Biomimetic oxidation with Fe-ZSM-5 and H2O2? Identification of an active, extra-framework binuclear core and an FeIII-OOH intermediate with resonance-enhanced Raman Spectroscopy

Hammond, Ceri ORCID: https://orcid.org/0000-0002-9168-7674, Hermans, Ive and Dimitratos, Nikolaos ORCID: https://orcid.org/0000-0002-6620-4335 2015. Biomimetic oxidation with Fe-ZSM-5 and H2O2? Identification of an active, extra-framework binuclear core and an FeIII-OOH intermediate with resonance-enhanced Raman Spectroscopy. ChemCatChem 7 (3) , pp. 434-440. 10.1002/cctc.201402642

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Abstract

Developing inorganic materials that can mimic nature’s ability to selectively oxidise inert C[BOND]H bonds remains a topic of intense scientific research. In recent years, zeolitic materials containing Fe and/or Cu have been shown to be highly active, heterogeneous catalysts for the selective oxidation of alkanes (including methane), amongst a range of other related oxidation challenges. By using resonance-enhanced Raman spectroscopy, we demonstrate that, following high-temperature pre-treatment (activation), Fe-containing ZSM-5 possesses an active binuclear core, and forms a key Fe[BOND]OOH intermediate upon activation with H2O2. Both factors are reminiscent of biological oxidation catalysts, and may account for the unique ability of this material to selectively oxidise methane to methanol at low temperature.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry
Subjects:	Q Science > QD Chemistry
Uncontrolled Keywords:	biomimetic catalysis; C[BOND]H activation; in situ analysis; methane oxidation; zeolites
Publisher:	Wiley
ISSN:	1867-3880
Last Modified:	27 Oct 2022 10:09
URI:	https://orca.cardiff.ac.uk/id/eprint/69093

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