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In situ 1H and 13C MAS NMR Study of the Mechanism of H/D Exchange for Deuterated Propane Adsorbed on H-ZSM-5 Full article

Общее Language: Английский, Genre: Full article,
Status: Published, Source type: Original
Journal Journal of Catalysis
ISSN: 0021-9517 , E-ISSN: 1090-2694
Output data Year: 2005, Volume: 235, Number: 1, Pages: 221-228 Pages count : 8 DOI: 10.1016/j.jcat.2005.08.002
Tags 13C MAS NMR, 1H MAS NMR, H-ZSM-5 zeolite, H/D exchange, In situ spectroscopy, Kinetics, Mechanism, Propane
Authors Stepanov Alexander G. 1 , Arzumanov Sergei S. 1 , Luzgin Mikhail V. 1 , Ernst Horst 2 , Freude Dieter 2 , Parmon Valentin N. 1
Affiliations
1 Boreskov Institute of Catalysis SB RAS
2 Universität Leipzig

Funding (4)

1 German Research Foundation FR 902/15
2 Russian Foundation for Basic Research 04-03-32372
3 Russian Science Support Foundation
4 International Association for the Promotion of Co-operation with Scientists from the New Independent States of the Former Soviet Union 03-51-5286

Abstract: The kinetics of hydrogen exchange between the molecules of propane-d8, propane-1,1,1,3,3,3-d6, propane-2,2-d2, and Brönsted acid sites of the zeolite H-ZSM-5 have been monitored in situ by 1H MAS NMR spectroscopy in the temperature range of 230–280 °C. The intramolecular hydrogen transfer was estimated by in situ 13C MAS NMR spectroscopy of the kinetics of 13C-label scrambling in adsorbed propane-2-13C. The hydrogen exchange was found to occur directly between methyl or methylene groups of the alkane and the zeolite acid sites via a pentacoordinated carbonium ion. The exchange with the methyl groups is faster than that with the methylene group. This accounts for the earlier observed regioselectivity of the hydrogen exchange for propane on acidic zeolites (J. Am. Chem. Soc. 117 (1995) 1135). The intramolecular hydrogen transfer between methyl and methylene groups is one order of magnitude slower than the hydrogen exchange of the both groups with the zeolite acid sites.
Cite: Stepanov A.G. , Arzumanov S.S. , Luzgin M.V. , Ernst H. , Freude D. , Parmon V.N.
In situ 1H and 13C MAS NMR Study of the Mechanism of H/D Exchange for Deuterated Propane Adsorbed on H-ZSM-5
Journal of Catalysis. 2005. V.235. N1. P.221-228. DOI: 10.1016/j.jcat.2005.08.002 publication_identifier_short.wos_identifier_type publication_identifier_short.scopus_identifier_type publication_identifier_short.rinz_identifier_type
Dates:
Submitted: Apr 19, 2005
Accepted: Aug 7, 2005
Published online: Sep 7, 2005
Published print: Oct 1, 2005
Identifiers:
publication_identifier.wos_identifier_type WOS:000232147500022
publication_identifier.scopus_identifier_type 2-s2.0-24944497188
publication_identifier.rinz_identifier_type 13478403
publication_identifier.accession_number_identifier_type 2005:1009268
publication_identifier.chemical_accession_number_identifier_type 143:439878
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