Theoretical Understanding of the Interface Effect in Promoting Electrochemical CO2 Reduction on Cu-Pd Alloys

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 C-2 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 C-1 products. The interface between Cu and Pd domains promotes the C-C bond coupling and the subsequent formation of C-2 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.

Automated summary

Bimetallic Cu-Pd alloys exhibit excellent activity and selectivity for the electrochemical conversion of CO2, with the interface effect promoting the formation of C-C bonds and subsequent C-2 products. Theoretical simulations comparing ordered and phase-separated Cu-Pd alloys provide insights into the catalytic mechanism and potential for designing efficient Cu-based alloy catalysts for the electrochemical CO2RR.