Shaping Single-Crystalline Trimetallic Pt–Pd–Rh Nanocrystals toward High-Efficiency C–C Splitting of Ethanol in Conversion to CO2

Abstract

Atomic-scale construction and high-throughput screening of robust multicomponent nanocatalysts with tunable well-defined surface structures and associated active sites for the ethanol electro-oxidation reaction (EOR) in high activity and selectivity, referring to C–C bond cleavage and full oxidation of ethanol as a clean and sustainable energy source, has remained a great challenge. Herein, we demonstrate a powerful conceptual approach to design, synthesize, and optimize single-crystalline Pt–Pd–Rh nanocrystals of altered shapes and compositions for enhanced EOR performance, based on combined density functional theory (DFT) calculations and experiment study. We prepared (111)-terminated Pt–Pd–Rh nanotruncated-octahedrons (NTOs) and (100)-terminated Pt–Pd–Rh nanocubes (NCs) with varied-compositions by regulating the reduction tendency of metal precursors in a facile hydrothermal method. Aided by DFT calculations, Pt3PdRh NTOs, PtPdRh NTO, and 8.8 nm PtPdRh NCs-200 were screened to be the best performing ca...