Density functional theory and kinetic Monte Carlo simulation study the strong metal-support interaction of dry reforming of methane reaction over Ni based catalysts

摘要

Oxide supports modify electronic structures of supported metal nanoparticles,and then affect the catalytic activity associated with the so-called strong metal-support interaction(SMSI).We herein report the strong influence of SMSI employing Ni_(4)/α-MoC(111) and defective Ni_(4)/MgO(100) catalysts used for dry reforming of methane(DRM,CO_(2)+CH_4→2 CO+2 H_(2)) by using density functional theory(DFT) and kinetic Monte Carlo simulation(KMC).The results show that α-MoC(111) and MgO(100) surface have converse electron and structural effect for Ni_(4) cluster.The electrons transfer from a-MoC(111) surface to Ni atoms,but electrons transfer from Ni atoms to MgO(100) surface;an extensive tensile strain is greatly released in the Ni lattice by MgO,but the extensive tensile strain is introduced in the Ni lattice by α-MoC.As a result,although both catalysts show good stability,H_(2)/CO ratio on Ni_(4)/α-MoC(111) is obviously larger than that on Ni_(4)/MgO(100).The result shows that Ni/α-MoC is a good catalyst for DRM reaction comparing with Ni/MgO catalyst.