▎ 摘　　要

CO2 adsorption on bare 3d transition-metal nanoclusters and 3d transition-metal nanoclusters supported on pyridinic N-3-doped graphene (PNG) was investigated by employing the density functional theory. First, the interaction of Co-13 and Cu-13 with PNG was analyzed by spin densities, interaction energies, charge transfers, and HUMO-LUMO gaps. According to the interaction energies, the Co-13 nanocluster was adsorbed more efficiently than Cu-13 on the PNG. The charge transfer indicated that the Co-13 nanocluster donated more charges to the PNG nanoflake than the Cu-13 nanocluster. The HUMO-LUMO gap calculations showed that the PNG improved the chemical reactivity of both Co-13 and Cu-13 nanoclusters. When the CO2 was adsorbed on the bare 3d transition-metal nanoclusters and 3d transition-metal nanoclusters supported on the PNG, it experienced a bond elongation and angle bending in both systems. In addition, the charge transfer from the nanoclusters to the CO2 molecule was observed. This study proved that Co-13/PNG and Cu-13/PNG composites are adequate candidates for CO2 adsorption and activation.