High-Power CO2-to-C2 Electroreduction on Ga-Spaced, Square-like Cu Sites

Shuai Yan; Zheng Chen; Yangshen Chen; Chen Peng; Xingyu Ma; Ximeng Lv; Zhehao Qiu; Yong Yang; Yaoyue Yang; Min Kuang; Xin Xu; Gengfeng Zheng

doi:10.1021/jacs.3c10202

High-Power CO₂-to-C₂ Electroreduction on Ga-Spaced, Square-like Cu Sites

J Am Chem Soc. 2023 Dec 6;145(48):26374-26382. doi: 10.1021/jacs.3c10202. Epub 2023 Nov 22.

Authors

Shuai Yan¹, Zheng Chen¹, Yangshen Chen¹, Chen Peng¹, Xingyu Ma², Ximeng Lv¹, Zhehao Qiu³, Yong Yang³, Yaoyue Yang², Min Kuang⁴, Xin Xu^{1

5

6}, Gengfeng Zheng¹

Affiliations

¹ Laboratory of Advanced Materials, Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, China.
² Key Laboratory of General Chemistry of the National Ethnic Affairs Commission, School of Chemistry and Environment, Southwest Minzu University, Chengdu, Sichuan Province 610041, China.
³ School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China.
⁴ State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China.
⁵ MOE Key Laboratory of Computational Physical Sciences, Fudan University, Shanghai 200433, China.
⁶ Hefei National Laboratory, Hefei 230088, China.

PMID: 37992232
DOI: 10.1021/jacs.3c10202

Abstract

The electrochemical conversion of CO₂ into multicarbon (C₂) products on Cu-based catalysts is strongly affected by the surface coverage of adsorbed CO (*CO) intermediates and the subsequent C-C coupling. However, the increased *CO coverage inevitably leads to strong *CO repulsion and a reduced C-C coupling efficiency, thus resulting in suboptimal CO₂-to-C₂ activity and selectivity, especially at ampere-level electrolysis current densities. Herein, we developed an atomically ordered Cu₉Ga₄ intermetallic compound consisting of Cu square-like binding sites interspaced by catalytically inert Ga atoms. Compared to Cu(100) previously known with a high C₂ selectivity, the Ga-spaced, square-like Cu sites presented an elongated Cu-Cu distance that allowed to reduce *CO repulsion and increased *CO coverage simultaneously, thus endowing more efficient C-C coupling to C₂ products than Cu(100) and Cu(111). The Cu₉Ga₄ catalyst exhibited an outstanding CO₂-to-C₂ electroreduction, with a peak C₂ partial current density of 1207 mA cm^-2 and a corresponding Faradaic efficiency of 71%. Moreover, the Cu₉Ga₄ catalyst demonstrated a high-power (∼200 W) electrolysis capability with excellent electrochemical stability.