Oxidation of Methane to Methanol 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: 2013,
Том: 300,
Страницы: 47-54
Страниц
: 8
DOI:
10.1016/j.jcat.2012.12.030
|
| Ключевые слова |
α-Oxygen, 13C MAS NMR, FeZSM-5, IR spectroscopy, Methane oxidation, Methanol from methane, Nitrous oxide, Product extraction, Quasicatalytic reaction mode, Spillover |
| Авторы |
Starokon Eugeny V.
1
,
Parfenov Mikhail V.
1
,
Arzumanov Sergey S.
1
,
Pirutko Larisa V.
1
,
Stepanov Alexander G.
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
|
In our previous work using FeZSM-5 zeolite with increased concentration of alpha-sites (100 mcmol/g), the oxidation of methane by a-oxygen predeposited from nitrous oxide was studied at room temperature. The reaction proceeded by hydrogen abstraction mechanism yielding methoxy and hydroxy groups bound to alpha-sites.
The present work conducted with the same zeolite is devoted to methane oxidation by N2O in the process of alpha-oxygen deposition at 160oC. Under these conditions, the reaction was shown to proceed at a stoichiometric ratio CH4 : N2O = 1:1 yielding directly methanol. Spillover of methanol from alpha-sites liberates them for further events of a-oxygen deposition, thus converting the reaction to a ‘‘quasicatalytic’’ mode that runs up to turnover number exceeding 3 with no product desorption into the gas phase. A part of methanol is converted to dimethyl ether, traces of acetaldehyde, and some amount of non-extractable products.
Mechanism of the reaction is discussed.