Muonium chemistry at diiron subsite analogues of [FeFe]-hydrogenase

Wright, Joseph A. ORCID: https://orcid.org/0000-0001-9603-1001, Peck, Jamie N. T., Cottrell, Stephen P., Jablonskyte, Ausra, Oganesyan, Vasily S. ORCID: https://orcid.org/0000-0002-8738-1146, Pickett, Christopher J. and Jayasooriya, Upali A. (2016) Muonium chemistry at diiron subsite analogues of [FeFe]-hydrogenase. Angewandte Chemie-International Edition, 55 (47). 14580–14583. ISSN 1433-7851

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Abstract

The chemistry of metal hydrides is implicated in a range of catalytic processes at metal centres. Gaining insight into the formation of such sites by protonation and/or electronation is therefore of significant value in fully exploiting the potential of such systems. Here, we show that the muonium radical (Mu·), used as a low isotopic mass analogue of hydrogen, can be exploited to probe the early stages of hydride formation at metal centres. Mu· undergoes the same chemistry as H· and can be directly observed due to its short lifetime (in the microseconds) and unique breakdown signature. By implanting Mu· into three models of the [FeFe]-hydrogenase active site we have been able to detect key muoniated intermediates of direct relevance to the hydride chemistry of these systems.

Item Type:	Article
Uncontrolled Keywords:	enzyme mimics,[fefe]-hydrogenase,hydrogen,muonium
Faculty \ School:	Faculty of Science > School of Chemistry (former - to 2024)
UEA Research Groups:	Faculty of Science > Research Groups > Chemistry of Materials and Catalysis Faculty of Science > Research Groups > Chemistry of Light and Energy Faculty of Science > Research Groups > Chemistry of Life Processes Faculty of Science > Research Centres > Centre for Molecular and Structural Biochemistry Faculty of Science > Research Groups > Energy Materials Laboratory Faculty of Science > Research Groups > Centre for Photonics and Quantum Science
Depositing User:	Pure Connector
Date Deposited:	26 Sep 2016 16:00
Last Modified:	05 Dec 2024 01:17
URI:	https://ueaeprints.uea.ac.uk/id/eprint/60596
DOI:	10.1002/ange.201607109

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