Kinetic Isotope Effects and Mechanism of Biomimetic Oxidation of Methane and Benzene on FeZSM-5 Zeolite Full article
| Journal |
Journal of Molecular Catalysis A: Chemical
ISSN: 1381-1169 |
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| Output data | Year: 1997, Volume: 123, Number: 2-3, Pages: 155-161 Pages count : 7 DOI: 10.1016/S1381-1169(97)00051-4 | ||||||
| Tags | Biomimetic oxidation, FeZSM-5, Kinetic isotope effect, Nitrous oxide, Oxidation of benzene to phenol, Oxidation of methane to methanol | ||||||
| Authors |
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| Affiliations |
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Funding (1)
| 1 | Russian Foundation for Basic Research | 96-03-32985 |
Abstract:
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 CH 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.
Cite:
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 ANCAN OpenAlex
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 ANCAN OpenAlex
Dates:
| Submitted: | Nov 8, 1996 |
| Accepted: | Feb 18, 1997 |
| Published print: | Aug 29, 1997 |
| Published online: | Mar 26, 1998 |
Identifiers:
| Web of science: | WOS:A1997XP87100009 |
| Scopus: | 2-s2.0-0030758178 |
| Elibrary: | 13270464 |
| Chemical Abstracts: | 1997:442501 |
| Chemical Abstracts (print): | 127:135477 |
| OpenAlex: | W1968748611 |