Design and synthesis of magnesium-modified copper oxide nanosheets as efficient electrocatalysts for CO2 reduction

Abstract

Electroreduction of carbon dioxide (CO₂) to multiple carbon products plays a significant role in carbon neutrality and the production of valuable chemicals. Herein, we developed a magnesium-modified copper oxide nanosheet catalyst (Mg–CuO) using a post-impregnation method. Comprehensive elemental analysis demonstrated the effective incorporation of magnesium into CuO nanosheets, resulting in a noticeable alteration of the electron density of Cu atoms. Consequently, the Mg–CuO nanosheets exhibited an increased efficiency for CO₂ electroreduction in comparison with the unmodified CuO nanosheets. The optimized Mg–CuO catalyst exhibited faradaic efficiencies of 46.33% for ethylene production and 62.64% for C₂₊ production at −1.3 V vs. reversible hydrogen electrode (RHE). DFT proved that the introduction of Mg species could increase the charge density of Cu and decrease the adsorption energy of *CO, which promoted C–C coupling and enhanced the selectivity of C₂₊ products. This study presents an effective way to adjust the electronic structure of common copper-based electrocatalysts and the corresponding interaction with *CO, resulting in an improved faradaic efficiency of C₂₊ products.