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Molecular Insight into the Slow Dynamics of C4 Hydrocarbons in the Zeolitic–Imidazole Framework (ZIF-8) Full article

Journal ACS Applied Materials and Interfaces
ISSN: 1944-8244 , E-ISSN: 1944-8252
Output data Year: 2021, Volume: 13, Number: 28, Pages: 33685–33692 Pages count : 8 DOI: 10.1021/acsami.1c08529
Tags MOF; ZIF-8; diffusion; hydrocarbons; butane; 1-butene; 2H NMR; molecular dynamics
Authors Khudozhitkov Alexander E. 1,2 , Zhao Hengli 3,4 , Ghoufi Aziz 3 , Arzumanov Sergei S. 2 , Kolokolov Daniil I. 2 , Maurin Guillaume 4 , Stepanov Alexander G. 2
Affiliations
1 Novosibirsk State University, Pirogova Street 2, Novosibirsk 630090, Russia
2 Boreskov Institute of Catalysis, Siberian Branch of Russian Academy of Sciences, Prospekt Akademika Lavrentieva 5, Novosibirsk 630090, Russia
3 Univ. Rennes, CNRS, IPR (Institut de Physique de Rennes) - UMR 6251, F-35000 Rennes, France
4 ICGM, Univ. Montpellier, CNRS, ENSCM, 34095 Montpellier, France

Funding (4)

1 Russian Foundation for Basic Research 18-29-04009
2 Ministry of Science and Higher Education of the Russian Federation 0239-2021-0003
3 The French National Research Agency
4 Grand Équipement National de Calcul Intensif A0100907613

Abstract: The family of zeolitic–imidazole framework (ZIF) materials is currently considered for the challenging separation of C4 hydrocarbons. However, yet, the microscopic diffusion mechanism for these hydrocarbons in these narrow gate porous materials remains elusive by conventional methods due to its very slow nature. Experimental (solid-state 2H nuclear magnetic resonance-NMR) and computational (molecular dynamics-MD) approaches were applied together to derive slow diffusional dynamics of n-butane and 1-butene in ZIF-8. By means of the 2H NMR technique, we evidenced the presence of two adsorption sites for the guests localized inside the cages of ZIF-8 and in the vicinity of the gates. We characterized the molecular mobility at each site and revealed that the translational intercage diffusion is realized by a slow directional motion associated with the gate-crossing. MD simulations provide an in-depth analysis of the diffusion and fully support the proposed dynamics picture for both n-butane and 1-butene. These calculations enable the derivation of the diffusivity and barriers for the long-range diffusion of both hydrocarbons in ZIF-8 and unraveled the microscopic diffusion mechanism implying intracage and intercage motions. We show that this NMR approach combined with modeling is a valuable tool to probe the molecular mobility for slow diffusing species in ordered cagelike porous frameworks.
Cite: Khudozhitkov A.E. , Zhao H. , Ghoufi A. , Arzumanov S.S. , Kolokolov D.I. , Maurin G. , Stepanov A.G.
Molecular Insight into the Slow Dynamics of C4 Hydrocarbons in the Zeolitic–Imidazole Framework (ZIF-8)
ACS Applied Materials and Interfaces. 2021. V.13. N28. P.33685–33692. DOI: 10.1021/acsami.1c08529 WOS Scopus РИНЦ ANCAN PMID OpenAlex
Dates:
Submitted: May 8, 2021
Accepted: Jun 29, 2021
Published online: Jul 9, 2021
Published print: Jul 21, 2021
Identifiers:
Web of science: WOS:000677540900105
Scopus: 2-s2.0-85111225518
Elibrary: 46936934
Chemical Abstracts: 2021:1504655
Chemical Abstracts (print): 179:186888
PMID: 34241993
OpenAlex: W3181903042
Citing:
DB Citing
Scopus 11
Web of science 11
Elibrary 9
OpenAlex 12
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