Catalytic role of graphitic nitrogen atoms in the CO oxidation reaction over N-containing graphene: a first-principles mechanistic evaluation

Abstract

Nitrogen-doped graphene has sparked a lot of interest due to its exceptional catalytic activity in a variety of chemical processes. We examine the catalytic ability of a series of nitrogen-containing graphene surfaces for CO oxidation using first-principles computations. The activation of the O₂ molecule in these systems is affected by the number and distribution of nitrogen impurities. According to the results, O₂ may be readily decomposed to O* species adsorbed on the nearest carbon atoms in the most active nitrogen-doped structures. The oxidation of a second CO is the rate-limiting step of the process due to the strong binding of the remaining O* moiety on the surface. Based on our findings, N-doped graphene can provide excellent metal-free catalytic performance for CO oxidation.