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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

Общая информация Язык: Английский, Жанр: Статья (Full article),
Статус опубликования: Опубликована, Оригинальность: Оригинальная
Журнал Chemistry - A European Journal
ISSN: 0947-6539 , E-ISSN: 1521-3765
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 Luzgin Mikhail V. 1 , Stepanov Alexander G. 1 , Arzumanov Sergei S. 1 , Rogov Vladimir A. 1 , Parmon Valentin N. 1 , Wang Wei 2 , Hunger Michael 2 , Freude Dieter 3
Организации
1 Boreskov Institute of Catalysis, Siberian Branch of the Russian Academy of Sciences, Prosp. Akademika Lavrentieva 5, Novosibirsk 630090 (Russia)
2 Institute of Chemical Technology, University of Stuttgart, 70550 Stuttgart (Germany)
3 Abteilung Grenzflachenphysik, Universitat Leipzig, Linnestrasse 5, 04103 Leipzig (Germany)

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
Даты:
Поступила в редакцию: 5 апр. 2005 г.
Опубликована online: 15 сент. 2005 г.
Опубликована в печати: 23 дек. 2005 г.
Идентификаторы:
Web of science WOS:000234453300013
Scopus 2-s2.0-29544437228
РИНЦ 13489769
Chemical Abstracts 2006:57772
Chemical Abstracts (print) 144:273875
Альметрики: