Manipulating Interfaces of Electrocatalysts Down to Atomic Scales: Fundamentals, Strategies, and Electrocatalytic Applications

Abstract Raising electrocatalysis by rationally devising catalysts plays a core role in almost all renewable energy conversion and storage systems. The principal catalytic properties can be controlled and improved well by manipulation of interfaces, ascribed to the interactions among different components/players at the interfaces. In particular, manipulating interfaces down to atomic scales is becoming increasingly attractive, not only because those atoms at around the interface are the key players during electrocatalysis, but also, understandings on the atomic level electrocatalysis allow one to gain deep insights into the reaction mechanism. With the feature down‐sizing to atomic scales, there is a timely need to redefine the interfaces, as some of them have gone beyond the conventionally perceived interfacial concept. In this overview, the key active players participating in the interfacial manipulation of electrocatalysts are examined, from a new angle of “atomic interface,” including those individual atoms, defects, and their interactions, together with the essential characterization techniques for them. The specific approaches and pathways to engineer better atomic interfaces are investigated, and thus to enable the unique electrocatalysis for targeted applications. Looking beyond recent progress, the challenges and prospects of the atomic level interfacial engineering are also briefly visited.