摘要

We investigate gas adsorption and transport in a disordered microporous silica membrane having mean pore diameter 1.5 nm, coated on a porous tubular asymmetric support. The adsorption isotherms are found to be Langmuirian, with equilibrium constants that are accurately predicted for nonpolar gases, considering Lennard-lones (Lj) interactions with a single layer of oxygen atoms on the pore surface. For the polar gas, CO2, the hydroxyls groups on the pore walls strongly increase the affinity with the pore walls, and a superposition of the Ll potential and an empirically represented electrostatic interaction is found to be adequate in correlating the Langmuirian equilibrium constant. The gas transport in the microporous silica layer is investigated using effective medium theory, with single pore transport represented by combination of pore mouth and internal pore diffusion resistances. Good agreement is observed for all the gases using different coordination numbers, indicating that the essential features of the transport in the silica micropores are captured in the approach It is found that the overall transport resistance is dominated by the pore mouth barrier; however, the internal diffusion resistance in the relatively smaller pores is significant, especially for weakly adsorbed gases at higher temperature. In addition, the dependence of the pore mouth barrier coefficient on temperature and diffusing species are in good agreement with predictions of transition-state theory, with larger more strongly adsorbed molecules having higher activation energy. The proposed methodology is validated against experiment by comparison of the predicted flux for different gases in the supported membrane at various feed pressures in the low pressure range of 200-400 kPa, using the parameters obtained at 200 kPa.

  • 出版日期2014-6-15