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Oh, Jin Woo,Cho, Kie Yong,Kan, Ming-Yang,Yu, Hyun Jung,Kang, Dun-Yen,Lee, Jong Suk Elsevier 2020 Journal of membrane science Vol.596 No.-
<P><B>Abstract</B></P> <P>Membrane-based gas separation requires highly delicate engineering of molecular structures for the desired separation performance. Herein, a new efficient approach to fabricate high-flux mixed matrix membranes (MMMs) for C<SUB>3</SUB>H<SUB>6</SUB>/C<SUB>3</SUB>H<SUB>8</SUB> separation is reported by utilizing ZnCo-mixed hybrid zeolitic imidazolate framework-8 (ZIF-8-67) with unexpectedly large aperture size. Our structural characterizations in molecular level reveal that the ZIF-8-67 exhibits a larger aperture size compared to ZIF-8. Such a large aperture size of ZIF-8-67 is attributed to the large angle between two neighboring ligands and the long metal-ligand bonding distance, which is confirmed by refining the computed XRD pattern until it matches the experimental one (Rietveld refinement). More importantly, the inclusion of ZIF-8-67 in the 6FDA-DAM matrix enhances the C<SUB>3</SUB>H<SUB>6</SUB> permeability by up to 240% with the moderate C<SUB>3</SUB>H<SUB>6</SUB>/C<SUB>3</SUB>H<SUB>8</SUB> selectivity improvement (70%), as compared to those of the polymeric counterpart. Furthermore, the temperature-dependent transport characterization verifies that the ZIF-containing MMMs improve the C<SUB>3</SUB>H<SUB>6</SUB>/C<SUB>3</SUB>H<SUB>8</SUB> energetic selectivity at the sacrifice of entropic selectivity due to a unique molecular sieving behavior of the ZIFs, thereby enhancing the diffusivity selectivity. This study proposes a simple strategy to enable the fine-tuning of the aperture size of parent ZIFs towards the desired gas separation performance.</P> <P><B>Highlights</B></P> <P> <UL> <LI> The effect of mixed metals of ZIFs on structure and transport properties was studied. </LI> <LI> Bimetallic ZnCo metal-mixed ZIF-8 (ZIF-8-67) exhibited an unexpected aperture size. </LI> <LI> ZIF-8-67-containing MMMs significantly enhanced C<SUB>3</SUB>H<SUB>6</SUB> permeability. </LI> <LI> ZIF-containing MMMs improved C<SUB>3</SUB>H<SUB>6</SUB>/C<SUB>3</SUB>H<SUB>8</SUB> energetic selectivity due to breathable behavior. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>
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