While copper-based electrocatalysts are strong contenders for the electrochemical reduction of CO2 (ERCO2) to C1 products (CO and formic acid) as feedstock for the energy and industry, their selectivity is a tricky issue. Herein, we propose a strategy to modulate the selectivity by equipped with various functional groups (N–, G–, −COOH, −NH2, and −OH) to affect the adsorption of key intermediates on the surface of Cu-based electrocatalysts. Among these as-prepared catalysts, the catalysts equipped with N– and −OH functional groups show excellent catalytic performance for ERCO2 with nearly 90% selectivities for C1 products. Moreover, the N– functional group has favorable formate selectivity when compared with the pristine Cu-based electrocatalyst. By investigating the catalysts’ electrochemical performance, it is demonstrated that the interactions between functional groups and catalytic active sites are critical in regulating the catalytic selectivity of electrocatalysts. According to economic feasibility analysis, it is further proven that this design principle can be applied on a larger scale.

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