Efficient Electrocatalytic CO2 Reduction to C2+ Alcohols at Defect-Site-Rich Cu Surface

Electrochemical CO2 reduction is a promising approach for upgrading excessive CO2 into value-added chemicals, while the exquisite control of the catalyst atomic structures to obtain high C2+ alcohol selectivity has remained challenging due to the intrinsically favored ethylene pathways at Cu surface. Herein, we demonstrate a rational strategy to achieve similar to 70% faradaic efficiency toward C2+ alcohols. We utilized a CO-rich environment to construct Cu catalysts with stepped sites that enabled high surface coverages of *CO intermediates and the bridge-bound *CO adsorption, which allowed to trigger CO2 reduction pathways toward the formation alcohols. Using this defect-site-rich Cu catalyst, we achieved C2+ alcohols with partial current densities of > 100 mA.cm(-2) in both a flow-cell electrolyzer and a membrane electrode assembly (MEA) electrolyzer. A stable alcohol faradaic efficiency of similar to 60% was also obtained, with similar to 500 mg C2+ alcohol production per cm(2) catalyst during a continuous 30-h operation.

Automated summary

A rational strategy was demonstrated to achieve a high faradaic efficiency towards C2+ alcohols by constructing copper catalysts with stepped sites in a CO-rich environment. The defect-site-rich copper catalyst enabled the formation of C2+ alcohols with partial current densities of > 100 mA.cm(-2) and achieved a stable alcohol faradaic efficiency of around 60% during a continuous 30-hour operation.