Periodic Single‐Metal Site Catalysts: Creating Homogeneous and Ordered Atomic‐Precision Structures

Abstract Heterogeneous single‐metal‐site catalysts (SMSCs), often referred to as single‐atom catalysts (SACs), demonstrate promising catalytic activity, selectivity, and stability across a wide spectrum of reactions due to their rationally designed microenvironments encompassing coordination geometry, binding ligands, and electronic configurations. However, the inherent disorderliness of SMSCs at both atomic scale and nanoscale poses challenges in deciphering working principles and establishing the correlations between microenvironments and the catalytic performances of SMSCs. The rearrangement of randomly dispersed single metals into homogeneous and atomic‐precisely structured periodic single‐metal site catalysts (PSMSCs) not only simplifies the chaos in SMSCs systems but also unveils new opportunities for manipulating catalytic performance and gaining profound insights into reaction mechanisms. Moreover, the synergistic effects of adjacent single metals and the integration effects of periodic single‐metal arrangement further broaden the industrial application scope of SMSCs. This perspective offers a comprehensive overview of recent advancements and outlines prospective avenues for research in the design and characterizations of PSMSCs, while also acknowledging the formidable challenges encountered and the promising prospects that lie ahead.