On the Role of Brønsted Acidity in theOxidation of Benzene to Phenol by Nitrous Oxide
Научная публикация
| Общее |
Язык:
Английский,
Жанр:
Статья (Full article),
Статус опубликования:
Опубликована,
Оригинальность:
Оригинальная
|
| Журнал |
Applied Catalysis A: General
ISSN: 0926-860X
, E-ISSN: 1873-3875
|
| Вых. Данные |
Год: 1996,
Том: 141,
Номер: 1-2,
Страницы: 185-192
Страниц
: 8
DOI:
10.1016/0926-860X(96)00055-5
|
| Ключевые слова |
Acidity, Benzene, Hydroxylation, Nitrous oxide, Oxidation, Phenol, ZSM-5 |
| Авторы |
Sobolev V.I.
1
,
Dubkov K.A.
1
,
Paukshtis E.A.
1
,
Pirutko L.V.
1
,
Rodkin M.A.
2
,
Kharitonov A.S.
1
,
Panov G.I.
1
|
| Организации |
| 1 |
Boreskov Institute of Catalysis, Novosibirsk, 630090
|
| 2 |
A Unit of Monsanto Company, P.O. Box 97
|
|
Oxidation of benzene to phenol with nitrous oxide being an untypical reaction for zeolite catalysis arouses a great interest among researchers. Several hypotheses concerning reaction mechanism are discussed. Some of them assume a key role of the Brønsted acid centers (BAC), though few experimental support for this idea is available. The goal of this work is to study the Brønsted acidity of FeZSM-5 zeolite catalyst (0.13 wt.% Fe2O3) to reveal a relationship (if any) between the BAC concentration and the catalytic activity in benzene oxidation. Various pretreatments of the sample including a high-temperature calcination up to 900°C were used to vary the BAC concentration, which was measured by infrared spectrometry. No evidence of the Brønsted acidity importance for catalyzing the reaction was found. What is more, a formal inverse correlation was discovered. Thus, a manifold decrease in BAC concentration was accompanied by a remarkable increase in the oxidation rate, with a small acid recreation under the reaction conditions used. The obtained results support an earlier suggested redox mechanism of the reaction involving a special oxygen form produced at N2O decomposition on Fe-containing active sites.