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Methane Mobility in Ag/H-ZSM‑5 Zeolite in the Presence of Ethene: A View Based on PFG 1H MAS NMR Analysis of Methane Diffusivity Научная публикация

Журнал The Journal of Physical Chemistry C
ISSN: 1932-7447 , E-ISSN: 1932-7455
Вых. Данные Год: 2015, Том: 119, Номер: 32, Страницы: 18481-18486 Страниц : 6 DOI: 10.1021/acs.jpcc.5b05953
Ключевые слова Activation energy; Diffusion; Ethylene; Nuclear magnetic resonance spectroscopy; Positive ions; Silver compounds; Zeolites
Авторы Arzumanov S.S. 1,2 , Kolokolov D.I. 1,2 , Freude D. 3 , Stepanov A.G. 1,2
Организации
1 Boreskov Institute of Catalysis, Siberian Branch of the Russian Academy of Sciences, Prospekt Akademika Lavrentieva 5, Novosibirsk 630090, Russia
2 Faculty of Natural Sciences, Department of Physical Chemistry, Novosibirsk State University, Pirogova Street 2, Novosibirsk 630090, Russia
3 Fakultat fur Physik und Geowissenschaften, Universitat Leipzig, Linnestrasse 5, 04103 Leipzig, Germany

Информация о финансировании (2)

1 Российский фонд фундаментальных исследований 14-03-91333
2 German Research Foundation HA 1893/16

Реферат: With regard to the influence of methane on the reactivity of ethene on Ag/H-ZSM-5 zeolite, the diffusivities of methane in the presence of ethene coadsorbed on Ag/H-ZSM- 5 has been analyzed by PFG 1H MAS NMR spectroscopy. It is established that the diffusion of methane in the absence of ethene occurs more slowly (activation energy Ea = 29 kJmol−1) than the diffusion of methane in the presence ofcoadsorbed ethene (Ea = 6−8 kJ mol−1). The higher value of Ea for the methane diffusion in the absence of ethene wasrelated with some strong interaction of methane with Ag+cations located in the zeolite channel system. Acceleration of diffusion and a decrease of its activation energy in the presence of ethene were assigned to the shielding effect of ethene adsorbed on Ag+ cations to form π-complexes. An absence of direct interaction of methane with Ag+ cations was assumed to provide a significant decrease of activation energy and acceleration of methane diffusion. Two ensembles of methane molecules different by diffusivity have been assumed to exist in the zeolite in the presence of coadsorbed ethene. The presence of two ensembles of diffusing methane in the zeolite was rationalized in terms of the existence of two pathways of methane diffusion through the zeolite channel system. By one pathway, methane presumably diffuses over π-complexes of ethene with Ag+ cations and the zeolite acid OH groups. The other pathway may include the methane diffusion in the zeolite channels exclusively over the zeolite OH groups.
Библиографическая ссылка: Arzumanov S.S. , Kolokolov D.I. , Freude D. , Stepanov A.G.
Methane Mobility in Ag/H-ZSM‑5 Zeolite in the Presence of Ethene: A View Based on PFG 1H MAS NMR Analysis of Methane Diffusivity
The Journal of Physical Chemistry C. 2015. V.119. N32. P.18481-18486. DOI: 10.1021/acs.jpcc.5b05953 WOS Scopus РИНЦ CAPlusCA OpenAlex
Даты:
Поступила в редакцию: 22 июн. 2015 г.
Принята к публикации: 27 июл. 2015 г.
Опубликована online: 5 авг. 2015 г.
Опубликована в печати: 13 авг. 2015 г.
Идентификаторы БД:
Web of science: WOS:000359683800051
Scopus: 2-s2.0-84939146820
РИНЦ: 24006365
Chemical Abstracts: 2015:1241598
Chemical Abstracts (print): 163:257538
OpenAlex: W2514695505
Цитирование в БД:
БД Цитирований
Web of science 12
Scopus 12
РИНЦ 12
OpenAlex 11
Альметрики: