Modulating the localized electronic distribution of Cu species during reconstruction for enhanced electrochemical CO2 reduction to C2+ products

Electrochemical conversion of carbon dioxide (CO2RR) into high-value multi-carbon (C2+) chemicals and fuels is of great significance for carbon neutrality, and so far Cu-based materials are still the dominant electrocatalysts with practical application potential for C2+ products during the CO2RR. However, Cu-based catalysts usually face problems such as an unstable valence state and lattice structure, low efficiency, and a narrow potential window for C2+ products which affect the comprehensive performance of the catalysts. Herein, we develop a simple co-precipitation-hydrothermal method for introducing zirconium dioxide (ZrO2) into copper oxide (CuO) to improve the selectivity of C2+ products via in situ reconstruction. The optimized CuO-ZrO2-1.0 catalyst exhibits a high faradaic efficiency of 82.3% for C2+ products with an industrial partial current density over 200 mA cm(-2), which presents a more than 1.7-fold improvement compared to that of CuO, also exceeding that of lots of Cu-based catalysts previously reported. DFT and in situ characterization studies reveal that the introduction of ZrO2 can induce the electronic distribution and stabilize the Cu+ species during the in situ reconstruction process which contributes to moderate adsorption and enhanced coupling of *CO intermediates to obtain C2+ products.