Mechanistic insights into high-throughput screening of tandem catalysts for CO2 reduction to multi-carbon products

Abstract

In carbon dioxide electrochemical reduction (CO₂ER), since isolated catalysts encounter challenges in meeting the demands of intricate processes for producing multi-carbon (C₂₊) products, tandem catalysis is emerging as a promising approach. Nevertheless, there remains an insufficient theoretical understanding of designing tandem catalysts. Herein, we utilized density functional theory (DFT) to screen 80 tandem catalysts for efficient CO₂ER to C₂ products systematically, which combines the advantages of nitrogen-doped carbon-supported transition metal single-atom catalysts (M–N–C) and copper clusters. Three crucial criteria were designed to select structures for generation and transfer of *CO and facilitate C–C coupling. The optimal Cu/RuN₄-pl catalyst exhibited an excellent ethanol production capacity. Additionally, the relationship between CO adsorption strength and transfer energy barrier was established, and the influence of the electronic structure on its adsorption strength was studied. This provided a novel and well-considered solution and theoretical guidance for the design of rational composition and structurally superior tandem catalysts.