Adsorption and Diffusion of Methane in Carbon Pores at Low Temperatures
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We report a theoretical study of the adsorption behavior of methane in carbon pores at subcritical temperatures, using a combination of molecular simulation and nonlocal density functional theory. The multilayer adsorption isotherm and monolayer isosteric heat of adsorption for methane on a single carbon surface at 77.5 K are obtained from Grand Canonical Monte Carlo (GCMC) simulations and compared with the experimental results. The GCMC method is then used to carry out the study of adsorption at temperatures between 60 and 135 K and pore widths from 19 to 76 A, and used to investigate freezing transitions. Molecular dynamics (MD) simulations are used to study diffusion and to investigate the fluid structure near the wall of the pores, particularly in the neighborhood of the freezing transitions. A general picture of the adsorption behavior for a wide range of pore sizes and temperatures is obtained using the theory and compared with GCMC results. The development of a kinetic theory to calculate transport coefficients is also discussed. 1993 Kodansha Ltd.