Adjusting *CO adsorption configuration over tandem trimetallic AuAgCu heterojunction boosts CO2 electroreduction to ethanol via asymmetric C-C coupling

IF 6.8 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Science China Materials Pub Date : 2024-11-18 DOI:10.1007/s40843-024-3162-2

Yongxia Shi (, ), Junjun Li (, ), Zhiwen Min (, ), Xinyi Wang (, ), Man Hou (, ), Hao Ma (, ), Zechao Zhuang (, ), Yuchen Qin (, ), Yuanmiao Sun (, ), Dingsheng Wang (, ), Zhicheng Zhang (, )

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引用次数: 0

Abstract

Rationally modulating the adsorption configuration of the key *CO intermediate could facilitate carbon-carbon (C-C) coupling to generate multi-carbon products in the electrochemical CO₂ reduction reaction. In this work, theoretical calculations reveal that C-C coupling via atop-adsorbed *CHO and hollow-adsorbed *CO over Cu sites is an energetically favorable pathway. As a proof of concept, a tandem trimetallic AuAgCu heterojunction (Au@Ag/Cu) was prepared, where the atop-adsorbed *CO over Au@Ag sites could migrate to Cu sites with hollow adsorption configuration, and then the asymmetric C-C coupling via transferred hollow-adsorbed *CO and existed atop-adsorbed *CHO over Cu sites facilitates the formation of the ethanol product, exhibiting a maximum Faraday efficiency of 65.9% at a low potential of −0.3 V vs. reverse hydrogen electrode. Our work provides new insights into the intrinsic understanding of tandem catalysis by regulating adsorption configuration of the intermediate products.

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来源期刊

Science China Materials Materials Science-General Materials Science

CiteScore

11.40

自引率

7.40%

发文量

949

期刊介绍： Science China Materials (SCM) is a globally peer-reviewed journal that covers all facets of materials science. It is supervised by the Chinese Academy of Sciences and co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China. The journal is jointly published monthly in both printed and electronic forms by Science China Press and Springer. The aim of SCM is to encourage communication of high-quality, innovative research results at the cutting-edge interface of materials science with chemistry, physics, biology, and engineering. It focuses on breakthroughs from around the world and aims to become a world-leading academic journal for materials science.