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 |
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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 |
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Affiliations |
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Funding (2)
1 |
Russian Science Foundation German Research Foundation |
19-43-04101 |
2 | German Research Foundation | HA 1893/22-1 |
Abstract:
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.
Cite:
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
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
Dates:
Submitted: | May 16, 2019 |
Accepted: | Sep 4, 2019 |
Published online: | Sep 25, 2019 |
Published print: | Oct 1, 2019 |
Identifiers:
Web of science: | WOS:000494887100038 |
Scopus: | 2-s2.0-85072571872 |
Elibrary: | 41677003 |
Chemical Abstracts: | 2019:1867441 |
Chemical Abstracts (print): | 171:456650 |
OpenAlex: | W2976773995 |