A Universal Descriptor for Complicated Interfacial Effects on Electrochemical Reduction Reactions

Supported catalysts have exhibited excellent performance in various reactions. However, the rational design of supported catalysts with high activity and certain selectivity remains a great challenge because of the complicated interfacial effects. Using recently emerged two-dimensional materials supported dual-atom catalysts (DACs@2D) as a prototype, we propose a simple and universal descriptor based on inherent atomic properties (electronegativity, electron type, and number), which can well evaluate the complicated interfacial effects on the electrochemical reduction reactions (i.e., CO2, O-2, and N-2 reduction reactions). Based on this descriptor, activity and selectivity trends in CO2 reduction reaction are successfully elucidated, in good agreement with available experimental data. Moreover, several potential catalysts with superior activity and selectivity for target products are predicted, such as CuCr/g-C3N4 for CH4 and CuSn/N-BN for HCOOH. More importantly, this descriptor can also be extended to evaluate the activity of DACs@2D for O-2 and N-2 reduction reactions, with very small errors between the prediction and reported experimental/computational results. This work provides feasible principles for the rational design of advanced electrocatalysts and the construction of universal descriptors based on inherent atomic properties.

Automated summary

In this study, a simple and universal descriptor based on inherent atomic properties was proposed for evaluating the complicated interfacial effects on electrochemical reduction reactions. The activity and selectivity trends in CO2 reduction reaction were successfully elucidated, and several potential catalysts with superior activity and selectivity were predicted. Furthermore, the descriptor was also extended to evaluate the activity of dual-atom catalysts for O-2 and N-2 reduction reactions.