Heterostructure Engineering in High‐Entropy Alloy Catalysts

ABSTRACT Confronting the limitation of traditional homogeneous high‐entropy alloys (HEAs) with randomly distributed elements and active sites, heterostructured HEAs were developed to further amplify catalytic activity and stability. This perspective dissects the genesis of heterogeneity within HEAs, highlighting how their expansive compositional space facilitates the customization of heterogeneity. By manipulating key factors, such as chemical affinity, standard redox potentials, and oxidation potential, researchers are tapping into heterostructured HEAs with unprecedented attributes. Strategies like acid leaching, galvanic replacement, and additive deposition are broadening the structural repertoire of HEAs, steering the development of heterostructured catalysts. This perspective synthesizes current discoveries, introduces provocative concepts, and provides a roadmap for structural engineering in HEA catalysts, particularly harnessing the heterogeneity of HEAs to elevate their catalytic efficiency. The confluence of theoretical and practical advancements is anticipated to lead the way in the evolution of HEA catalysts, endowing them with exceptional capabilities.