| Summary: | This study investigated the permeation behaviors of <i>n</i>-hexane and 2-methylpentane through two-types of silicalite-1 membranes that have different pore-connectivity. The permeation mechanisms of these hydrocarbons were able to be explained by the adsorption–diffusion model. In addition, the fluxes through silicalite-1 membranes could be expressed by the modified Fick’s first law. The hydrocarbon fluxes through S-1<sub>S</sub> with better pore-connectivity were ca. 3–20 times larger than those through S-1<sub>M</sub> with poor pore-connectivity. For these membranes with different pore-connectivity, the activation energy of diffusion of <i>n</i>-hexane was 17.5 kJ mol<sup>−1</sup> for the membrane with better pore-connectivity and 18.0 kJ mol<sup>−1</sup> for the membrane with poorer pore-connectivity, whereas for 2-methylpentane it was 17.9 and 33.0 kJ mol<sup>−1</sup>, respectively. We concluded that the pore-connectivity in silicalite-1 membrane significantly influences the molecular diffusivities.
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