Anomalous Relationship between Molecular Size and Diffusivity of Ethane and Ethylene inside Crystals of Zeolitic Imidazolate Framework-11Click to copy article linkArticle link copied!
- Amineh BanianiAmineh BanianiDepartment of Chemical Engineering, University of Florida, Gainesville, Florida 32611, United StatesMore by Amineh Baniani
- Christian ChmelikChristian ChmelikFaculty of Physics and Earth Sciences, Leipzig University, Linnéstraße 5, D-04103 Leipzig, GermanyMore by Christian Chmelik
- Evan M. FormanEvan M. FormanDepartment of Chemical Engineering, University of Florida, Gainesville, Florida 32611, United StatesMore by Evan M. Forman
- Lei FanLei FanDepartment of Chemical Engineering, University of Florida, Gainesville, Florida 32611, United StatesMore by Lei Fan
- Erkang ZhouErkang ZhouSchool of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United StatesMore by Erkang Zhou
- Fengyi ZhangFengyi ZhangSchool of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United StatesMore by Fengyi Zhang
- Richelle LyndonRichelle LyndonSchool of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United StatesMore by Richelle Lyndon
- Ryan P. LivelyRyan P. LivelySchool of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United StatesMore by Ryan P. Lively
- Sergey Vasenkov*Sergey Vasenkov*E-mail: [email protected]Department of Chemical Engineering, University of Florida, Gainesville, Florida 32611, United StatesMore by Sergey Vasenkov
Abstract

Multinuclear pulsed field gradient (PFG) NMR was used to study the self-diffusion of ethane and ethylene inside loosely packed beds of zeolitic imidazolate framework-11 (ZIF-11) crystals. Diffusion measurements were performed at different temperatures under conditions where the length scales of displacements were smaller than or comparable with the mean size of the ZIF-11 crystals. For the crystal beds loaded with a single sorbate, these studies showed a larger intracrystalline diffusivity for ethane than that for ethylene under the same or comparable experimental conditions, an unexpected result due to the larger size of ethane compared to that of ethylene. PFG NMR diffusion studies of ZIF-11 beds loaded with ethane/ethylene mixtures revealed that substituting a fraction of ethane molecules by ethylene molecules decreases the intracrystalline diffusivity of ethane. These results in combination with an observation of a higher-for-ethylene-than-for-ethane activation energy of intracrystalline self-diffusion in single-sorbate systems suggest a hindering effect of ethylene molecules on the intra-ZIF diffusion. To further confirm and investigate the anomalous relationship between ethane and ethylene intracrystalline diffusivities in ZIF-11, uptake curves for ethane and ethylene were measured in single crystals using IR microscopy and in a thin crystal bed using a volumetric technique. The diffusion data obtained from these complementary uptake studies under the same or comparable conditions were found to be consistent with the PFG NMR measurements. The observed anomalous relationship between ethane and ethylene diffusivities in ZIF-11 is discussed in the context of the flexibility of the ZIF-11 framework.
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