Asymmetric Atomic Dual‐Sites for Photocatalytic CO2 Reduction

Abstract Atomically dispersed active sites in a photocatalyst offer unique advantages such as locally tuned electronic structures, quantum size effects, and maximum utilization of atomic species. Among these, asymmetric atomic dual‐sites are of particular interest because their asymmetric charge distribution generates a local built‐in electric potential to enhance charge separation and transfer. Moreover, the dual sites provide flexibility for tuning complex multielectron and multireaction pathways, such as CO 2 reduction reactions. The coordination of dual sites opens new possibilities for engineering the structure–activity–selectivity relationship. This comprehensive overview discusses efficient and sustainable photocatalysis processes in photocatalytic CO 2 reduction, focusing on strategic active‐site design and future challenges. It serves as a timely reference for the design and development of photocatalytic conversion processes, specifically exploring the utilization of asymmetric atomic dual‐sites for complex photocatalytic conversion pathways, here exemplified by the conversion of CO 2 into valuable chemicals.