Hetero-Interfaces on Cu Electrode for Enhanced Electrochemical Conversion of CO(2) to Multi-Carbon Products

Electrochemical CO(2) reduction reaction (CO(2)RR) to multi-carbon products would simultaneously reduce CO(2) emission and produce high-value chemicals. Herein, we report Cu electrodes modified by metal–organic framework (MOF) exhibiting enhanced electrocatalytic performance to convert CO(2) into ethylene and ethanol. The Zr-based MOF, UiO-66 would in situ transform into amorphous ZrO(x) nanoparticles (a-ZrO(x)), constructing a-ZrO(x)/Cu hetero-interface as a dual-site catalyst. The Faradaic efficiency of multi-carbon (C2+) products for optimal UiO-66-coated Cu (0.5-UiO/Cu) electrode reaches a high value of 74% at − 1.05 V versus RHE. The intrinsic activity for C2+ products on 0.5-UiO/Cu electrode is about two times higher than that of Cu foil. In situ surface-enhanced Raman spectra demonstrate that UiO-66-derived a-ZrO(x) coating can promote the stabilization of atop-bound CO* intermediates on Cu surface during CO(2) electrolysis, leading to increased CO* coverage and facilitating the C–C coupling process. The present study gives new insights into tailoring the adsorption configurations of CO(2)RR intermediate by designing dual-site electrocatalysts with hetero-interfaces. [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-022-00879-5.