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

Joseph A. Wright, Atheer M. Madlool, Stephen P. Cottrell

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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.
Original languageEnglish
Article number012054
JournalJournal of Physics: Conference Series
Volume2462
Early online date31 Mar 2023
DOIs
Publication statusPublished - 2023

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