Propane Activation on Zn-Modified Zeolite. The Effect of the Nature of Zn-Species on the Mechanism of H/D Hydrogen Exchange of the Alkane with Brønsted Acid Sites | Sciact - CRIS-system of Boreskov Institute of Catalysis

Propane Activation on Zn-Modified Zeolite. The Effect of the Nature of Zn-Species on the Mechanism of H/D Hydrogen Exchange of the Alkane with Brønsted Acid Sites Full article

Journal

Journal of Catalysis
ISSN: 0021-9517 , E-ISSN: 1090-2694

Output data

Year: 2019, Volume: 378, Pages: 341-352 Pages count : 12 DOI: 10.1016/j.jcat.2019.09.006

Tags

1H MAS NMR in situ; Activation; Brønsted acid sites; H/D hydrogen exchange; Mechanism; Nature of Zn species; Propane; Zn-modified H-BEA zeolite; Zn2+ cations; ZnO small clusters

Authors

Arzumanov Sergei S. ^1,2 , Gabrienko Anton A. ^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, Russian Federation
2	Novosibirsk State University, Faculty of Natural Sciences, Department of Physical Chemistry, Pirogova Str. 2, Novosibirsk, 630090, Russian Federation
3	Universität Leipzig, Fakultät für Physik und Geowissenschaften, Linnéstr. 5, Leipzig, 04103, Germany

Funding (2)

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

Zn-modified zeolites exhibit high activity for the aromatization of C2+ alkanes. To understand the effect of Zn-species of different nature on propane molecules activation and transformation, the H/D hydrogen exchange of zeolite Brønsted acid sites (BAS) with deuterated propane-d8 has been investigated. Two samples of the Zn-modified zeolite containing exclusively either isolated Zn2+ cations (Zn2+/H-BEA) or small (ZnO)n clusters (ZnO/H-BEA) have been studied. Zn-species of either type work jointly with BAS and may provide the synergy effect for propane C[sbnd]H bond activation resulting in dramatic acceleration of the H/D exchange between propane and BAS. The accelerating effect of isolated Zn2+ cations is more pronounced compared to zinc oxide clusters. Moreover, the H/D exchange occurs regioselectively into the methyl groups of propane on Zn2+/H-BEA zeolite. For ZnO/H-BEA, the methylene group becomes also involved in the exchange after some induction period. Various mechanisms providing the regioselective H/D exchange on Zn2+/H-BEA as well as the involvement of the methylene group after the induction period on ZnO/H-BEA are discussed. © 2019 Elsevier Inc.

Arzumanov S.S. , Gabrienko A.A. , Toktarev A.V. , Freude D. , Haase J. , Stepanov A.G.
Propane Activation on Zn-Modified Zeolite. The Effect of the Nature of Zn-Species on the Mechanism of H/D Hydrogen Exchange of the Alkane with Brønsted Acid Sites
Journal of Catalysis. 2019. V.378. P.341-352. DOI: 10.1016/j.jcat.2019.09.006 WOS Scopus РИНЦ ANCAN OpenAlex

Submitted:	May 16, 2019
Accepted:	Sep 4, 2019
Published online:	Sep 25, 2019
Published print:	Oct 1, 2019

Web of science:	WOS:000494887100038
Scopus:	2-s2.0-85072571872
Elibrary:	41677003
Chemical Abstracts:	2019:1867441
Chemical Abstracts (print):	171:456650
OpenAlex:	W2976773995

DB	Citing
Scopus	29
Web of science	29
Elibrary	28
OpenAlex	29