Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 18, Pages 10103-10111Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202015635
Keywords
gas separations; hybrid metal– organic frameworks; hybrid zeolitic– imidazolate frameworks; linker doping
Categories
Funding
- National Science Foundation [DBI-0116835, CMMI-1561897]
- European Union [894585]
- NPRP grant from Qatar National Research Fund (Qatar Foundation) [12S-0209-190064]
- VP for Research Office
- Texas A&M Engineering Experimental Station
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The delayed linker addition (DLA) synthesis strategy allows for efficient incorporation of Im linkers into ZIF-8 framework, improving gas separation performance. The Im/ZIF-8 synthesized via DLA demonstrates outstanding performance in gas separation.
We present a novel synthesis strategy termed delayed linker addition (DLA) to synthesize hybrid zeolitic-imidazolate frameworks containing unsubstituted imidazolate linkers (Im) with SOD topology (hereafter termed Im/ZIF-8). Im linker incorporation can create larger voids and apertures, which are important properties for gas storage and separation. To date, there have been only a handful of reports of Im linkers incorporated into ZIF-8 frameworks, typically requiring arduous and complicated post synthesis approaches. DLA, as reported here, is a simple one-step synthesis strategy allowing high incorporation of Im linker into the ZIF-8 framework while still retaining its SOD topology. We fabricated mixed-matrix membranes (MMMs) with 6FDA-DAM polymer and Im/ZIF-8 obtained via DLA as a filler. The Im/ZIF-8-containing MMMs showed excellent performance for both propylene/propane and n-butane/i-butane separation, displaying permeability and ideal selectivity well above the polymer upper bound. Moreover, highly detailed molecular simulations shed light to the aperture size and flexibility response of Im/ZIF-8 and its improved diffusivity as compared to ZIF-8.
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