Theoretical Understanding of the Interface Effect in Promoting Electrochemical CO<sub>2</sub> Reduction on Cu–Pd Alloys
Yanle Li, Ziqi Tian, Liang Chen
Abstract
The electrochemical conversion of CO2 holds promise to relieve the excess CO2 emission and store renewable energy. Bimetallic copper-based alloys show outstanding activity and selectivity for the electrochemical CO2 reduction reaction (CO2RR). Understanding the catalytic nature of Cu-based alloys may promote the development of high-performance CO2RR electrocatalysts. The interface in the bimetallic system plays a key role in gaining C2 products in experiments. Here, we performed theoretical simulations to compare the activity of ordered and phase-separated Cu–Pd alloy catalysts for CO2 conversion. The reaction pathways to CO, CH4, C2H4, and C2H5OH are analyzed in detail to uncover the interface effect. Our calculation shows that the ordered Cu–Pd surface is favorable for the formation of C1 products. The interface between Cu and Pd domains promotes the C–C bond coupling and the subsequent formation of C2 products. This study provides insights into the catalytic mechanism of the bimetallic system and will be beneficial for designing efficient Cu-based alloy catalysts for the electrochemical CO2RR.