Oxidation of Methane to Methanol on the Surface of FeZSM-5 Zeolite Full article
Journal |
Journal of Catalysis
ISSN: 0021-9517 , E-ISSN: 1090-2694 |
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Output data | Year: 2013, Volume: 300, Pages: 47-54 Pages count : 8 DOI: 10.1016/j.jcat.2012.12.030 | ||
Tags | α-Oxygen, 13C MAS NMR, FeZSM-5, IR spectroscopy, Methane oxidation, Methanol from methane, Nitrous oxide, Product extraction, Quasicatalytic reaction mode, Spillover | ||
Authors |
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Affiliations |
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Funding (2)
1 | Russian Foundation for Basic Research | 12-03-00063 |
2 | Russian Foundation for Basic Research | 12-03-31701 |
Abstract:
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.
Cite:
Starokon E.V.
, Parfenov M.V.
, Arzumanov S.S.
, Pirutko L.V.
, Stepanov A.G.
, Panov G.I.
Oxidation of Methane to Methanol on the Surface of FeZSM-5 Zeolite
Journal of Catalysis. 2013. V.300. P.47-54. DOI: 10.1016/j.jcat.2012.12.030 WOS Scopus РИНЦ ANCAN OpenAlex
Oxidation of Methane to Methanol on the Surface of FeZSM-5 Zeolite
Journal of Catalysis. 2013. V.300. P.47-54. DOI: 10.1016/j.jcat.2012.12.030 WOS Scopus РИНЦ ANCAN OpenAlex
Dates:
Submitted: | Sep 19, 2012 |
Accepted: | Dec 23, 2012 |
Published online: | Feb 1, 2013 |
Published print: | Apr 1, 2013 |
Identifiers:
Web of science: | WOS:000317558000006 |
Scopus: | 2-s2.0-84874873175 |
Elibrary: | 20435042 |
Chemical Abstracts: | 2013:417822 |
Chemical Abstracts (print): | 158:392516 |
OpenAlex: | W2002612078 |