Epoxidation of Ethylene by Anion Radicals of α-Oxygen on the Surface of FeZSM-5 Zeolite
Научная публикация
| Общее |
Язык:
Английский,
Жанр:
Статья (Full article),
Статус опубликования:
Опубликована,
Оригинальность:
Оригинальная
|
| Журнал |
Journal of Catalysis
ISSN: 0021-9517
, E-ISSN: 1090-2694
|
| Вых. Данные |
Год: 2014,
Том: 309,
Страницы: 453-459
Страниц
: 7
DOI:
10.1016/j.jcat.2013.11.001
|
| Ключевые слова |
α-Oxygen, Ethylene epoxidation, Infrared spectroscopy, N2O oxidant, Oxygen anion radicals, Product extraction |
| Авторы |
Starokon Eugeny V.
1
,
Parfenov Mikhail V.
1
,
Pirutko Larisa V.
1
,
Soshnikov Igor E.
1
,
Panov Gennady I.
1
|
| Организации |
| 1 |
Институт катализа им. Г.К. Борескова СО РАН
|
|
Информация о финансировании (2)
|
1
|
Российский фонд фундаментальных исследований
|
12-03-00063
|
|
2
|
Российский фонд фундаментальных исследований
|
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.