Methane Activation on In-Modified ZSM-5 Zeolite. H/D Hydrogen Exchange of the Alkane with Bronsted Acid Sites Научная публикация
Журнал |
The Journal of Physical Chemistry C
ISSN: 1932-7447 , E-ISSN: 1932-7455 |
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Вых. Данные | Год: 2014, Том: 118, Номер: 26, Страницы: 14427-14432 Страниц : 6 DOI: 10.1021/jp5037316 | ||||||
Ключевые слова | Activation analysis; Activation energy; Hydrogen; Magic angle spinning; Nuclear magnetic resonance spectroscopy; Zeolites | ||||||
Авторы |
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Организации |
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Информация о финансировании (1)
1 | Российский фонд фундаментальных исследований | 14-03-00040 |
Реферат:
In relation to clarifying the pathway of methane activation on In-modified zeolites, a comparative analysis of kinetics of hydrogen (H/D) exchange between methane-d4 and Brønsted acid sites (BAS) for both the pure acid form zeolite (H-ZSM-5) and In-modified zeolites (In+/H-ZSM-5 and InO+/H-ZSM-5) has been performed. Monitoring of the kinetics has been carried out with 1H magic-angle spinning NMR spectroscopy in situ within the temperature range of 453–568 K. While the rate of exchange on In+/H-ZSM-5 is 1 order of magnitude larger than that on H-ZSM-5, the exchange occurs on InO+/H-ZSM-5 by 2 orders of magnitude faster than that on H-ZSM-5. Significant increase of the rate and decrease of the activation energy (Ea = 74 ± 6 kJ mol–1) and the temperature threshold (453 K) for the reaction of the exchange on InO+/H-ZSM-5 compared to the rate, activation energy, and temperature threshold (543 K) for the reaction on In+/H-ZSM-5 (Ea = 127 ± 27 kJ mol–1) and H-ZSM-5 (Ea = 118 ± 9 kJ mol–1) have been rationalized in terms of involvement of both InO+ and BAS in activation of methane molecules on the zeolite. Some transient intermediate complex of methane with the zeolite InO+ species and BAS has been assumed to be formed within the zeolite pore. This complex is involved either in the reaction of H/D exchange with BAS of the zeolite or evolves further to offer indium methyl species.
Библиографическая ссылка:
Arzumanov S.S.
, Moroz I.B.
, Freude D.
, Haase J.
, Stepanov A.G.
Methane Activation on In-Modified ZSM-5 Zeolite. H/D Hydrogen Exchange of the Alkane with Bronsted Acid Sites
The Journal of Physical Chemistry C. 2014. V.118. N26. P.14427-14432. DOI: 10.1021/jp5037316 WOS Scopus РИНЦ CAPlusCA OpenAlex
Methane Activation on In-Modified ZSM-5 Zeolite. H/D Hydrogen Exchange of the Alkane with Bronsted Acid Sites
The Journal of Physical Chemistry C. 2014. V.118. N26. P.14427-14432. DOI: 10.1021/jp5037316 WOS Scopus РИНЦ CAPlusCA OpenAlex
Даты:
Поступила в редакцию: | 16 апр. 2014 г. |
Принята к публикации: | 5 июн. 2014 г. |
Опубликована online: | 19 июн. 2014 г. |
Опубликована в печати: | 3 июл. 2014 г. |
Идентификаторы БД:
Web of science: | WOS:000338693600039 |
Scopus: | 2-s2.0-84903761055 |
РИНЦ: | 24064226 |
Chemical Abstracts: | 2014:938835 |
Chemical Abstracts (print): | 161:87993 |
OpenAlex: | W2314378242 |