High-Power CO₂‑to‑C₂ Electroreduction on Ga-Spaced, Square-like Cu Sites
Date
2023
Authors
Yan, S.
Chen, Z.
Chen, Y.
Peng, C.
Ma, X.
Lv, X.
Qiu, Z.
Yang, Y.
Yang, Y.
Kuang, M.
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Journal Title
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Journal article
Citation
Journal of the American Chemical Society, 2023; 145(48):1-9
Statement of Responsibility
Shuai Yan, Zheng Chen, Yangshen Chen, Chen Peng, Xingyu Ma, Ximeng Lv, Zhehao Qiu, Yong Yang, Yaoyue Yang, Min Kuang, Xin Xu, and Gengfeng Zheng
Conference Name
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.
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© 2023 American Chemical Society