electrolyte counterparts. Nevertheless, their practical implementation faces a fundamental bottleneck: the strong dependence on high external stack pressure to maintain interfacial contact and suppress mechanical degradation during operation. This requirement not only reduces energy efficiency and packaging flexibility but also severely restricts scalability and commercialization, as maintaining uniform high pressure in large-format cells is technically challenging and economically costly. Addressing the critical challenge of achieving low-pressure or even ambient-pressure operation in sulfide-based ASSLIBs is therefore of both scientific and technological significance. In this review, we systematically analyze the origins of pressure-dependent performance, including particle fracture in Ni-rich layered cathodes, dynamic interfacial instability, and insufficient mechanical compliance of composite electrodes. Building on this mechanistic understanding, we summarize recent advances and design strategies across multiple scales. At the cathode level, particle size regulation, compositional doping, and engineered porosity, combined with conformal interfacial coatings, effectively mitigate stress concentration and suppress degradation. On the electrolyte and electrode interface, optimizing particle size distribution, tailoring interfacial chemistry, and introducing dynamic polymeric binders with balanced adhesion and elasticity significantly enhance ionic transport and maintain robust contact under low pressure. At the system level, strategies such as optimized temperature management, adjustment of the electrochemical window, and controlled isostatic pressure provide additional means to stabilize operation and complement materials-level solutions. Taken together, these advances demonstrate that the key to pressure-independent ASSLIBs lies in a synergistic design framework that integrates intrinsic materials engineering, interfacial stabilization, and system-level control. We further propose a cross-scale design roadmap toward the realization of low-pressure and flexible ASSLIBs, highlighting the need for dynamic adaptation between mechanical properties and electrochemical processes. This perspective underscores that enabling stable performance under minimized external pressure is not only essential for translating laboratory demonstrations into practical large-scale devices but also paves the way for safer, lighter, and more energy-efficient solid-state battery technologies.
Sulfide-based all-solid-state lithium-ion batteries (ASSLIBs) have emerged as one of the most promising candidates for next-generation energy storage systems owing to their high energy density, wide electrochemical stability window, and intrinsic safety benefits over liquid electrolyte counterparts. Nevertheless, their practical implementation faces a fundamental bottleneck: the strong dependence on high external stack pressure to maintain interfacial contact and suppress mechanical degradation during operation. This requirement not only reduces energy efficiency and packaging flexibility but also severely restricts scalability and commercialization, as maintaining uniform high pressure in large-format cells is technically challenging and economically costly. Addressing the critical challenge of achieving low-pressure or even ambient-pressure operation in sulfide-based ASSLIBs is therefore of both scientific and technological significance. In this review, we systematically analyze the origins of pressure-dependent performance, including particle fracture in Ni-rich layered cathodes, dynamic interfacial instability, and insufficient mechanical compliance of composite electrodes. Building on this mechanistic understanding, we summarize recent advances and design strategies across multiple scales. At the cathode level, particle size regulation, compositional doping, and engineered porosity, combined with conformal interfacial coatings, effectively mitigate stress concentration and suppress degradation. On the electrolyte and electrode interface, optimizing particle size distribution, tailoring interfacial chemistry, and introducing dynamic polymeric binders with balanced adhesion and elasticity significantly enhance ionic transport and maintain robust contact under low pressure. At the system level, strategies such as optimized temperature management, adjustment of the electrochemical window, and controlled isostatic pressure provide additional means to stabilize operation and complement materials-level solutions. Taken together, these advances demonstrate that the key to pressure-independent ASSLIBs lies in a synergistic design framework that integrates intrinsic materials engineering, interfacial stabilization, and system-level control. We further propose a cross-scale design roadmap toward the realization of low-pressure and flexible ASSLIBs, highlighting the need for dynamic adaptation between mechanical properties and electrochemical processes. This perspective underscores that enabling stable performance under minimized external pressure is not only essential for translating laboratory demonstrations into practical large-scale devices but also paves the way for safer, lighter, and more energy-efficient solid-state battery technologies.
