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n-Butene Conversion on H-Ferrierite Studied by 13C MAS NMR Full article

Journal Journal of Catalysis
ISSN: 0021-9517 , E-ISSN: 1090-2694
Output data Year: 2002, Volume: 211, Number: 1, Pages: 165-172 Pages count : 8 DOI: 10.1016/S0021-9517(02)93726-7
Tags 13C MAS NMR spectroscopy, 13C-label scrambling, Conjunct polymerization, H-FER zeolite, Isomerization, n-butene, Reaction mechanism
Authors Stepanov Alexander G. 1 , Luzgin Mikhail V. 1 , Arzumanov Sergei S. 1 , Ernst Horst 2 , Freude Dieter 2
Affiliations
1 Boreskov Institute of Catalysis, Siberian Branch, Russian Academy of Sciences, Prospekt Akademika Lavrentieva 5, Novosibirsk 630090, Russia
2 Abteilung Grenzflachenphysik, Universität Leipzig, Linnëstraße 5, 04103 Leipzig, Germany

Funding (1)

1 German Research Foundation SBF 294

Abstract: 13C MAS NMR analysis of the hydrocarbon products formed from the selectively 13C-labeled n-but-1-ene on zeolite ferrierite (H-FER) in a closed batch reactor revealed the following successive steps of the olefin conversion with temperature increase from 300 to 823 K: a double-bond-shift reaction, scrambling of the selective 13C label in the formed n-but-2-ene, oligomerization (dimerization), conjunct polymerization, formation of condensed aromatics, and formation of the simple aromatics. Arguments in favor of either bimolecular or pseudo-monomolecular mechanisms are provided, excluding at the same time the monomolecular isomerization of n- to isobutene on a fresh sample. The arguments are based on selective label redistribution in the n-but-2-enes, the impossibility of the existence of isobutene inside the pores of the zeolite under static conditions and the observation of n-but-2-enes oligomerization (dimerization). Conjunct polymerization leads to the formation of alkyl-substituted cyclopentenyl cations (CPCs), which can serve as an intermediate for pseudo-monomolecular isomerization. Carbonaceous deposits (polycyclic aromatics), which deactivate the catalyst in the isomerization reaction, are formed from the CPCs. Polycyclic aromatics are transformed into simple aromatics with methane and ethane evolution at 823 K.
Cite: Stepanov A.G. , Luzgin M.V. , Arzumanov S.S. , Ernst H. , Freude D.
n-Butene Conversion on H-Ferrierite Studied by 13C MAS NMR
Journal of Catalysis. 2002. V.211. N1. P.165-172. DOI: 10.1016/S0021-9517(02)93726-7 WOS Scopus Scopus РИНЦ ANCAN OpenAlex OpenAlex
Dates:
Submitted: Mar 5, 2002
Accepted: Jun 19, 2002
Published print: Oct 1, 2002
Published online: Oct 4, 2002
Identifiers:
Web of science: WOS:000178377800017
Scopus: 2-s2.0-0036026475 | 2-s2.0-85008406212
Elibrary: 41800554
Chemical Abstracts: 2002:752057
Chemical Abstracts (print): 138:41638
OpenAlex: W4249284802 | W2052156266
Citing:
DB Citing
Web of science 50
Scopus 42 10
Elibrary 38
OpenAlex 9 45
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