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Surface plasmon of coinage metal nanostructures has been employed as a powerful route in boosting the performances in heterogenous catalysis. Development of efficient plasmonic nanocatalysts with high catalytic performance and efficient light harvesting properties is of vital importance. Herein, we rationally designed and synthesized a plasmonic nanocatalyst composed of Au-framed Pd nanocubes by an Ag(I)-assisted seed-mediated growth method. In the synthesis, the incorporation of Ag(I) suppresses the reduction of Au on the {100} surface of cubic Pd seeds and leads to the formation of Au nanoframes on the Pd nanocubes. The unique Au-framed Pd nanocubes can integrate the superior electrocatalytic of Pd and the outstanding plasmonic properties of Au. Thus, these nanostructures were employed as plasmonic nanocatalysts for plasmon-enhanced electrocatalytic oxidation of ethanol with improved stability.

Metallic heterogeneous nanostructures with plasmonic functionality have attracted great attention in the field of plasmon‐enhanced electrocatalysis, where surface plasmons produced under light excitation could facilitate the overall electrocatalytic performances. Owing to their controllability, multifunctionality, and complexity, heterogeneous metallic nanostructures take advantages of the properties from individual components and synergistic effects from adjacent components, thus may achieve remarkable electrocatalytic performances. This review highlights the state‐of‐the‐art progress of the application of metallic heterostructures for plasmon‐enhanced electrocatalysis. First, a brief introduction to plasmonic heterogeneous nanostructures is demonstrated. Then, fundamental principles of localized surface plasmon resonance and the underlying mechanisms of plasmonic heterogeneous nanostructures in catalysis are discussed. This is followed by a discussion of recent advances of plasmonic heterogeneous nanostructures in plasmon‐enhanced electrocatalysis, in which the enhanced activity, selectivity, and stability are particularly emphasized. Finally, an outlook of remaining challenges and future opportunities for plasmonic heterogeneous nanomaterials and plasmon‐related electrocatalysis is presented.