Significant Influence of Zn on Activation of the C-H Bonds of Small Alkanes by Brønsted Acid Sites of Zeolite
Full article
| Общее |
Language:
Английский,
Genre:
Full article,
Status:
Published,
Source type:
Original
|
| Journal |
ChemPhysChem
ISSN: 1439-4235
, E-ISSN: 1439-7641
|
| Output data |
Year: 2008,
Volume: 9,
Number: 17,
Pages: 2559-2563
Pages count
: 5
DOI:
10.1002/cphc.200800569
|
| Tags |
Alkanes, H/D exchange, Heterogeneous catalysis, Solid-state NMR, Zeolites |
| Authors |
Stepanov Alexander G.
1
,
Arzumanov Sergei S.
1
,
Gabrienko Anton A.
1
,
Parmon Valentin N.
1
,
Ivanova Irina I.
2
,
Freude Dieter
3
|
| Affiliations |
| 1 |
Boreskov Institute of Catalysis, Siberian Branch of the Russian Academy of Sciences, Prospekt Akademika Lavrentieva 5, Novosibirsk 630090 (Russia)
|
| 2 |
Department of Chemistry, Moscow State University, Lenin Hills 1, Bld. 3, Moscow 119992 (Russia)
|
| 3 |
Abteilung Grenzflchenphysik, Universitt Leipzig, Linnstraße 5, 04103 Leipzig (Germany)
|
|
Funding (3)
|
1
|
Russian Foundation for Basic Research
|
07-03-00136
|
|
2
|
German Research Foundation
|
FR 902/15
|
|
3
|
International Association for the Promotion of Co-operation with Scientists from the New Independent States of the Former Soviet Union
|
03-51-5286
|
Herein, we analyze earlier obtained and new data about peculiarities of the H/D hydrogen exchange of small C1–n-C4 alkanes on Zn-modified high-silica zeolites ZSM-5 and BEA in comparison with the exchange for corresponding purely acidic forms of these zeolites. This allows us to identify an evident promoting effect of Zn on the activation of CH bonds of alkanes by zeolite Brønsted sites. The effect of Zn is demonstrated by observing the regioselectivity of the H/D exchange for propane and n-butane as well as by the increase in the rate and a decrease in the apparent activation energy of the exchange for all C1–n-C4 alkanes upon modification of zeolites with Zn. The influence of Zn on alkane activation has been rationalized by dissociative adsorption of alkanes on Zn oxide species inside zeolite pores, which precedes the interaction of alkane with Brønsted acid sites.