Mechanism Studies of the Conversion of 13C-Labeled n-Butane on Zeolite H-ZSM-5 by Using 13C Magic Angle Spinning NMR Spectroscopy and GC–MS Analysis Научная публикация
Журнал |
Chemistry - A European Journal
ISSN: 0947-6539 , E-ISSN: 1521-3765 |
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Вых. Данные | Год: 2006, Том: 12, Номер: 2, Страницы: 457-465 Страниц : 9 DOI: 10.1002/chem.200500382 | ||||||
Ключевые слова | Butane, GC-MS analysis, NMR spectroscopy, Reaction mechanisms, Zeolites | ||||||
Авторы |
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Организации |
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Информация о финансировании (6)
1 | German Research Foundation | FR 902/15 |
2 | Российский фонд фундаментальных исследований | 04-03-32372 |
3 | North Atlantic Treaty Organization | PST.CLG.979335 |
4 | International Association for the Promotion of Co-operation with Scientists from the New Independent States of the Former Soviet Union | 03-51-5286 |
5 | Сибирское отделение Российской академии наук | |
6 | Региональный общественный Фонд содействия отечественной науке |
Реферат:
By using 13C MAS NMR spectroscopy (MAS=magic angle spinning), the conversion of selectively 13C-labeled n-butane on zeolite H-ZSM-5 at 430–470 K has been demonstrated to proceed through two pathways: 1) scrambling of the selective 13C-label in the n-butane molecule, and 2) oligomerization–cracking and conjunct polymerization. The latter processes (2) produce isobutane and propane simultaneously with alkyl-substituted cyclopentenyl cations and condensed aromatic compounds. In situ 13C MAS NMR and complementary ex situ GC–MS data provided evidence for a monomolecular mechanism of the 13C-label scrambling, whereas both isobutane and propane are formed through intermolecular pathways. According to 13C MAS NMR kinetic measurements, both pathways proceed with nearly the same activation energies (Ea=75 kJ mol−1 for the scrambling and 71 kJ mol−1 for isobutane and propane formation). This can be rationalized by considering the intermolecular hydride transfer between a primarily initiated carbenium ion and n-butane as being the rate-determining stage of the n-butane conversion on zeolite H-ZSM-5.
Библиографическая ссылка:
Luzgin M.V.
, Stepanov A.G.
, Arzumanov S.S.
, Rogov V.A.
, Parmon V.N.
, Wang W.
, Hunger M.
, Freude D.
Mechanism Studies of the Conversion of 13C-Labeled n-Butane on Zeolite H-ZSM-5 by Using 13C Magic Angle Spinning NMR Spectroscopy and GC–MS Analysis
Chemistry - A European Journal. 2006. V.12. N2. P.457-465. DOI: 10.1002/chem.200500382 WOS Scopus РИНЦ
Mechanism Studies of the Conversion of 13C-Labeled n-Butane on Zeolite H-ZSM-5 by Using 13C Magic Angle Spinning NMR Spectroscopy and GC–MS Analysis
Chemistry - A European Journal. 2006. V.12. N2. P.457-465. DOI: 10.1002/chem.200500382 WOS Scopus РИНЦ
Даты:
Поступила в редакцию: | 5 апр. 2005 г. |
Опубликована online: | 15 сент. 2005 г. |
Опубликована в печати: | 23 дек. 2005 г. |
Идентификаторы БД:
Web of science | WOS:000234453300013 |
Scopus | 2-s2.0-29544437228 |
РИНЦ | 13489769 |
Chemical Abstracts | 2006:57772 |
Chemical Abstracts (print) | 144:273875 |
PMID (PubMed) | 16163765 |
OpenAlex | W2171329660 |