Molecular Dynamics of Carbon Dioxide, Methane and Their Mixtures in a Zeolite Possessing Two Independent Pore Networks as Revealed by Computer Simulations

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Abstract
The molecular motion of methane (CH4) and carbon dioxide (CO2) sorbed in the two independent pore networks, being termed hereafter as large cavity (LC) and sinusoidal channel (SC) regions of the siliceous MWW-framework-type zeolite ITQ-1, is studied by means of atomistic computer simulation. Equilibrium molecular dynamics predicts different loading dependences for the two gases, for both the self and the collective (Maxwell−Stefan) diffusion coefficients; in particular, the transport coefficients of CH4 go through a maximum as its loading in the zeolite increases, whereas CO2 dynamics exhibits the decreasing trend with loading usually observed in nanoporous materials. The different loading dependence of the self-diffusivity for the two sorbates is attributed to their different probability density distribution within the supercages in the LC system of the ITQ-1 unit cell. The composition and occupancy dependence of the self-diffusivity of each component in their binary mixtures can be explained in terms of the selectivity for CO2 sorption thermodynamics in the zeolite. The collective diffusivity loading dependence of the single and binary sorbate system is explainable on the basis of the strength of intermolecular interactions along the diffusion direction connecting the supercages by invoking the quasichemical mean field theory.

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