Heteroatom-doped C3N as a promising metal-free catalyst for a high-efficiency carbon dioxide reduction reaction

Converting CO(2)into useful fuels and chemicals offers a promising strategy for mitigating the issues of energy crisis and global warming. However, it is still a fundamental challenge to find highly efficient catalysts for the CO(2)electrochemical reduction (CO2ER) reaction. In this work, the catalytic performance of heteroatom (B, P, Si, and S)-doped C3N materials as metal-free CO2ER electrocatalysts was investigated by means of density functional theory (DFT) calculations. The results reveal that these heteroatom-doped C3N materials exhibit high stability. On the basis of the calculated Gibbs free energies, B-N-doped C3N exhibits superior CO2ER catalytic activity for CO(2)reduction to HCOOH with a low overpotential of 0.14 Vvs.RHE. The present work demonstrates the promising potential of B-N-doped C3N as an active and selective CO2ER catalyst, and provides an effective strategy for electrochemical applications.