Abstract Electrochemical conversion of CO2 to valuable fuels is appealing for CO2 fixation and energy storage. The Cu‐based catalysts feature unique superiorities, but achieving high ethylene selectivity is still restricted. In this study, we propose the anchoring of an ionic liquid (IL) on a Cu electrocatalyst for improving the electrochemical CO2 reduction to ethylene. In a water‐based electrolyte and a commonly used H‐type cell, a high ethylene Faradaic efficiency of 77.3?% was achieved at ?1.49?V (vs. RHE). Experimental and theoretical studies reveal that an IL can modify the electronic structure of a Cu catalyst through its interaction with Cu, making it more conducive to *CO dimerization for ethylene formation.
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