Ga-Modification Near-Surface Composition of Pt–Ga/C Catalyst Facilitates High-Efficiency Electrochemical Ethanol Oxidation through a C2 Intermediate

• DOI: 10.1021/jacs.3c04320
• Publication Date: 2023-07-26T07:57:51Z
• Authors: Wei Yan; Guang Li; Shuangshuang Cui; Gyeong-Su Park; Rena Oh; Weixin Chen; Xiaoyang Cheng; Jun-Ming Zhang; Weize Li; Li-Fei Ji; Ouardia Akdim; Xiaoyang Huang; Haixin Lin; Jian Yang; Yan-Xia Jiang; Shi-Gang Sun

In electrochemical ethanol oxidation reactions (EOR) catalyzed by Pt metal nanoparticles through a C2 route, the dissociation of C-C bond in molecule can be limiting factor. Complete EOR processes producing CO2 were always exemplified oxidative dehydrogenation C1 intermediates, reaction route with less energy utilization efficiency. Here, we report Pt3Ga/C electrocatalyst uniform distribution Ga over nanoparticle surface for that produces at medium potentials (>0.3 V vs SCE) efficiently direct and sustainable intermediate species, i.e., acetaldehyde. We demonstrate excellent performance Pt3Ga-200/C catalyst using situ Fourier transform infrared reflection spectroscopy (FTIR) an isotopic labeling method. The atomic interval structure between makes nonensembled, avoiding formation poisonous *CHx *CO species via bridge-type adsorption molecules. Meanwhile, electron redistribution from to diminishes *O/*OH CO poisoning on atoms, exposing more available sites interaction intermediates. Furthermore, H2O into *OH is facilitated high hydrophilicity Ga, which supported DFT calculations, promoting deep Our work represents extremely rare process without observing kinetic limitations under potential conditions.