Yan, S.Chen, Z.Chen, Y.Peng, C.Ma, X.Lv, X.Qiu, Z.Yang, Y.Yang, Y.Kuang, M.Xu, X.Zheng, G.2024-01-122024-01-122023Journal of the American Chemical Society, 2023; 145(48):1-90002-78631520-5126https://hdl.handle.net/2440/140355The 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.en© 2023 American Chemical SocietyAdsorption; Catalysts; Electrocatalysts; Electrolysis; Evolution reactionsJournal article10.1021/jacs.3c102022023-11-26677222Peng, C. [0000-0003-2767-7698]