期刊
DALTON TRANSACTIONS
卷 50, 期 30, 页码 10423-10435出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1dt01477c
关键词
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资金
- German Research Foundation (DFG) [SCHN 1539/1-1]
- Cooperative Research Program of Institute for Catalysis, Hokkaido University [20B1030]
- Alexander von Humboldt foundation
- JSPS KAKENHI [JP19H04570]
- Sandia National Laboratories Truman Fellowship Program - Laboratory Directed Research and Development (LDRD) Program
- U.S. Department of Energy's National Nuclear Security Administration [DE-NA0003525]
This study demonstrates the successful adsorptive removal of ethane from ethylene streams using a series of metal-organic frameworks, with Zn-2(TM-bdc)(2)(dabco) showing the best performance. High pressure coadsorption measurements reveal an increase in ethane capacity and selectivity with increased pressures, which is rarely studied in most scientific research on hydrocarbon separation on MOFs.
The trapping of paraffins is beneficial compared to selective olefin adsorption for adsorptive olefin purification from a process engineering point of view. Here we demonstrate the use of a series of Zn-2(X-bdc)(2)(dabco) (where X-bdc(2-) is bdc(2-) = 1,4-benzenedicarboxylate with substituting groups X, DM-bdc(2-) = 2,5-dimethyl-1,4-benzenedicarboxylate or TM-bdc(2-) = 2,3,5,6-tetramethyl-1,4-benzenedicarboxylate and dabco = diazabicyclo[2.2.2.]octane) metal-organic frameworks (MOFs) for the adsorptive removal of ethane from ethylene streams. The best performing material from this series is Zn-2(TM-bdc)(2)(dabco) (DMOF-TM), which shows a high ethane uptake of 5.31 mmol g(-1) at 110 kPa, with a good IAST selectivity of 1.88 towards ethane over ethylene. Through breakthrough measurements a high productivity of 13.1 L kg(-1) per breakthrough is revealed with good reproducibility over five consecutive cycles. Molecular simulations show that the methyl groups of DMOF-TM are forming a van der Waals trap with the methylene groups from dabco, snuggly fitting the ethane. Further, rarely used high pressure coadsorption measurements, in pressure regimes that most scientific studies on hydrocarbon separation on MOFs ignore, reveal an increase in ethane capacity and selectivity for binary mixtures with increased pressures. The coadsorption measurements reveal good selectivity of 1.96 at 1000 kPa, which is verified also through IAST calculations up to 3000 kPa. This study overall showcases the opportunities that pore engineering by alkyl group incorporation and pressure increase offer to improve hydrocarbon separation in reticular materials.
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