Catalytic Potential of Post‐Transition Metal Doped Graphene‐Based Single‐Atom Catalysts for the CO₂ Electroreduction Reaction

Abstract

Catalysts are required to ensure electrochemical reduction of CO₂ to fuels proceeds at industrially acceptable rates and yields. As such, highly active and selective catalysts must be developed. Herein, a density functional theory study of p-block element and noble metal doped graphene-based single-atom catalysts in two defect sites for the electrochemical reduction of CO₂ to CO and HCOOH is systematically undertaken. It is found that on all of the systems considered, the thermodynamic product is HCOOH. Pb/C₃ , Pb/N₄ and Sn/C₃ are identified as having the lowest overpotential for HCOOH production while Al/C₃ , Al/N₄ , Au/C₃ and Ga/C₃ are identified as having the potential to form higher order products due to the strength of binding of adsorbed HCOOH.