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The Fe Active Dites in FeZSM-5 Catalyst for Selective Oxidation of CH4 to CH3OH at Room Temperature Научная публикация

Журнал Journal of Radioanalytical and Nuclear Chemistry
ISSN: 0236-5731 , E-ISSN: 1588-2780
Вых. Данные Год: 2000, Том: 246, Номер: 1, Страницы: 149-152 Страниц : 4 DOI: 10.1023/A:1006722207492
Ключевые слова hydroxide; iron derivative; methane; methyl group; zeolite
Авторы Ovanesyan N.S. 1 , Dubkov K.A. 2 , Pyalling A.A. 1 , Shteinman A.A. 1
Организации
1 Institute of Problems of Chemical Physics, RAS, Chernogolovka, 142432 Russia
2 Boreskov Institute of Catalysis, RAS, Novosibirsk, 630090 Russia

Информация о финансировании (1)

1 Российский фонд фундаментальных исследований 97-03-33754

Реферат: It was shown recently that iron complexes formed during the thermal treatment of FeZSM-5 zeolite perform single-turnover cycles of methane oxidation to methanol at ambient conditions when nitrous oxide is used as a source of oxygen. The long-living active intermediate is capable of transferring accepted O atom (called α-oxygen) into C-H bond of methane to produce methanol at 100% selectivity. The present work is aimed to the identification of iron active sites through a comparison of in situ 57Fe Mössbauer spectra of FeZSM-5 after various thermal treatments and reaction stages. It is established that vacuum activation at 900 °C accompanied by a manifold increase of α-centers leads to the transformation of inactive Fe3+ to the active, coordinatively unsaturated Fe2+ states. After α-oxygen loading, active Fe2+ states transform to a new Fe3+ states responsible for further methane oxidation. The latter reaction, as well as reaction with 2H2, is not fully reversible: part of active Fe3+ transforms to other inactive Fe3+ form. On the contrary, reaction of α-oxygen with CO leads to a complete restoration of the initial, vacuum activated Fe2+ states. On the base of joint Mössbauer and catalytic data, the structure and composition of iron active centers are suggested.
Библиографическая ссылка: Ovanesyan N.S. , Dubkov K.A. , Pyalling A.A. , Shteinman A.A.
The Fe Active Dites in FeZSM-5 Catalyst for Selective Oxidation of CH4 to CH3OH at Room Temperature
Journal of Radioanalytical and Nuclear Chemistry. 2000. V.246. N1. P.149-152. DOI: 10.1023/A:1006722207492 WOS Scopus РИНЦ CAPlusCA OpenAlex
Даты:
Поступила в редакцию: 8 мая 2000 г.
Опубликована в печати: 1 окт. 2000 г.
Идентификаторы БД:
Web of science: WOS:000090034600025
Scopus: 2-s2.0-0033788654
РИНЦ: 13357717
Chemical Abstracts: 2000:785437
Chemical Abstracts (print): 134:56350
OpenAlex: W1756312672
Цитирование в БД:
БД Цитирований
Web of science 30
Scopus 36
РИНЦ 32
OpenAlex 29
Альметрики: