High-Power CO<sub>2</sub>-to-C<sub>2</sub> Electroreduction on Ga-Spaced, Square-like Cu Sites
Shuai Yan, Zheng Chen, Yangshen Chen, Peng Chen, Xingyu Ma, Ximeng Lv, Zhehao Qiu, Yong Yang, Yao‐Yue Yang, Min Kuang, Xin Xu, Gengfeng Zheng
Abstract
The electrochemical conversion of CO 2 into multicarbon (C 2 ) 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 CO 2 -to-C 2 activity and selectivity, especially at ampere-level electrolysis current densities. Herein, we developed an atomically ordered Cu 9 Ga 4 intermetallic compound consisting of Cu square-like binding sites interspaced by catalytically inert Ga atoms. Compared to Cu(100) previously known with a high C 2 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 C 2 products than Cu(100) and Cu(111). The Cu 9 Ga 4 catalyst exhibited an outstanding CO 2 -to-C 2 electroreduction, with a peak C 2 partial current density of 1207 mA cm –2 and a corresponding Faradaic efficiency of 71%. Moreover, the Cu 9 Ga 4 catalyst demonstrated a high-power (∼200 W) electrolysis capability with excellent electrochemical stability.