▎ 摘　　要

By the density functional theory (DFT) calculations, the formation geometries, electronic structures and catalytic properties of metal Pt and nonmetal (NM) atom-co-modified graphene (Pt-3NM-graphene, NM = N, Si, P) as reactive substrates were investigated. First, the formation energy of the Pt-3N-graphene configuration was less than that of the Pt-3Si- and Pt-3P-graphene systems. The adsorbed O-2 on Pt-3NM-graphene was more stable than that of CO molecules and their corresponding electronic and magnetic properties were analyzed in detail. Compared with the isolated O-2 or CO molecule, the coadsorption of CO/O-2 (or 2CO) had larger adsorption energies on Pt-3NM-graphene, which might have facilitated the catalytic reactions for CO oxidation. Furthermore, the different reaction mechanisms of CO oxidation on Pt-3NM-graphene were systematically investigated. It was found that the Eley-Rideal (ER) mechanism (CO + O-2 -> CO3), as the initial state on Pt-3NM-graphene sheets, had larger energy barriers than those of the Langmuir-Hinshelwood (LH) and new termolecular Eley-Rideal (TER) mechanisms. For the Pt-3N- and Pt-3Si-graphene, the catalytic oxidation of CO reactions through LH and TER reactions had much small energy barriers (<0.3 eV), which indicated that the initial state was energetically more favorable. These results provide valuable guidance on selecting dopants in graphene to design carbon-based catalysts with low price and high activity.