A Computational Study about Reduction of Carbon Dioxide by Hydrogen Molecule over Graphene Surface Doped with Ni and N Atoms

Today, climate change caused by the emission of greenhouse gasses is one of the most important environmental challenges facing humankind. In this work, using density functional theory calculations, the probable reaction mechanisms for the reduction of CO2 by H2 molecule were investigated over a Ni atom incorporated nitrogen-doped graphene. Our results indicated that the Ni atom can be efficiently adsorbed over the monovacancy site in the nitrogen-doped graphene. According to the obtained results, the catalytic activity of the mentioned surface is mainly originated from the strong hybridization between the σ orbital of the hydrogen molecule and 3d orbitals of nickel. The activation energies indicated that for the reduction of CO2, the formation of carboxylate is energetically more favorable than that of the formate intermediate.