Mg-Doped Cu Catalyst for Electroreduction of CO to Multicarbon Products: Lewis Acid Sites Simultaneously Promote *CO Adsorption and Water Dissociation.

The electroreduction of CO to valuable fuels or high-value chemicals by using sustainable electric energy provides a promising strategy for solving environmental problems dominated by the greenhouse effect. Copper-based materials are the only catalysts that can convert CO into multicarbon products, but they are plagued by high potential, low selectivity, and poor stability. The key factors to optimize the conversion of CO into multicarbon products are to improve the adsorption capacity of intermediates on the catalyst surface, accelerate the hydrogenation step, and improve the C-C coupling efficiency. Herein, we successfully doped Lewis acid Mg into Cu-based materials using a simple liquid-phase chemical method. In situ Raman and FT-IR tracking show that the Mg site enhances the surface coverage of the *CO intermediate, simultaneously promoting water dissociation. Under an industrial current density of 0.7 A cm, the FE reaches 73.9 ± 3.48% with remarkable stability. Density functional theory studies show that doping the Lewis acid Mg site increases the coverage of *CO and accelerates the splitting of water, thus promoting the C-C coupling efficiency, reducing the reaction energy barrier, and greatly improving the selectivity of C products.