화학공학소재연구정보센터
Journal of Catalysis, Vol.378, 341-352, 2019
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 Bronsted acid sites
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 Brensted acid sites (BAS) with deuterated propane-d(8) 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-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. (C) 2019 Elsevier Inc. All rights reserved.