Molecular Insight into the Slow Dynamics of C4 Hydrocarbons in the Zeolitic–Imidazole Framework (ZIF-8) | Sciact - CRIS-система Института катализа

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

Журнал

ACS Applied Materials and Interfaces
ISSN: 1944-8244 , E-ISSN: 1944-8252

Вых. Данные

Год: 2021, Том: 13, Номер: 28, Страницы: 33685–33692 Страниц : 8 DOI: 10.1021/acsami.1c08529

Ключевые слова

MOF; ZIF-8; diffusion; hydrocarbons; butane; 1-butene; 2H NMR; molecular dynamics

Авторы

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

Организации

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

Информация о финансировании (4)

1	Российский фонд фундаментальных исследований	18-29-04009
2	Министерство науки и высшего образования Российской Федерации (с 15 мая 2018)	0239-2021-0003
3	The French National Research Agency
4	Grand Équipement National de Calcul Intensif	A0100907613

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.

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 CAPlusCA PMID OpenAlex

Поступила в редакцию:	8 мая 2021 г.
Принята к публикации:	29 июн. 2021 г.
Опубликована online:	9 июл. 2021 г.
Опубликована в печати:	21 июл. 2021 г.

Web of science:	WOS:000677540900105
Scopus:	2-s2.0-85111225518
РИНЦ:	46936934
Chemical Abstracts:	2021:1504655
Chemical Abstracts (print):	179:186888
PMID (PubMed):	34241993
OpenAlex:	W3181903042

БД	Цитирований
Scopus	11
Web of science	11
РИНЦ	7
OpenAlex	12