Abstract
The pulsed field gradient nuclear magnetic resonance method has been used to study self-diffusion of cyclohexane in a commercial MCM-41 material at different external gas pressures from zero to saturated vapor pressure. It is found that the effective diffusivities exhibit three different regions with increasing pressure: decrease at low pressures, a sudden drop at intermediate pressures, and increase at higher pressures. In addition, in the region of irreversible adsorption (hysteresis loop) the diffusivities are also found to differ on the adsorption and the desorption branches. A simple analytical model taking account of different molecular ensembles with different transport properties due to the complex architecture of the porous structure is developed which provides a quantitative prediction of the experimental data. The analysis reveals that the effective diffusivity is predominantly controlled by the adsorption properties of the individual mesoporous MCM-41 crystallites which, in combination with high transport rates, provide a simple instrument for fine tuning of the transport properties by a subtle variation of the external conditions.
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