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Molecular Diffusion in a Flexible Mesoporous Metal–Organic Framework over the Course of Structural Contraction
[Image: see text] In situ (1)H pulsed field gradient (PFG) NMR was used to investigate the molecular diffusion of n-butane in the pores of the flexible metal–organic framework DUT-49(Cu) at 298 K at different pore loadings, including pressure ranges below and above the negative gas adsorption (NGA)...
Autores principales: | , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical
Society
2020
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9115798/ https://www.ncbi.nlm.nih.gov/pubmed/33136403 http://dx.doi.org/10.1021/acs.jpclett.0c02745 |
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author | Walenszus, Francesco Bon, Volodymyr Evans, Jack D. Kaskel, Stefan Dvoyashkin, Muslim |
author_facet | Walenszus, Francesco Bon, Volodymyr Evans, Jack D. Kaskel, Stefan Dvoyashkin, Muslim |
author_sort | Walenszus, Francesco |
collection | PubMed |
description | [Image: see text] In situ (1)H pulsed field gradient (PFG) NMR was used to investigate the molecular diffusion of n-butane in the pores of the flexible metal–organic framework DUT-49(Cu) at 298 K at different pore loadings, including pressure ranges below and above the negative gas adsorption (NGA) transition caused by structural contraction of the material. Supported by molecular dynamics simulations, the investigation provided crucial insight into confined diffusion within a highly flexible pore environment. The self-diffusion coefficients were derived from the experiment and compared with simulations, capturing the diffusion during n-butane adsorption and desorption. This complementary approach has yielded experimental characterization of molecular diffusion mechanisms during the unique process of NGA. This includes the observation of a 4-fold decrease of diffusivity within a less than 2 kPa gas pressure variation, corresponding to the NGA transition point. |
format | Online Article Text |
id | pubmed-9115798 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2020 |
publisher | American Chemical
Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-91157982022-05-19 Molecular Diffusion in a Flexible Mesoporous Metal–Organic Framework over the Course of Structural Contraction Walenszus, Francesco Bon, Volodymyr Evans, Jack D. Kaskel, Stefan Dvoyashkin, Muslim J Phys Chem Lett [Image: see text] In situ (1)H pulsed field gradient (PFG) NMR was used to investigate the molecular diffusion of n-butane in the pores of the flexible metal–organic framework DUT-49(Cu) at 298 K at different pore loadings, including pressure ranges below and above the negative gas adsorption (NGA) transition caused by structural contraction of the material. Supported by molecular dynamics simulations, the investigation provided crucial insight into confined diffusion within a highly flexible pore environment. The self-diffusion coefficients were derived from the experiment and compared with simulations, capturing the diffusion during n-butane adsorption and desorption. This complementary approach has yielded experimental characterization of molecular diffusion mechanisms during the unique process of NGA. This includes the observation of a 4-fold decrease of diffusivity within a less than 2 kPa gas pressure variation, corresponding to the NGA transition point. American Chemical Society 2020-11-02 2020-11-19 /pmc/articles/PMC9115798/ /pubmed/33136403 http://dx.doi.org/10.1021/acs.jpclett.0c02745 Text en © 2020 American Chemical Society https://creativecommons.org/licenses/by-nc-nd/4.0/Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works (https://creativecommons.org/licenses/by-nc-nd/4.0/). |
spellingShingle | Walenszus, Francesco Bon, Volodymyr Evans, Jack D. Kaskel, Stefan Dvoyashkin, Muslim Molecular Diffusion in a Flexible Mesoporous Metal–Organic Framework over the Course of Structural Contraction |
title | Molecular Diffusion in a Flexible Mesoporous Metal–Organic
Framework over the Course of Structural Contraction |
title_full | Molecular Diffusion in a Flexible Mesoporous Metal–Organic
Framework over the Course of Structural Contraction |
title_fullStr | Molecular Diffusion in a Flexible Mesoporous Metal–Organic
Framework over the Course of Structural Contraction |
title_full_unstemmed | Molecular Diffusion in a Flexible Mesoporous Metal–Organic
Framework over the Course of Structural Contraction |
title_short | Molecular Diffusion in a Flexible Mesoporous Metal–Organic
Framework over the Course of Structural Contraction |
title_sort | molecular diffusion in a flexible mesoporous metal–organic
framework over the course of structural contraction |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9115798/ https://www.ncbi.nlm.nih.gov/pubmed/33136403 http://dx.doi.org/10.1021/acs.jpclett.0c02745 |
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