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Mixed matrix membranes (MMMs) prepared with 6FDA‐DAM polymer using ordered mesoporous silica MCM‐41 spheres (MSSs), Grignard surface functionalized MSSs (Mg‐MSSs) and hollow zeolite spheres are studied to evaluate the effects of surface modification on performance. Performance near or above the so‐called permeability‐selectivity trade‐off curve was achieved for the H2/CH4, CO2/N2, CO2/CH4, and O2/N2 systems. Two loadings (8 wt % and 16 wt %) of MSSs were tested using both constant volume and Wicke–Kallenbach sweep gas permeation systems. Besides single gas H2, CO2, O2, N2, and CH4 tests, mixed gas (50/50 vol %) selectivities were obtained for H2/CH4, CO2/N2, CO2/CH4, and O2/N2 and found to show enhancements vs. single gases for CO2 including cases. Mg‐MSS/6FDA‐DAM was the best performing MMM with H2/CH4, CO2/N2, CO2/CH4, and O2/N2 separation selectivities of 21.8 (794 Barrer of H2), 24.4 (1214 Barrer of CO2), 31.5 (1245 Barrer of CO2), and 4.3 (178 Barrer of O2), respectively. © 2015 American Institute of Chemical Engineers AIChE J, 61: 4481–4490, 2015  相似文献   
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