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Issue 11, 2016
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Vibrational spectroscopy reveals the initial steps of biological hydrogen evolution

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Abstract

[FeFe] hydrogenases are biocatalytic model systems for the exploitation and investigation of catalytic hydrogen evolution. Here, we used vibrational spectroscopic techniques to characterize, in detail, redox transformations of the [FeFe] and [4Fe4S] sub-sites of the catalytic centre (H-cluster) in a monomeric [FeFe] hydrogenase. Through the application of low-temperature resonance Raman spectroscopy, we discovered a novel metastable intermediate that is characterized by an oxidized [FeIFeII] centre and a reduced [4Fe4S]1+ cluster. Based on this unusual configuration, this species is assigned to the first, deprotonated H-cluster intermediate of the [FeFe] hydrogenase catalytic cycle. Providing insights into the sequence of initial reaction steps, the identification of this species represents a key finding towards the mechanistic understanding of biological hydrogen evolution.

Graphical abstract: Vibrational spectroscopy reveals the initial steps of biological hydrogen evolution

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Publication details

The article was received on 09 Mar 2016, accepted on 29 Jun 2016 and first published on 11 Jul 2016


Article type: Edge Article
DOI: 10.1039/C6SC01098A
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Chem. Sci., 2016,7, 6746-6752
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    Vibrational spectroscopy reveals the initial steps of biological hydrogen evolution

    S. Katz, J. Noth, M. Horch, H. S. Shafaat, T. Happe, P. Hildebrandt and I. Zebger, Chem. Sci., 2016, 7, 6746
    DOI: 10.1039/C6SC01098A

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