Study on syngas methanation mechanism over Ni4/MCM-41 catalyst based on density functional theory

The density functional theory method is employed to systematically explore the mechanism of syngas methanation on the Ni4/MCM-41 catalyst surface. The calculation results show that the optimal pathway of CH4 formation is CO + H → CHO + H → CH2O + H → CH3O → CH3 + H → CH4 with the rate-determining step of CH3O direct dissociation. Because the activation energy for the direct dissociation of CH3O species is much lower than that for the CH3OH formation (198.6 vs 264.8 kJ mol−1), there is almost no by-product CH3OH that appeared in the products of the syngas methanation over the Ni4/MCM-41 catalyst. Compared with other conventional nickel-based methanation catalysts, Ni4/MCM-41 catalyst is an excellent methanation catalyst with high selectivity of CH4.