Abstract
<h2>Summary</h2> Electrochemical reduction of CO<sub>2</sub> to value-added multicarbon products has been limited by the inefficiency of the C–C coupling process on Cu. Coupling metal oxides with Cu surfaces offers new freedom to break scaling relationships, thus regulating the product distribution on Cu. Herein, we show that metal oxides with the capability to stabilize the adsorbed CO<sub>2</sub>∗/CO∗ and decrease the Gibbs free energies of the C–C coupling process can promote the formation of C<sub>2+</sub> products on oxide-modified Cu electrodes. As a representative, ZrO<sub>2</sub>-modified Cu (Cu/ZrO<sub>2</sub>) electrode shows a high faradic efficiency of 85% for C<sub>2+</sub> products. <i>In situ</i> surface-enhanced Raman spectra confirm the enhanced adsorption of CO∗ on the Cu/ZrO<sub>2</sub> electrode, while theoretical calculations reveal the decreased energy barriers of the C–C coupling process at the Cu-ZrO<sub>2</sub> interfacial boundaries. This study sheds light on the structure-property relationship of metal-oxide heterostructured electrocatalysts and accelerates the implementation of CO<sub>2</sub> electroreduction toward high-value products.
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