Hetero-Interfaces on Cu Electrode for Enhanced Electrochemical Conversion of CO2 to Multi-Carbon Products

Electrochemical CO2 reduction reaction (CO2RR) to multi-carbon products would simultaneously reduce CO2 emission and produce high-value chemicals. Herein, we report Cu electrodes modified by metal-organic framework (MOF) exhibiting enhanced electrocatalytic performance to convert CO2 into ethylene and ethanol. The Zr-based MOF, UiO-66 would in situ transform into amorphous ZrOx nanoparticles (a-ZrOx), constructing a-ZrOx/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-ZrOx coating can promote the stabilization of atop-bound CO* intermediates on Cu surface during CO2 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 CO2RR intermediate by designing dual-site electrocatalysts with hetero-interfaces.