Optimizing photocatalysis via electron spin control.

Solar-driven photocatalytic technology holds significant potential for addressing energy crisis and mitigating global warming, yet is limited by light absorption, charge separation, and surface reaction kinetics. The past several years has witnessed remarkable progress in optimizing photocatalysis via electron spin control. This approach enhances light absorption through energy band tuning, promotes charge separation by spin polarization, and improves surface reaction kinetics via strengthening surface interaction and increasing product selectivity. Nevertheless, the lack of a comprehensive and critical review on this topic is noteworthy. Herein, we provide a summary of the fundamentals of electron spin control and the techniques employed to scrutinize the electron spin state of active sites in photocatalysts. Subsequently, we highlight advanced strategies for manipulating electron spin, including doping design, defect engineering, magnetic field regulation, metal coordination modulation, chiral-induced spin selectivity, and combined strategies. Additionally, we review electron spin control-optimized photocatalytic processes, including photocatalytic water splitting, CO₂ reduction, pollutant degradation, and N₂ fixation, providing specific examples and detailed discussion on underlying mechanisms. Finally, we outline perspectives on further enhancing photocatalytic activity through electron spin manipulation. This review seeks to offer valuable insights to guide future research on electron spin control for improving photocatalytic applications.