期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 28, 页码 15541-15547出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202103936
关键词
crystallography; ethylene; host-guest interactions; metal-organic framework; propylene
资金
- EPSRC [EP/I011870]
- Royal Society
- University of Manchester
- European Research Council (ERC) under the European Union [742401]
- DOE Office of Science User Facility [DE-AC0205CH11231]
- Royal Society Newton International Fellowship
- China Scholarship Council (CSC)
- Laboratory Directed Research and Development programme
- Compute and Data Environment for Science (CADES) at ORNL
- Henry Royce Institute for Advanced Materials - EPSRC [EP/R00661X/1, EP/S019367/1, EP/P025021/1, EP/P025498/1]
This study reports a method of separating propylene and ethylene from propane, ethane, and acetylene using a microporous material, and reveals the mechanism of synergistic host-guest interactions.
Industrial purification of propylene and ethylene requires cryogenic distillation and selective hydrogenation over palladium catalysts to remove propane, ethane and/or trace amounts of acetylene. Here, we report the excellent separation of equimolar mixtures of propylene/propane and ethylene/ethane, and of a 1/100 mixture of acetylene/ethylene by a highly robust microporous material, MFM-520, under dynamic conditions. In situ synchrotron single crystal X-ray diffraction, inelastic neutron scattering and analysis of adsorption thermodynamic parameters reveal that a series of synergistic host-guest interactions involving hydrogen bonding and pi...pi stacking interactions underpin the cooperative binding of alkenes within the pore. Notably, the optimal pore geometry of the material enables selective accommodation of acetylene. The practical potential of this porous material has been demonstrated by fabricating mixed-matrix membranes comprising MFM-520, Matrimid and PIM-1, and these exhibit not only a high permeability for propylene (approximate to 1984 Barrer), but also a separation factor of 7.8 for an equimolar mixture of propylene/propane at 298 K.
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