Propane Transformation on Zn-Modified Zeolite. Effect of the Nature of Zn Species on Alkane Aromatization and Hydrogenolysis
Full article
| Общее |
Language:
Английский,
Genre:
Full article,
Status:
Published,
Source type:
Original
|
| Journal |
The Journal of Physical Chemistry C
ISSN: 1932-7447
, E-ISSN: 1932-7455
|
| Output data |
Year: 2019,
Volume: 123,
Number: 50,
Pages: 30473-30485
Pages count
: 13
DOI:
10.1021/acs.jpcc.9b09718
|
| Tags |
SOLID-STATE NMR; IN-SITU NMR; BRONSTED ACID SITES; METHANE ACTIVATION; LIGHT ALKANES; Zn/MFI CATALYST; INITIAL-STAGES; H/D EXCHANGE; CONVERSION; H-ZSM-5 |
| Authors |
Arzumanov Sergei S.
1,2
,
Gabrienko Anton A.
1,2
,
Toktarev Alexander V.
1
,
Lashchinskaya Zoya N.
1,2
,
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 |
Faculty of Natural Sciences, Department of Physical Chemistry, Novosibirsk State University, Pirogova Str. 2, Novosibirsk, 630090, Russia
|
| 3 |
Fakultät für Physik und Geowissenschaften, Universität Leipzig, Linnéstr. 5, Leipzig, 04103, Germany
|
|
Funding (2)
|
1
|
Russian Science Foundation
German Research Foundation
|
19-43-04101
|
|
2
|
German Research Foundation
|
HA 1893/22-1
|
With regard to establishing the effect of the nature of Zn species loaded in a zeolite on the aromatization of propane, the transformation of 13C-labeled propane (propane-1-13C and propane-2-13C) has been monitored by 1H and 13C (CP) MAS NMR at 296-623 K for two zeolite samples, containing exclusively either isolated Zn2+ cations (Zn2+/H-BEA zeolite sample) or small (ZnO)n clusters of zinc oxide (ZnO/H-BEA zeolite sample). It has been established that similar intermediates, π-complex of propene and σ-allylzinc species, are formed at propane transformation to aromatics on both zeolite samples. However, the formation of the identified intermediates and their evolution to final aromatic products have been detected to occur on Zn2+/H-BEA at lower temperature (by 100 K) as compared to the same transformation on ZnO/H-BEA zeolite. Analysis of the kinetics of propane transformation by 1H MAS NMR in situ has shown similar regularities for propane aromatization and hydrogenolysis on the different zeolite samples, but the reactions on Zn2+/H-BEA occur 10 times faster than on ZnO/H-BEA. This allows us to conclude on a higher efficiency of Zn2+ cations compared to ZnO species for propane aromatization on Zn-modified zeolites. © 2019 American Chemical Society.