物理化学学报2026，Vol.42Issue(4)：13-38,26.DOI:10.1016/j.actphy.2025.100178
精准调控自旋态:可持续催化领域的创新理念
Tailored spin states:a transformative paradigm for sustainable catalysis
摘要
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.关键词
自旋控制/催化反应/自旋调控方法/表征技术Key words
Spin controlling/Catalytic reaction/Spin modulation method/Characterization technique分类
化学化工引用本文复制引用
任伟,李金河,朱成章,王伟康,刘芹芹..精准调控自旋态:可持续催化领域的创新理念[J].物理化学学报,2026,42(4):13-38,26.基金项目
国家自然科学基金(22472069,22302080) （22472069,22302080）
中国博士后科学基金(2024M760028)和江苏省研究生科研与实践创新计划项目(KYCX25_4194)资助 （2024M760028）
