Mixed-valence hydrides at [FeFe]-hydrogenase active site mimics

Wright, Joseph A. ORCID: https://orcid.org/0000-0001-9603-1001, Madlool, Atheer M. and Cottrell, Stephen P. (2023) Mixed-valence hydrides at [FeFe]-hydrogenase active site mimics. Journal of Physics: Conference Series, 2462. ISSN 1742-6588

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The number of methods to study transient paramagnetic hydrides at organometallic centres is extremely limited. The reactivity of {2Fe2S} centres with protons to produce both diamagnetic and paramagnetic systems is of central interest in developing novel catalysts for hydrogen production, inspired by the [FeFe]-hydrogenase enzymes. Here, we show how a combination of spectroscopic and electrochemical techniques is allowing access to detail of the reactivity of key species on these pathways. Electron paramagnetic resonance and infra-red spectroelectrochemical approaches have been used to observe the reduction of pre-generated diamagnetic hydrides. In contrast, avoided level crossing muon spin resonance (ALC-µSR) has been used to form the open-shell species directly and to examine the formation of short-lived intermediates in the reaction process. The combination of these techniques suggests the involvement of terminal hydrides or CO-protonation states on the pathway to the isolable bridging hydride products.

Item Type: Article
Additional Information: Issue for the 15th International Conference on Muon Spin Rotation, Relaxation and Resonance 28/08/2022 - 02/09/2022 Parma, Italy. Funding Information: The authors thank the Leverhulme Trust for funding (grant RPG-2019-115).
Uncontrolled Keywords: physics and astronomy(all),sdg 7 - affordable and clean energy ,/dk/atira/pure/subjectarea/asjc/3100
Faculty \ School: Faculty of Science > School of Chemistry
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Depositing User: LivePure Connector
Date Deposited: 11 Sep 2023 09:30
Last Modified: 07 May 2024 01:37
URI: https://ueaeprints.uea.ac.uk/id/eprint/93013
DOI: 10.1088/1742-6596/2462/1/012054


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