Transition metal doped C3N monolayer as efficient electrocatalyst for carbon dioxide electroreduction: A computational study

Recently, two-dimensional graphitic carbon nitrides have emerged as potential electrocatalysts for CO2 electroreduction (CO2ER). Herein, a series of transition metal (M = Mn-Cu, Ru-Ag) doped C3N monolayer (M-C3N) as a novel CO2ER catalyst has been investigated by employing the density functional method. By a careful computational screening, Mn-C3N is identified as the best catalyst for CO2ER, due to its high catalytic activity and high selectivity. HCOOH is the final product with a low overpotential of 0.04 V and a low kinetic energy barrier of 0.75 eV. The hydrogen evolution is also suppressed on Mn-C3N surface. Therefore, the CO2ER activity could be tuned by adjusting the metal atom in the C3N monolayer, which may shed new light on designing novel C3N-based CO2ER catalyst.

Automated summary

In this study, a series of transition metal-doped C3N monolayers were investigated as potential electrocatalysts for CO2 electroreduction (CO2ER) using density functional method. Mn-C3N was identified as the best catalyst for CO2ER, with high catalytic activity and selectivity for producing HCOOH while suppressing hydrogen evolution. Adjusting the metal atom in the C3N monolayer can tune the CO2ER activity, offering new insights for designing novel C3N-based CO2ER catalysts.