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Biomimetic Oxidation with Fe‐ZSM‐5 and H 2 O 2 ? Identification of an Active, Extra‐Framework Binuclear Core and an Fe III OOH Intermediate with Resonance‐Enhanced Raman Spectroscopy
Author(s) -
Hammond Ceri,
Hermans Ive,
Dimitratos Nikolaos
Publication year - 2015
Publication title -
chemcatchem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.497
H-Index - 106
eISSN - 1867-3899
pISSN - 1867-3880
DOI - 10.1002/cctc.201402642
Subject(s) - catalysis , chemistry , raman spectroscopy , methanol , methane , heterogeneous catalysis , zeolite , photochemistry , inorganic chemistry , organic chemistry , physics , optics
Developing inorganic materials that can mimic nature’s ability to selectively oxidise inert CH 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 FeOOH intermediate upon activation with H 2 O 2 . 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.