ABSTRACT Spin catalysis offers a new perspective for developing highly efficient catalytic reactions by leveraging electron angular momentum—another fundamental parameter controlling the chemical reaction. Electron spin plays a critical role in reactions including but not limited to electrochemistry, photochemistry, and organic synthesis. However, the correlation between spin state and reaction efficiency remains incompletely elucidated, which hinders the advancement in this field. The unique capabilities of single‐molecule platforms enable real‐time spin‐state observation and precise manipulation, thus inspiring the exploration of their potential to advance spin catalysis. Accordingly, this perspective examines the prospects of single‐molecule platforms in spin catalysis, with the goal of fostering interdisciplinary research to elucidate the mechanism of spin catalysis and develop novel synthesis methodologies based on precise control of spin states. We first discuss the influence of electron spin on spin‐dependent reaction thermodynamics and kinetics, along with effective approaches to achieve spin manipulation. Building on this foundation, we summarize key challenges and opportunities in spin catalysis and evaluate the potential of single‐molecule platforms for mechanistic studies and precision synthesis in spin catalysis, including efficient spin injection, precise spin‐state detection, and coherent spin manipulation.
Huang et al. (Mon,) studied this question.