Conjugating plasmonic metals with catalytically active materials with controlled configurations can harness their light energy harvesting ability in catalysis. Herein, we present a well-defined core-shell nanostructure composed of an octahedral Au nanocrystal core and a PdPt alloy shell as a bifunctional energy conversion platform for plasmon-enhanced electrocatalysis. The prepared Au@PdPt core-shell nanostructures exhibited significant enhancements in electrocatalytic activity for methanol oxidation and oxygen reduction reactions under visible-light irradiation. Our experimental and computational studies revealed that the electronic hybridization of Pd and Pt allows the alloy material to have a large imaginary dielectric function, which can efficiently induce the shell-biased distribution of plasmon energy upon illumination and, hence, its relaxation at the catalytically active region to promote electrocatalysis.
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