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Publication Details
AFRICAN RESEARCH NEXUS
SHINING A SPOTLIGHT ON AFRICAN RESEARCH
Catalytic and mechanistic insights of the low-temperature selective oxidation of methane over Cu-promoted Fe-ZSM-5
Chemistry - A European Journal, Volume 18, No. 49, Year 2012
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Description
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 H2O 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 C1-oxidation to proceed under intrinsically mild reaction conditions. Activate methane! A reaction network consisting of the activation of methane, the formation of an activated hydroperoxy species, and the by-production of hydroxyl radicals is presented (see scheme). The catalytic system results in a low-energy methane activation route, and allows selective C1-oxidation to proceed under intrinsically mild reaction conditions. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Authors & Co-Authors
Hammond, Ceri
United Kingdom, Cardiff
Cardiff University
Switzerland, Zurich
Eth Zürich
Jenkins, Robert L.
United Kingdom, Cardiff
Cardiff University
Dimitratos, Nikolaos
United Kingdom, Cardiff
Cardiff University
Lopez-Sanchez, Jose A.
United Kingdom, Cardiff
Cardiff University
Ab Rahim, Mohd Hasbi
United Kingdom, Cardiff
Cardiff University
Murphy, Damien Martin
United Kingdom, Cardiff
Cardiff University
Moulijn, Jacob M.
United Kingdom, Cardiff
Cardiff University
Taylor, Stuart H.
United Kingdom, Cardiff
Cardiff University
Willock, David J.
United Kingdom, Cardiff
Cardiff University
Hutchings, Graham John
United Kingdom, Cardiff
Cardiff University
Statistics
Citations: 97
Authors: 10
Affiliations: 3
Identifiers
Doi:
10.1002/chem.201202802
ISSN:
15213765