First-principles calculations on Rh loaded BC3N2 for understanding the mechanism of electrocatalytic reduction of CO2

Transition metals modified to enhance the performance of electrocatalytic reduction of carbon dioxide (CO2) has received significant attention. In this work, a novel high-efficiency electrocatalyst Rh-BC3N2 has been constructed and simulated using first-principles calculations to reveal the mechanism of enhanced electrocatalytic reduction of CO2. Our results reveal that Rh atom can be stably supported on top of N site of BC3N2 monolayer. For CO2 activation, CO2 was activated to a bent structure with the bond angle OI-C-OII of 146.0 degrees, resulting of the charge transfer between CO2 molecule and Rh-BC3N2. And for CO2 reduction, the rate-determining step for the formation of CH3OH is *CO hydrogenation into *CHO, and the overpotential for *COOH hydrogenation into HCOOH is 0.23 V. Our work provides a promising candidate for the CO2 reutilization, with valuable insights and an important prototype for future practical design.

Automated summary

In this study, a novel high-efficiency electrocatalyst Rh-BC3N2 was constructed and simulated using first-principles calculations to reveal the mechanism behind the enhanced electrocatalytic reduction of CO2. The results show that Rh atom can be stably supported on top of N site of BC3N2 monolayer. The research provides a promising candidate for CO2 reutilization and valuable insights for future practical design.