精准调控自旋态:可持续催化领域的创新理念OA

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.