Unraveling the Selectivity and Synergistic Mechanism of Cu-Based Alloys for CO2 Reduction

Understanding the synergistic effect of Cu-based alloyson theadsorption behavior and selectivity of the CO2 reductionreaction is a crucial step toward directional catalyst design. Tothis end, density functional theory calculations are employed to investigateCu-based alloys with diverse doping elements and contents. The resultsshow that the scaling relation still holds in the alloy system, andthe strategies to improve the selectivity are put forward based onthe adsorption strength of *C and *OCHO intermediates. Further, amodel combining the adsorption theory and machine learning algorithmis proposed to capture the relationship between the adsorption energyand the geometric environment. It explains that the difference ind-band centers between the doped metals and Cu affects the variationtrend of the adsorption strength and reveals that the intermetallicsynergistic effect can be quantified by the bonding distance and dorbital radius on both the adsorbate and metal side.