n-Butane Transformation on Zn/H-BEA. The Effect of Different Zn Species (Zn2+ and ZnO) on the Reaction Performance
Full article
| Общее |
Language:
Английский,
Genre:
Full article,
Status:
Published,
Source type:
Original
|
| Journal |
Journal of Catalysis
ISSN: 0021-9517
, E-ISSN: 1090-2694
|
| Output data |
Year: 2020,
Volume: 391,
Pages: 69-79
Pages count
: 11
DOI:
10.1016/j.jcat.2020.08.011
|
| Tags |
Aromatization; Hydrogenolysis; Kinetics; Mechanism; n-butane; Solid-state NMR; Zeolite BEA; Zn2+ cations; ZnO clusters |
| Authors |
Gabrienko Anton A.
1,2
,
Arzumanov Sergei S.
1,2
,
Lashchinskaya Zoya N.
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, Russia
|
| 2 |
Novosibirsk State University, Faculty of Natural Sciences, Department of Physical Chemistry, Pirogova Str. 2, Novosibirsk 630090, Russia
|
| 3 |
Universität Leipzig, Fakultät für Physik und Geowissenschaften, Linnéstr. 5, 04103 Leipzig, Germany
|
|
Funding (2)
|
1
|
Russian Science Foundation
German Research Foundation
|
19-43-04101
|
|
2
|
German Research Foundation
|
HA 1893/22-1
|
Using solid-state 1H and 13C MAS NMR spectroscopy, the performance of H-BEA zeolite, modified with either Zn2+ cations (Zn2+/H-BEA) or ZnO clusters (ZnO/H-BEA), has been investigated with respect to n-butane transformation by aromatization and hydrogenolysis pathways. 13C-labeled n-butane has been used to follow the main stages of n-butane transformation on both Zn2+/H-BEA and ZnO/H-BEA with 13C MAS NMR at 298–623 K. Similar surface species, including n-butylzinc, n-butene, allyl-like oligomers, are formed as the intermediates on both zeolites. The kinetics of n-butane transformation has been monitored with 1H MAS NMR in situ at 543–573 K. Kinetics modeling reveals that Zn2+/H-BEA is more active for n-butane transformation than ZnO/H-BEA. A remarkable difference in the rates and the pathways of hydrogenolysis for Zn2+/H-BEA and ZnO/H-BEA has also been established. Propane and methane are hydrogenolysis products on ZnO/H-BEA whereas ethane is produced by the reaction on Zn2+/H-BEA. 13C NMR data and the kinetics analysis provide an insight on the occurrence of joint methane and n-butane conversion on Zn-modified zeolites under non-oxidative conditions. © 2020 Elsevier Inc.