ИСТИНА

At the moment, the study of dry reforming of methane mechanism (DRM) and the search for active cata- lysts of this important process is a hot topic. Possible models of catalytic active sites for methane activation as the first stage of DRM were calculated and studied. The models were based on experimentally obtained and characterized via X-ray analysis copper sulfide cluster Cu12S6(PR2R’)8 (R = Et, Ph; R’ = Et, “Pr, Ph)1 (Fig. 1). Firstly, structures of Cu12S6(PH3)8, Cu12S6, Cu12O6(PH3)8, Cu12O6 were calculated. Since it is known3 that nickel exhibits good catalytic performance in the DRM process, these clusters were doped with a nickel atom, and the structures of all possible isomers of NiCu11S6(PH3)8, NiCu11S6, NiCu11O6(PH3)8, and NiCu11O6 were studied. Simulation of C-H bond dissociation in CH4 was carried out on the most energetically stable isomer from each group, energy barriers of this stage were calculated using DFT PBE approach. The smallest barrier in this process is observed for the NiCu11O6 cluster (99 kJ/mol), which gives grounds to consider this model of the active center promising for DRM.