Epoxidation of Ethylene by Anion Radicals of α-Oxygen on the Surface of FeZSM-5 Zeolite
Science 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: 2014,
Volume: 309,
Pages: 453-459
Pages count
: 7
DOI:
10.1016/j.jcat.2013.11.001
|
| Tags |
α-Oxygen, Ethylene epoxidation, Infrared spectroscopy, N2O oxidant, Oxygen anion radicals, Product extraction |
| Authors |
Starokon Eugeny V.
1
,
Parfenov Mikhail V.
1
,
Pirutko Larisa V.
1
,
Soshnikov Igor E.
1
,
Panov Gennady I.
1
|
| Affiliations |
| 1 |
Boreskov Institute of Catalysis SB RAS
|
|
Funding (2)
|
1
|
Russian Foundation for Basic Research
|
12-03-00063
|
|
2
|
Russian Foundation for Basic Research
|
12-03-31701
|
The stoichiometric oxidation of ethylene by anion radicals of α-oxygen, (FeIII–O-)α, created on the surface of non-modified and Na-modified FeZSM-5 zeolite was studied in the temperature range from 25 down to -60oC. Upon extraction, the products were identified using the gas chromatography, gas chromatography–mass spectrometry, and nuclear magnetic resonance. Unlike the oxidation of methane, the reaction C2H4 + Oα was shown to proceed without hydrogen abstraction from the ethylene (infrared spectroscopy data). It leads to Oα addition over the double C=C bond yielding the ethylene oxide (EO) primary product. Sodium modification of the zeolite strongly increases the selectivity for EO, which attains 80-84% at the reaction temperature of 60oC. A much lower selectivity at room temperature relates mainly to a secondary reaction of EO with ethylene leading to butyraldehyde.
High epoxidizing selectivity of α-oxygen is discussed in relation to the mechanism of ethylene epoxidation on silver catalyst.