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Catalytic and mechanistic insights of the low-temperature selective oxidation of methane over Cu-promoted Fe-ZSM-5

Hammond, Ceri, Jenkins, Robert Leyshon, Dimitratos, Nikolaos, Lopez-Sanchez, Jose Antonio, Ab Rahim, Mohd Hasbi, Forde, Michael M., Thetford, Adam, Murphy, Damien Martin, Hagen, Henk, Stangland, Eric E., Moulijn, Jacob, Taylor, Stuart Hamilton, Willock, David James and Hutchings, Graham John 2012. Catalytic and mechanistic insights of the low-temperature selective oxidation of methane over Cu-promoted Fe-ZSM-5. Chemistry - a European Journal 18 (49) , pp. 15735-15745. 10.1002/chem.201202802

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Abstract

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 H2O2 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.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Advanced Research Computing @ Cardiff (ARCCA)
Chemistry
Cardiff Catalysis Institute (CCI)
Subjects: Q Science > QD Chemistry
Uncontrolled Keywords: catalysis; gas; heterogeneous catalysis; methane; oxidation; zeolites
Publisher: Wiley Blackwell
ISSN: 0947-6539
Funders: EPSRC
Last Modified: 24 May 2019 01:56
URI: http://orca.cf.ac.uk/id/eprint/41347

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