Theoretical modulation of Cu-based ternary alloys for the selectivity of electrochemical reduction of carbon dioxide

Utilizing electrochemical methods to convert carbon dioxide (CO2) into renewable energy and chemical raw materials is crucial for the development of sustainable technologies. However, the absence of catalysts with both high activity and high selectivity is a bottleneck hindering the progression of this technology. Here, a systematical exploration of the theoretical catalytic performance of CO2 reduction reaction on 276 Cu-based ternary alloys is conducted. The findings indicate that the cooperative effect of carbophilic elements adjusts the optimal adsorption capabilities of Cu sites for *CO, while oxophilic elements significantly enhance the selectivity for various products, exemplified by Cu2CoZn, Cu2FeAu, Cu2AlAu, and Cu2ZrBi for methane. Furthermore, the overall selectivity of C2 products is theoretically promising within these ternary alloys. This work not only sheds light on the relationship between ternary alloy composition and catalytic activity but also paves the way for the rational design of Cu-based catalysts.