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

Sergei S. Arzumanov, Anton A. Gabrienko, Alexander V. Toktarev, Dieter Freude, Jürgen Haase, Alexander G. Stepanov

Результат исследования: Научные публикации в периодических изданияхстатья

4 Цитирования (Scopus)

Аннотация

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.

Язык оригиналаанглийский
Страницы (с-по)341-352
Число страниц12
ЖурналJournal of Catalysis
Том378
DOI
СостояниеОпубликовано - 1 окт 2019

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