物理化学学报最新文献

{"title":"Recent advances and challenges of eco-friendly Ni-rich cathode slurry systems in lithium-ion batteries","authors":"Rongrong Wang ,&nbsp;Chen Li ,&nbsp;Xiang Ren ,&nbsp;Keliang Zhang ,&nbsp;Yu Sun ,&nbsp;Xianzhong Sun ,&nbsp;Kai Wang ,&nbsp;Xiong Zhang ,&nbsp;Yanwei Ma","doi":"10.1016/j.actphy.2025.100222","DOIUrl":"10.1016/j.actphy.2025.100222","url":null,"abstract":"<div><div>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 <em>N</em>-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.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 4","pages":"Article 100222"},"PeriodicalIF":13.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006569","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Charge transfer mechanism investigation of S-scheme photocatalyst using soft X-ray absorption spectroscopy","authors":"Lingling Li,&nbsp;Zhe Chen","doi":"10.1016/j.actphy.2025.100215","DOIUrl":"10.1016/j.actphy.2025.100215","url":null,"abstract":"","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 4","pages":"Article 100215"},"PeriodicalIF":13.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006550","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tailored spin states: a transformative paradigm for sustainable catalysis","authors":"Wei Ren ,&nbsp;Jinhe Li ,&nbsp;Chengzhang Zhu ,&nbsp;Weikang Wang ,&nbsp;Qinqin Liu","doi":"10.1016/j.actphy.2025.100178","DOIUrl":"10.1016/j.actphy.2025.100178","url":null,"abstract":"<div><div>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<em>.</em>, Co₃O₄, Y₂Ru₂O₇), sulfides, alloys, and coordination compounds (e.g<em>.</em>, MOF-Co/Cu/Ni), we elucidate how targeted spin-state modulation—achieved <em>via</em> coordination engineering (doping/defect introduction, ligand regulation), valence modulation, size control (quantum confinement), and external stimuli (magnetic coupling)—dynamically tailors <em>d</em>-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.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 4","pages":"Article 100178"},"PeriodicalIF":13.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006551","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Machine learning potentials for property predictions of two-dimensional group-III nitrides","authors":"Jian Cao ,&nbsp;Chang Liu ,&nbsp;Danling Wang ,&nbsp;Haichao Li ,&nbsp;Lina Xu ,&nbsp;Hongping Xiao ,&nbsp;Shaoqi Zhan ,&nbsp;Xiao He ,&nbsp;Guoyong Fang","doi":"10.1016/j.actphy.2025.100224","DOIUrl":"10.1016/j.actphy.2025.100224","url":null,"abstract":"<div><div>Due to the hexagonal structure, thermal stability, and wide bandgap, two-dimensional group-III nitrides (<em>h</em>-BN, <em>h</em>-AlN, <em>h</em>-GaN and <em>h</em>-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. <em>h</em>-BN exhibits high strength but brittle fracture characteristics, while <em>h</em>-AlN and <em>h</em>-GaN demonstrate good strength and ductility. <em>h</em>-InN shows relatively weak overall mechanical performance. Non-equilibrium MD simulations on thermal conductivity reveal significant length-dependent effects in <em>h</em>-BN and <em>h</em>-AlN, attributed to longer phonon mean free paths. Enhanced phonon scattering in <em>h</em>-GaN and <em>h</em>-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.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 4","pages":"Article 100224"},"PeriodicalIF":13.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146025668","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Towards practical circularly polarized luminescence: Carbon dots-based circularly polarized lasers","authors":"Ting Li ,&nbsp;Xiao Zeng ,&nbsp;Yuzhuo Yang ,&nbsp;Xinyi Wen,&nbsp;Shurong Ding,&nbsp;Linlin Shi,&nbsp;Yongqiang Zhang,&nbsp;Siyu Lu","doi":"10.1016/j.actphy.2025.100191","DOIUrl":"10.1016/j.actphy.2025.100191","url":null,"abstract":"<div><div>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 (<em>g</em>), 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 <em>g</em> (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 <em>g</em>, 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.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 4","pages":"Article 100191"},"PeriodicalIF":13.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146076182","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"MOF-derived g-C3N4/ZnIn2S4 S-scheme heterojunction: Interface-engineering enhanced photocatalytic NO conversion","authors":"Yanping Qiu ,&nbsp;Jiatong Zhang ,&nbsp;Linping Li ,&nbsp;Yangqin Gao ,&nbsp;Ning Li ,&nbsp;Lei Ge","doi":"10.1016/j.actphy.2025.100175","DOIUrl":"10.1016/j.actphy.2025.100175","url":null,"abstract":"<div><div>Addressing the growing challenge of nitrogen oxides (NO_<em>x</em>) 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.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 4","pages":"Article 100175"},"PeriodicalIF":13.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006607","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"MOF/MOF nanosheets S-scheme heterojunction for accelerated charge kinetics and efficient photocatalytic H2 evolution","authors":"Danfeng Yi ,&nbsp;Yulin Li","doi":"10.1016/j.actphy.2025.100220","DOIUrl":"10.1016/j.actphy.2025.100220","url":null,"abstract":"","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 4","pages":"Article 100220"},"PeriodicalIF":13.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146025665","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Mitigate pressure dependence in sulfide-based all-solid-state batteries via structural and interfacial engineering of Ni-rich cathodes","authors":"Yajuan Zhang ,&nbsp;Jinliang Li ,&nbsp;Xi Zhang ,&nbsp;Yue Li ,&nbsp;Peng Sun ,&nbsp;Hao Xu ,&nbsp;Likun Pan","doi":"10.1016/j.actphy.2025.100204","DOIUrl":"10.1016/j.actphy.2025.100204","url":null,"abstract":"<div><div>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.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 4","pages":"Article 100204"},"PeriodicalIF":13.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006568","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Rational design of S-scheme CdS/MnO2 heterojunctions for high-value photothermal synergistic catalytic oxidation of toluene","authors":"Zhen Li,&nbsp;Sujuan Zhang,&nbsp;Zhongliao Wang,&nbsp;Jinfeng Zhang,&nbsp;Gaoli Chen,&nbsp;Shifu Chen","doi":"10.1016/j.actphy.2025.100179","DOIUrl":"10.1016/j.actphy.2025.100179","url":null,"abstract":"<div><div>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 °C. Mechanistic investigations via EPR and FT-IR 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.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 4","pages":"Article 100179"},"PeriodicalIF":13.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146025667","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Dual built-in electric field-driven S-scheme heterojunction of D-A COFs/ZnIn2S4 for accelerated charge separation toward high-efficiency H2O2 photosynthesis in pure water","authors":"Jie Guo,&nbsp;Lijun Xue,&nbsp;Fahui Song,&nbsp;Chengpeng Li,&nbsp;Zhuo Chen,&nbsp;Lili Wen","doi":"10.1016/j.actphy.2025.100177","DOIUrl":"10.1016/j.actphy.2025.100177","url":null,"abstract":"<div><div>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.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"42 4","pages":"Article 100177"},"PeriodicalIF":13.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146025666","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}