Tuning the Mechanism of H/D Exchange for Isobutane on H-BEA by Loading Zn Species in Zeolite

被引：1
|
作者：
Arzumanov, Sergei S. [1 ]
Gabrienko, Anton A. [1 ]
Freude, Dieter [2 ]
Haase, Juergen [2 ]
Stepanov, Alexander G. [1 ]
机构：
[1] Russian Acad Sci, Boreskov Inst Catalysis, Siberian Branch, Prospekt Akad Lavrentieva 5, Novosibirsk 630090, Russia
[2] Univ Leipzig, Fak Phys & Geowissensch, Linnestr 5, D-04103 Leipzig, Germany
来源：
CHEMISTRY-A EUROPEAN JOURNAL | 2023年 / 29卷 / 05期
关键词：
alkanes; H; D exchange; in situ NMR spectroscopy; kinetics; reaction mechanism; zeolites; IN-SITU H-1; SOLID-STATE NMR; SMALL ALKANES; ACTIVATION-ENERGY; LOW-TEMPERATURE; AB-INITIO; PROPANE ACTIVATION; HYDROGEN-EXCHANGE; ZINC IONS; ACID;
D O I：
10.1002/chem.202202962
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
Kinetics of H/D hydrogen exchange between deuterated isobutane-d(10) and Bronsted acid sites (BAS) of three zeolite samples (H-BEA, ZnO/H-BEA, Zn2+/H-BEA) were monitored with H-1 MAS NMR in situ at 343-468 K. The regioselective H/D exchange in the methyl groups detected on H-BEA can be rationalized in terms of the mechanism of indirect exchange, which involves protonation of the intermediate olefin and further hydride abstraction from the other alkane molecule by the formed carbenium ion. Loading of Zn species in the zeolite results in a decrease of the rate and an increase of the activation energy of the exchange. The loaded Zn species provide the tuning effect on the reaction occurrence, changing the mechanism from the indirect one to the mechanism of the direct exchange.
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页数：9
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