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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Abstract
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 |
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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 (former - to 2024) |
Related URLs: | |
Depositing User: | LivePure Connector |
Date Deposited: | 11 Sep 2023 09:30 |
Last Modified: | 06 Nov 2024 00:56 |
URI: | https://ueaeprints.uea.ac.uk/id/eprint/93013 |
DOI: | 10.1088/1742-6596/2462/1/012054 |
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