Mechanism of NO reduction by CO over single atomic nickel catalyst: DFT and microkinetic study

This dataset was constructed based on Gaussian 09 quantum chemistry calculation software package, and mainly contains the mechanism research data of Ni single-atom catalyst catalytic reduction of NO. After the catalyst surface model is constructed with Gaussian 09, density functional theory (DFT) is used to optimize the geometric structure and search the transition state. In the calculation process, the B3LYP/6-31G (d) group is used to optimize the non-metallic atoms N, C, H and O, and the B3LYP/Lanl2DZ group is used to optimize the transition metal Ni atoms. B3lyp-d3 dispersion correction was adopted to solve the dispersion effect of B3LYP method. TS (Berny) method is used to calculate the transition state of the reaction process. BFGS algorithm is used to search and optimize the transition state of the reaction path to ensure the calculation accuracy and efficiency. The information of the wave function is computed using the Multiwin program and part of the results are visualized using VMD. In addition, CATMAP software was used to conduct microkinetic simulation, combined with the energy data obtained by DFT simulation, to explore the influence of reaction temperature and reaction pressure on the catalytic reduction activity of Ni single atom catalyst under each reaction path. The data set files include PDF files and Origin 2021 project files.1) PDF file as follows:Figure 1 (a) Optimal structure of graphene quantum dots, (b) Optimal structure of Ni/G catalyst and (c) electron localization function (ELF) in DFT simulationFigure 2 Geometrically optimized structure diagram of reactants, intermediates, transition states and products in P1 pathFigure 4 Geometrically optimized structure diagram of reactants, intermediates, transition states and products in P2 pathFigure 6 Differential electron density maps of different NO adsorption structures (a) P2-E-IM2, (b) P2-L-IM1Figure 7 Geometrically optimized structures of reactants, intermediates, transition states and products of O* reduction reactionFigure 10 Temperature/pressure graphs of CO2 and N2 production rates for (a) - (b)P1 paths, (c) - (d) P2-E paths and (e) - (f) P2-L pathsFigure 12 O* coverage of Ni atomic catalyst surface under P2-L pathThe Origin 2021 project documents are as follows:Figure 3 Gibbs free energy of Ni/G reduction of NO reaction based on P1 pathFigure 5 Gibbs free energy of N2O formation reaction based on P2 pathwayFigure 8 Gibbs free energy spectrum of O* reduction reactionFigure 9 (a) The order of transition states P2-L-TS1 along the Mayer bond of IRC in the P2 pathFigure 9 (b) The order of the transition states P1-TS2 along the IRC Mayer bond in the P2 pathFigure 9 (c) The order of transition states P2-TS1 along the Mayer bond of IRC in the P2 pathFigure 11 Reaction rate constants at different reaction temperatures