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AbstractMixed‐matrix membranes (MMMs) were prepared by combinations of two different kinds of porous fillers [metal‐organic frameworks (MOFs) HKUST‐1 and ZIF‐8, and zeolite silicalite‐1] and polysulfone. In the search for filler synergy, the MMMs were applied to the separation of CO2/N2, CO2/CH4, O2/N2, and H2/CH4 mixtures and we found important selectivity improvements with the HKUST‐1‐silicalite‐1 system (CO2/CH4 and CO2/N2 separation factors of 22.4 and 38.0 with CO2 permeabilities of 8.9 and 8.4 Barrer, respectively).
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