Diffusion of a mixture of methane and xenon in silicalite: A molecular dynamics study and pulsed field gradient nuclear magnetic resonance experiments

The diffusion of a mixture of methane and xenon in the zeolite silicalite is studied by use of molecular dynamics (MD) simulations and pulsed field gradient (PFG) nuclear magnetic resonance (NMR). For a fixed total number of guest molecules, the ratio of xenon to methane is varied in order to examine the special properties of diffusion in a mixture. High xenon concentrations were found to slow the methane diffusivity in the mixture, while the diffusion of xenon is nearly unaffected by high methane concentrations. The reason for the dominance of xenon is the larger local heat of adsorption of xenon and the larger mass of xenon compared to methane in combination with channel size and topology in silicalite. Simulated and experimental data are in very good agreement with each other. Diffusion anisotropy as resulting from the MD simulations is discussed in terms of the correlation rule for diffusion in the interconnected pore system of ZSM-5 (Karger, J. J. Phys. Chem. 1991, 98, 5558).