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Developing electrocatalytic reactions with high‐efficiency can make important contributions to carbon neutrality. However, poor long‐term stability of catalysts is a bottleneck for its practical application. Herein, an "in situ periodic regeneration of catalyst (PR‐C)" strategy is proposed to give long‐term high efficiency of CO2 electroreduction to generate C2+ products over Cu catalyst by applying a positive potential pulse for a short time periodically in the halide‐containing electrolyte. The high Faradaic efficiency (81.2 %) and current density (22.6 mA cm−2) could be maintained completely at least 36 h, while the activity and selectivity decreased continuously without using the PR‐C method. Control experiments and operando characterization demonstrated that the surface structure and oxidation state of Cu could be recovered periodically by the PR‐C method, which was beneficial for CO2 activation and C−C coupling. [ABSTRACT FROM AUTHOR]

Electrochemical reduction of CO2 by renewable electricity offers a promising way to settle excessive greenhouse gases and achieve carbon neutrality under a mild environment. Cu-based catalysts have a unique catalytic activity towards multicarbon (C2+) products in the CO2 electroreduction reaction and are widely studied to promote the corresponding selectivity and activity. Here we report a F-doped Cu (F–Cu) catalyst to improve C2+ products in CO2 electroreduction. A high C2+ product (mainly ethylene and ethanol) faradaic efficiency of 70.4% was achieved on the F–Cu catalyst with a high current density (above 400 mA cm−2) in the flow-cell system. The in situ surface enhanced Raman spectroscopy results and electrochemical performance analysis demonstrated that CO2 could be reduced into CO at low potentials and the adsorption of CO could be strengthened on F–Cu, which is beneficial to the subsequent C–C coupling step and formation of the C2+ products. [ABSTRACT FROM AUTHOR]