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The demand for cost-efficient separations requires membranes with high gas flux and high selectivity which opens the path for further improvements. Mixed matrix membranes (MMMs) made from 33.3 wt % ZIF-8 in 6FDA-durene were tested at 35 °C and 3.5 atm. At 33.3 wt % loading of ZIF-8, H2, N2, O2, and CH4 gas permeabilities increased approximately 400%. Cross-linking the surface of this MMM, by reacting with ethylenediamine vapor, yielded a 10-fold increase in H2/CO2, H2/N2, and H2/CH4 selectivities with respect to 6FDA-durene, preserving 55% of the H2 permeability of 6FDA-durene. The permselective properties of the cross-linked skin of the MMM fall above the most recent permeability–selectivity trade-off lines (2008 Robeson upper bounds) for H2/CO2, H2/N2, and H2/CH4 separations. To the best of our knowledge, this is the first example of a cross-linked ZIF/polymer MMM for gas separation.

A carbon aerogel was prepared by carbonizing a resorcinol−formaldehyde polymer gel at 800 °C. Nitrogen adsorption shows the obtained carbon aerogel has both micropores (0.54 nm) and mesopores (2.14 nm). Matrimid mixed-matrix membranes containing the carbon aerogels were successfully prepared and evaluated for the permeation of H2, N2, O2, CH4, CO2, and gas mixtures. The ideal selectivity of H2/N2, CO2/CH4, and O2/N2 gas pairs increased from 79.6, 34.5, and 6.6 for pure Matrimid to 111, 47.8, and 9.1 at 20% loading, respectively. These results suggest that the polymer chains can penetrate the carbon mesopores to achieve good contact between the carbon aerogel and Matrimid, while the micropores may provide size and shape selectivity.