Atomic Diffusion Engineered PtSnCu Nanoframes with High‐Index Facets Boost Ethanol Oxidation

Abstract

AbstractElectrochemical ethanol oxidation is crucial to directly convert a biorenewable liquid fuel with high energy density into electrical energy, but it remains as an inefficient reaction even with the best catalysts. To boost ethanol oxidation, developing multimetallic nanoalloy has emerged as one of the most effective strategies, yet faces a challenge in the rational engineering of multimetallic active‐site ensembles at atomic‐level. Herein, starting from typical PtCu nanocrystals, we developed an atomic Sn diffusion strategy to construct well‐defined Pt47Sn12Cu41 octopod nanoframes, which is enclosed by high‐index facets of n (111)‐(111), such as {331} and {221}. Benefiting from this ternary active‐site ensembles with enlarged lattice spacings and multiple high‐index facets, Pt47Sn12Cu41 achieves a high mass activity of 3.10 A mg−1Pt and promotes the C‐C bond breaking and oxidation of poisonous CO intermediate, representing a state‐of‐the‐art electrocatalyst toward ethanol oxidation in acidic electrolyte. Density functional theory calculations have confirmed that the introduction of Sn improves the electroactivity by uplifting the d‐band center through the s‐p‐d coupling. Meanwhile, the strong binding of ethanol and the reduced energy barrier of CO oxidation guarantee a highly efficient ethanol oxidation process with improved Faradic efficiency of C1 products. This work offers a promising strategy for constructing novel multimetallic nanoalloys tailored by atomic metal sites as the efficient electrocatalysts.This article is protected by copyright. All rights reserved