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Publication Details
AFRICAN RESEARCH NEXUS
SHINING A SPOTLIGHT ON AFRICAN RESEARCH
Elucidation and evolution of the active component within Cu/Fe/ZSM-5 for catalytic methane oxidation: From synthesis to catalysis
ACS Catalysis, Volume 3, No. 4, Year 2013
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Description
The development of a catalytic, one-step route for the oxidation of methane to methanol remains one of the greatest challenges within catalysis. Of particular importance is the need to develop an efficient route that proceeds under mild reaction conditions so as to avoid deeper oxidation and the economic limitations of the currently practiced syngas route. Recently, it was demonstrated that a copper- and iron-containing zeolite is an efficient catalyst for such a one-step process. The catalyst in question (Cu-Fe-ZSM-5) is capable of selectively transforming methane to methanol in an aqueous medium with hydrogen peroxide as the terminal oxidant. Nevertheless, despite its high activity and unparalleled methanol selectivity, the origin of its activity and the precise nature of its active species are not yet fully understood. Through a combination of catalytic and spectroscopic studies, we hereby demonstrate that extraframework Fe species are the active component of the catalyst for methane oxidation, although the speciation of these sites from synthesis to catalysis significantly alters the observed activity and selectivity. The analogies and differences between this system and other iron-containing zeolite-catalyzed processes, such as N2O-mediated benzene hydroxylation, are also considered. © 2013 American Chemical Society.
Authors & Co-Authors
Hammond, Ceri
United Kingdom, Cardiff
Cardiff University
Switzerland, Zurich
Eth Zürich
Dimitratos, Nikolaos
United Kingdom, Cardiff
Cardiff University
United Kingdom, London
University College London
United Kingdom, Didcot
Rutherford Appleton Laboratory
Jenkins, Robert L.
United Kingdom, Cardiff
Cardiff University
Lopez-Sanchez, Jose A.
United Kingdom, Cardiff
Cardiff University
United Kingdom, Liverpool
University of Liverpool
Kondrat, Simon A.
United Kingdom, Cardiff
Cardiff University
Ab Rahim, Mohd Hasbi
United Kingdom, Cardiff
Cardiff University
Taylor, Stuart H.
United Kingdom, Cardiff
Cardiff University
Moulijn, Jacob M.
United Kingdom, Cardiff
Cardiff University
Willock, David J.
United Kingdom, Cardiff
Cardiff University
Hutchings, Graham John
United Kingdom, Cardiff
Cardiff University
Statistics
Citations: 111
Authors: 10
Affiliations: 6
Identifiers
Doi:
10.1021/cs3007999
ISSN:
21555435