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4085467 
Journal Article 
Oxidation of methane to methanol on the surface of FeZSM-5 zeolite 
Starokon, EV; Parfenov, MV; Arzumanov, SS; Pirutko, LV; Stepanov, AG; Panov, GI 
2013 
Yes 
Journal of Catalysis
ISSN: 0021-9517
EISSN: 1090-2694 
Elsevier 
300 
Elsevier 
47-54 
English 
WOS:000317558000006 
In our previous work using FeZSM-5 zeolite with increased concentration of alpha-sites (100 mu mol/g), the oxidation of methane by alpha-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 160 degrees C. 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 alpha-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. (C) 2013 Elsevier Inc. All rights reserved. 
FeZSM-5; Nitrous oxide; Methane oxidation; Methanol from methane; alpha-Oxygen; Quasicatalytic reaction mode; IR spectroscopy; C-13 MAS NMR; Product extraction; Spillover