2026, 42(4): 100222
doi: 10.1016/j.actphy.2025.100222
Abstract:
Ni-rich layered cathodes have become the mainstream choice to meet the growing demand for high-energy lithium-ion batteries (LIBs), which typically involves the use of highly polar N-methyl-2-pyrrolidone (NMP) to dissolve polymeric binders and form rheologically stable slurries for strong mechanical adhesion within the electrode. However, growing health and environmental concerns over NMP have triggered increasingly stringent regulations for sustainable development of LIB industries, thereby accelerating a long-overdue paradigm shift toward greener and safer solvent systems. In this context, this review first establishes a comprehensive theoretical framework for green solvent selection and slurry evaluation, including key concepts of solvent-binder compatibility, such as solubility theory, Hansen solubility parameters, Flory-Huggins interactions, and rheological characterization. Subsequently, the review highlights recent research progress in the development of green solvent-based slurries, covering a variety of solvent systems such as lactones, sulfoxides, phosphates, amides, and bio-based alternatives. Special emphasis is placed on elucidating how the processing behavior of green slurry influences the architecture of electrodes and determines their key performance indicators. Binder solubility, dispersion stability, rheological properties, and drying dynamics are analyzed in relation to their effects on electrode morphology, mechanical cohesion, capacity retention, and cycling stability. Despite encouraging laboratory results, these green slurry systems still face several practical barriers, including incomplete binder dissolution, binder migration during drying, and limited adaptability to high-solid-content formulations and accelerated drying protocols. To address these challenges, this review also proposes corresponding mitigation strategies and design recommendations, including thermodynamic-based solvent screening, rheological optimization, and drying kinetics control tailored to Ni-rich electrode systems. Finally, by integrating the latest advances in artificial intelligence, this review outlines future directions for predictable green slurry systems enabled by techniques such as machine learning-assisted solubility prediction, data-driven rheology modeling, and numerical model-enhanced drying simulations. By combining classical theoretical insights with advanced computational strategies, this review is expected to provide new perspectives for the sustainable manufacturing of next-generation high-energy batteries.
Ni-rich layered cathodes have become the mainstream choice to meet the growing demand for high-energy lithium-ion batteries (LIBs), which typically involves the use of highly polar N-methyl-2-pyrrolidone (NMP) to dissolve polymeric binders and form rheologically stable slurries for strong mechanical adhesion within the electrode. However, growing health and environmental concerns over NMP have triggered increasingly stringent regulations for sustainable development of LIB industries, thereby accelerating a long-overdue paradigm shift toward greener and safer solvent systems. In this context, this review first establishes a comprehensive theoretical framework for green solvent selection and slurry evaluation, including key concepts of solvent-binder compatibility, such as solubility theory, Hansen solubility parameters, Flory-Huggins interactions, and rheological characterization. Subsequently, the review highlights recent research progress in the development of green solvent-based slurries, covering a variety of solvent systems such as lactones, sulfoxides, phosphates, amides, and bio-based alternatives. Special emphasis is placed on elucidating how the processing behavior of green slurry influences the architecture of electrodes and determines their key performance indicators. Binder solubility, dispersion stability, rheological properties, and drying dynamics are analyzed in relation to their effects on electrode morphology, mechanical cohesion, capacity retention, and cycling stability. Despite encouraging laboratory results, these green slurry systems still face several practical barriers, including incomplete binder dissolution, binder migration during drying, and limited adaptability to high-solid-content formulations and accelerated drying protocols. To address these challenges, this review also proposes corresponding mitigation strategies and design recommendations, including thermodynamic-based solvent screening, rheological optimization, and drying kinetics control tailored to Ni-rich electrode systems. Finally, by integrating the latest advances in artificial intelligence, this review outlines future directions for predictable green slurry systems enabled by techniques such as machine learning-assisted solubility prediction, data-driven rheology modeling, and numerical model-enhanced drying simulations. By combining classical theoretical insights with advanced computational strategies, this review is expected to provide new perspectives for the sustainable manufacturing of next-generation high-energy batteries.
2026, 42(4): 100215
doi: 10.1016/j.actphy.2025.100215
Abstract:
2026, 42(4): 100216
doi: 10.1016/j.actphy.2025.100216
Abstract:
2026, 42(4): 100220
doi: 10.1016/j.actphy.2025.100220
Abstract:
