Charge Redistribution of Atomic Catalysts in Electrocatalysis

ABSTRACT Atomic catalysts, through their atomic‐level dispersion achieving maximize atomic utilization, unique electronic structure and coordination environment, designability and multi‐functionality, as well as high selectivity, demonstrate advantages over traditional catalysts in terms of catalytic efficiency, cost‐effectiveness and sustainability. Charge redistribution reveals the structure–activity relationship of atomic catalysts in electrocatalysis from the perspective of electronic structure. Here, we summarize charge redistribution effect of atomic catalysts in electrocatalysis, including orbital hybridization, electronic metal–support interaction, spin state transition and charge transfer, along with descriptors and methods that reveal charge redistribution in atomic catalysts, as evidenced by techniques such as differential charge density, Bader charge analysis, electronic configuration and electron localization function and ab initio molecular dynamics. Next, we focus on identifying inducing factors involving transition from single‐atom sites to dual‐atom/multi‐atom sites, asymmetric micro‐environment, vacancy defects, strain and reaction conditions that drive charge redistribution of atomic catalysts in electrocatalysis, followed by an introduction to the potential applications in energy storage and conversion devices. Finally, we present our personal perspective on the obstacles in the future that still need to be addressed and overcome in elucidating the structure–activity relationship from the perspective of charge redistribution in atomic catalysts for electrocatalysis.