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Copper-based nanomaterials are attractive in CO2 electroreduction into valuable chemicals but still suffer from limited selectivity of C2+ products due to the parasitic hydrogen evolution reaction and inefficient dimerization of absorbed CO intermediate (*CO). Herein, we report an in situ polymerization strategy to coat hydrophobic polymer containing methoxyl silane ((CH3O)3Si–) and trifluoromethyl (–CF3) functional groups on Cu nanoparticles. The optimized Cu-poly exhibits a high Faradaic efficiency of 71.08 % and a remarkable partial current density of 355.4 mA cm−2 for C2+ products in a membrane electrode assembly electrolyzer using a bicarbonate electrolyte. A combined study of density functional theory calculations and in situ infrared characterizations indicates that the enhanced performances could be ascribed to the decreased formation energy of *COCOH, induced by the withdraw-electron effect of –CF3 and enhanced coverage of *CO. This work offers a new insight in tuning the electrocatalytic microenvironment through the surface polymerization process.
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•Cu-poly catalysts are synthesized by in situ polymerization process.•Fluoric functional groups decrease the formation energy of *COCOH intermediates.•Hydrophobic coating limits the water wettability and increases the coverage of *CO.•Mechanism of enhanced C2 + selectivity on polymer-modified Cu is proposed.