Degradation pathways of a highly active iron(iii) tetra-NHC epoxidation catalyst

Dyckhoff, Florian, Schlagintweit, Jonas F., Bernd, Marco A., Jakob, Christian H. G., Schlachta, Tim P., Hofmann, Benjamin J., Reich, Robert M. and Kühn, Fritz E. (2021) Degradation pathways of a highly active iron(iii) tetra-NHC epoxidation catalyst. Catalysis Science & Technology, 11 (3). pp. 795-799. ISSN 2044-4753

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Abstract

Pivotal degradation pathways of the most active non-heme iron epoxidation catalyst to date are investigated in detail. In-depth HR-ESI-MS and NMR spectroscopy decomposition studies and comparative catalytic experiments exclude the generally accepted literature paths of μ2-oxo bridged FeIII–O–FeIII dimer formation and methylene bridge oxidation. Instead, the Fe–NHC bond has been identified as the “weak spot”. It is shown that direct oxidation of one of the carbenes (ImC[double bond, length as m-dash]O) results in its de-coordination and induces protonation of the other NHC moieties, thus completely deactivating the catalyst. Evidence for protonation prior to carbene oxidation has not been found in this study.

Item Type: Article
Uncontrolled Keywords: catalysis ,/dk/atira/pure/subjectarea/asjc/1500/1503
Faculty \ School: Faculty of Science > School of Chemistry
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Depositing User: LivePure Connector
Date Deposited: 17 Jul 2021 00:12
Last Modified: 21 Jul 2021 01:50
URI: https://ueaeprints.uea.ac.uk/id/eprint/80626
DOI: 10.1039/D0CY02433C

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