n-Butane Transformation on Zn/H-BEA. The Effect of Different Zn Species (Zn2+ and ZnO) on the Reaction Performance | Sciact - CRIS-system of Boreskov Institute of Catalysis

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

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.

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

Submitted:	May 5, 2020
Accepted:	Aug 4, 2020
Published online:	Aug 15, 2020
Published print:	Nov 1, 2020

Web of science:	WOS:000590678100007
Scopus:	2-s2.0-85090047528
Elibrary:	45325629
Chemical Abstracts:	2020:1779489
OpenAlex:	W3049582762

DB	Citing
Scopus	14
Web of science	13
OpenAlex	14
Elibrary	12