Document Detail


Catalytic and Mechanistic Insights of the Low-Temperature Selective Oxidation of Methane over Cu-Promoted Fe-ZSM-5.
MedLine Citation:
PMID:  23150452     Owner:  NLM     Status:  Publisher    
Abstract/OtherAbstract:
The partial oxidation of methane to methanol presents one of the most challenging targets in catalysis. Although this is the focus of much research, until recently, approaches had proceeded at low catalytic rates (<10 h(-1) ), not resulted in a closed catalytic cycle, or were unable to produce methanol with a reasonable selectivity. Recent research has demonstrated, however, that a system composed of an iron- and copper-containing zeolite is able to catalytically convert methane to methanol with turnover frequencies (TOFs) of over 14 000 h(-1) by using H(2) O(2) as terminal oxidant. However, the precise roles of the catalyst and the full mechanistic cycle remain unclear. We hereby report a systematic study of the kinetic parameters and mechanistic features of the process, and present a reaction network consisting of the activation of methane, the formation of an activated hydroperoxy species, and the by-production of hydroxyl radicals. The catalytic system in question results in a low-energy methane activation route, and allows selective C(1) -oxidation to proceed under intrinsically mild reaction conditions.
Authors:
Ceri Hammond; Robert L Jenkins; Nikolaos Dimitratos; Jose Antonio Lopez-Sanchez; Mohd Hasbi Ab Rahim; Michael M Forde; Adam Thetford; Damien M Murphy; Henk Hagen; Eric E Stangland; Jacob M Moulijn; Stuart H Taylor; David J Willock; Graham J Hutchings
Publication Detail:
Type:  JOURNAL ARTICLE     Date:  2012-11-13
Journal Detail:
Title:  Chemistry (Weinheim an der Bergstrasse, Germany)     Volume:  -     ISSN:  1521-3765     ISO Abbreviation:  Chemistry     Publication Date:  2012 Nov 
Date Detail:
Created Date:  2012-11-14     Completed Date:  -     Revised Date:  -    
Medline Journal Info:
Nlm Unique ID:  9513783     Medline TA:  Chemistry     Country:  -    
Other Details:
Languages:  ENG     Pagination:  -     Citation Subset:  -    
Copyright Information:
Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Affiliation:
Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff, CF10 3AT (UK); Current address: Department of Chemistry and Applied Biosciences, ETH Zürich, Wolfgang-Pauli-Str. 10, 8093 Zürich (Switzerland). ceri.hammond@chem.ethz.ch.
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