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n-Butane Transformation on Zn/H-BEA. The Effect of Different Zn Species (Zn2+ and ZnO) on the Reaction Performance Full article

Journal Journal of Catalysis
ISSN: 0021-9517 , E-ISSN: 1090-2694
Output data Year: 2020, Volume: 391, Pages: 69-79 Pages count : 11 DOI: 10.1016/j.jcat.2020.08.011
Tags Aromatization; Hydrogenolysis; Kinetics; Mechanism; n-butane; Solid-state NMR; Zeolite BEA; Zn2+ cations; ZnO clusters
Authors Gabrienko Anton A. 1,2 , Arzumanov Sergei S. 1,2 , Lashchinskaya Zoya N. 1,2 , Toktarev Alexander V. 1 , Freude Dieter 3 , Haase Jürgen 3 , Stepanov Alexander G. 1,2
Affiliations
1 Boreskov Institute of Catalysis, Siberian Branch of the Russian Academy of Sciences, Prospekt Akademika Lavrentieva 5, Novosibirsk 630090, Russia
2 Novosibirsk State University, Faculty of Natural Sciences, Department of Physical Chemistry, Pirogova Str. 2, Novosibirsk 630090, Russia
3 Universität Leipzig, Fakultät für Physik und Geowissenschaften, Linnéstr. 5, 04103 Leipzig, Germany

Funding (2)

1 Russian Science Foundation
German Research Foundation
19-43-04101
2 German Research Foundation HA 1893/22-1

Abstract: Using solid-state 1H and 13C MAS NMR spectroscopy, the performance of H-BEA zeolite, modified with either Zn2+ cations (Zn2+/H-BEA) or ZnO clusters (ZnO/H-BEA), has been investigated with respect to n-butane transformation by aromatization and hydrogenolysis pathways. 13C-labeled n-butane has been used to follow the main stages of n-butane transformation on both Zn2+/H-BEA and ZnO/H-BEA with 13C MAS NMR at 298–623 K. Similar surface species, including n-butylzinc, n-butene, allyl-like oligomers, are formed as the intermediates on both zeolites. The kinetics of n-butane transformation has been monitored with 1H MAS NMR in situ at 543–573 K. Kinetics modeling reveals that Zn2+/H-BEA is more active for n-butane transformation than ZnO/H-BEA. A remarkable difference in the rates and the pathways of hydrogenolysis for Zn2+/H-BEA and ZnO/H-BEA has also been established. Propane and methane are hydrogenolysis products on ZnO/H-BEA whereas ethane is produced by the reaction on Zn2+/H-BEA. 13C NMR data and the kinetics analysis provide an insight on the occurrence of joint methane and n-butane conversion on Zn-modified zeolites under non-oxidative conditions. © 2020 Elsevier Inc.
Cite: Gabrienko A.A. , Arzumanov S.S. , Lashchinskaya Z.N. , Toktarev A.V. , Freude D. , Haase J. , Stepanov A.G.
n-Butane Transformation on Zn/H-BEA. The Effect of Different Zn Species (Zn2+ and ZnO) on the Reaction Performance
Journal of Catalysis. 2020. V.391. P.69-79. DOI: 10.1016/j.jcat.2020.08.011 WOS Scopus РИНЦ AN OpenAlex
Dates:
Submitted: May 5, 2020
Accepted: Aug 4, 2020
Published online: Aug 15, 2020
Published print: Nov 1, 2020
Identifiers:
Web of science: WOS:000590678100007
Scopus: 2-s2.0-85090047528
Elibrary: 45325629
Chemical Abstracts: 2020:1779489
OpenAlex: W3049582762
Citing:
DB Citing
Scopus 15
Web of science 14
OpenAlex 15
Elibrary 13
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