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Abstract The electrochemical reduction of CO 2 (CO 2 RR) mainly occurs at the three‐phase interface, and the properties of an interface can directly affect the CO 2 RR pathway. Cu‐based materials can produce considerable amounts of alcohols and hydrocarbons, but it is hard to precisely regulate the reaction interface and obtain specific target products. Herein, the properties of the Cu surface through a facile strategy of ionic liquid modification are successfully adjusted. According to theoretical calculations and in situ Raman and FTIR spectra characterizations, it is revealed that the introduction of ionic liquids (e.g., BmimPF 6 ) can control the energy barriers and distribution density of key intermediates on Cu interface, thus totally change the reaction pathway of CO 2 electroreduction. Consequently, the dominant products from the Cu catalyst will be dramatically switched between C 2 H 4 with a 71.1% Faraday efficiency (FE) and CH 4 with a 67.2% FE. It is rarely seen in previous reports that the CO 2 RR products can be fundamentally changed through simple interface modifications. This work offers a straightforward approach to tune the interfacial properties and understand the mechanisms in various electrocatalytic reactions.
Cai et al. (Mon,) studied this question.