The Emergence of Spin-Enhanced Catalysis for CO2 Conversion.

Spin catalysis provides a new opportunity to overcome conventional performance limits in carbon dioxide (CO2) conversion by exploiting spin-dependent charge transfer and radical reaction pathways. A clear understanding of spin effects and effective strategies for spin regulation is therefore essential for advancing CO2 conversion catalysis. This review briefly summarizes recent advances in the underlying mechanisms and a few representative examples of spin-enhanced CO2 conversion, highlighting their importance in steering CO2 conversion toward high value-added products. It begins with an introduction to spin-dependent reaction pathways and spin regulation at catalytic active sites, followed by a discussion of emerging approaches for spin-enhanced CO2 conversion. Spin catalysis strategies based on external magnetic fields and internal magnetic interactions are presented, highlighting their roles in promoting photocatalytic and electrocatalytic CO2 reduction toward diverse and value-added products. Besides, in situ/operando characterization techniques are essential for exploring the underlying mechanisms of spin catalysis and tracking the spin-sensitive reaction intermediates during CO2 conversion. Finally, key challenges and future opportunities in the design of spin catalysts, as well as the reactor engineering for practical applications, are discussed, advancing the concept of spin catalysis for achieving sustainable CO2 conversion.