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Kinetic Isotope Effects and Mechanism of Biomimetic Oxidation of Methane and Benzene on FeZSM-5 Zeolite Научная публикация

Журнал Journal of Molecular Catalysis A: Chemical
ISSN: 1381-1169
Вых. Данные Год: 1997, Том: 123, Номер: 2-3, Страницы: 155-161 Страниц : 7 DOI: 10.1016/S1381-1169(97)00051-4
Ключевые слова Biomimetic oxidation, FeZSM-5, Kinetic isotope effect, Nitrous oxide, Oxidation of benzene to phenol, Oxidation of methane to methanol
Авторы Dubkov K.A. 1 , Sobolev V.I. 1 , Talsi E.P. 1 , Rodkin M.A. 2 , Watkins N.H. 2 , Shteinman A.A. 3 , Panov G.I. 1
Организации
1 Boreskov Institute of Catalysis, Siberian Branch of RAS, Novosibirsk 630090, Russia
2 Monsanto Company, P.O. Box 97, Gonzales, FL 32560-0097, USA
3 Instihdte of Chemical Physics in Chemogolouka, RAS, Moscow Region, Chernogolouko 142432, Russia

Информация о финансировании (1)

1 Российский фонд фундаментальных исследований 96-03-32985

Реферат: Earlier, iron complexes stabilized in a ZSM-5 zeolite matrix have been shown to produce a new form of surface oxygen (called α-oxygen) upon decomposition of N2O. α-Oxygen exhibits a very high reactivity typical for oxygen of monooxygenases (MO) and mimics its unique ability in selective oxidation of hydrocarbons at room temperature. Kinetic isotope effect (KIE) measurements reported here reveal additional similarities between MO and the model. Depending on the temperature, the value of KIE for oxidation of methane with α-oxygen ranges from 1.9 to 5.5. For the oxidation of benzene the value of KIE is 1.0. This indicates that both biological and chemical oxidation of methane involves a rate limiting CH bond cleavage, whereas the reaction with benzene is probably limited by the formation of an epoxy-type intermediate. The assumed structure of the active sites as well as some features of the oxidation mechanism allow one to consider FeZSM-5-N2O system as a new and successful model for methane monooxygenase.
Библиографическая ссылка: Dubkov K.A. , Sobolev V.I. , Talsi E.P. , Rodkin M.A. , Watkins N.H. , Shteinman A.A. , Panov G.I.
Kinetic Isotope Effects and Mechanism of Biomimetic Oxidation of Methane and Benzene on FeZSM-5 Zeolite
Journal of Molecular Catalysis A: Chemical. 1997. V.123. N2-3. P.155-161. DOI: 10.1016/S1381-1169(97)00051-4 WOS Scopus РИНЦ CAPlusCA OpenAlex
Даты:
Поступила в редакцию: 8 нояб. 1996 г.
Принята к публикации: 18 февр. 1997 г.
Опубликована в печати: 29 авг. 1997 г.
Опубликована online: 26 мар. 1998 г.
Идентификаторы БД:
Web of science: WOS:A1997XP87100009
Scopus: 2-s2.0-0030758178
РИНЦ: 13270464
Chemical Abstracts: 1997:442501
Chemical Abstracts (print): 127:135477
OpenAlex: W1968748611
Цитирование в БД:
БД Цитирований
Web of science 157
Scopus 167
РИНЦ 167
OpenAlex 164
Альметрики: