Electrochemical CO2 Reduction to Ethanol on Zn‐Coordinated Cu Sites Formed by Atmosphere‐Induced Surface Reconstruction

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AbstractElectrochemical CO2 reduction reaction (CO2RR) to produce chemicals and fuels is a promising strategy to achieve carbon neutrality. However, due to the slow C─C coupling kinetics and the fact that C2H5OH and C2H4 products share the same *HCCOH intermediate, achieving high activity and selectivity for C2H5OH remains challenging. This paper describes an atmosphere‐induced reconstruction method to optimize the surface composition and coordination structure of the CuxZny bimetallic alloy catalysts for C2H5OH production. Specifically, the CuxZny alloy catalyst treated within CO atmosphere (CO‐CuxZny) enriches with low‐coordinated Cu sites, which are favorable for the adsorption of the *CO intermediates for promoted C2H5OH production. A C2+ Faradaic efficiency (FE) of 85.1% and a C2H5OH FE of 59.5% are achieved by the CO‐Cu84Zn16 at a current density of 300 mA cm−2. In‐situ spectroscopic studies and DFT calculations demonstrate that the enhanced *CO adsorption promotes the C─C coupling process. At the same time, the hydrogenation of *HCCOH is more favorable on CO‐Cu84Zn16 to inhibit the C2H4 pathway, thus enhancing the generation of C2H5OH. This study provides an effective strategy to regulate the selectivity of CO2RR through the control of the surface coordination environment of the active sites.