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Anomalous Relationship between Molecular Size and Diffusivity of Ethane and Ethylene inside Crystals of Zeolitic Imidazolate Framework-11
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    Anomalous Relationship between Molecular Size and Diffusivity of Ethane and Ethylene inside Crystals of Zeolitic Imidazolate Framework-11
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    • Amineh Baniani
      Amineh Baniani
      Department of Chemical Engineering, University of Florida, Gainesville, Florida 32611, United States
    • Christian Chmelik
      Christian Chmelik
      Faculty of Physics and Earth Sciences, Leipzig University, Linnéstraße 5, D-04103 Leipzig, Germany
    • Evan M. Forman
      Evan M. Forman
      Department of Chemical Engineering, University of Florida, Gainesville, Florida 32611, United States
    • Lei Fan
      Lei Fan
      Department of Chemical Engineering, University of Florida, Gainesville, Florida 32611, United States
      More by Lei Fan
    • Erkang Zhou
      Erkang Zhou
      School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
      More by Erkang Zhou
    • Fengyi Zhang
      Fengyi Zhang
      School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
      More by Fengyi Zhang
    • Richelle Lyndon
      Richelle Lyndon
      School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    • Ryan P. Lively
      Ryan P. Lively
      School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States
    • Sergey Vasenkov*
      Sergey Vasenkov
      Department of Chemical Engineering, University of Florida, Gainesville, Florida 32611, United States
      *E-mail: [email protected]
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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2019, 123, 27, 16813–16822
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    https://doi.org/10.1021/acs.jpcc.9b03933
    Published June 19, 2019
    Copyright © 2019 American Chemical Society

    Abstract

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    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.

    Copyright © 2019 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpcc.9b03933.

    • Ball-and-stick model of ZIF-11 (Figure S1); histogram (Figure S2); powder XRD pattern (Figure S3); single-component adsorption isotherms (Figure S4); 13C NMR spectra (Figure S5); 1H NMR spectra (Figure S6); 13C NMR relaxation curves (Figure S7); 1H NMR relaxation curves (Figure S8); 13C PFG NMR attenuation curves (Figure S9); uptake curves (Figure S10); mean size of ZIF-11 crystals (Table S1); T1 and T2 NMR relaxation times (Tables S2 and S3); PFG NMR diffusion data (Tables S4 and S5); and ratio of the self-diffusivities (Table S6) (PDF)

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    This article is cited by 15 publications.

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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2019, 123, 27, 16813–16822
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpcc.9b03933
    Published June 19, 2019
    Copyright © 2019 American Chemical Society

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