Please use this identifier to cite or link to this item: http://dx.doi.org/10.14279/depositonce-6230
Main Title: Vibrational spectroscopy reveals the initial steps of biological hydrogen evolution
Author(s): Katz, Sagie
Noth, Jens
Horch, Marius
Shafaat, Hannah
Happe, Thomas
Hildebrandt, Peter
Zebger, Ingo
Type: Article
Language Code: en
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 [(FeFeII)-Fe-I] 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.
URI: https://depositonce.tu-berlin.de//handle/11303/6891
http://dx.doi.org/10.14279/depositonce-6230
Issue Date: 2016
Date Available: 24-Oct-2017
DDC Class: 540 Chemie und zugeordnete Wissenschaften
Sponsor/Funder: EXC 314: Unifying Concepts in Catalysis
DFG, EXC 1069, RESOLV (Ruhr Explores Solvation) - Verständnis und Design lösungsmittelabhängiger Prozesse
EC/FP7/291728/EU/Development and Coordination of Synthetic Biology in the European Research Area/ERASYNBIO
Creative Commons License: https://creativecommons.org/licenses/by/3.0/
Journal Title: Chemical Science
Publisher: Royal Society of Chemistry
Publisher Place: Cambridge
Volume: 7
Issue: 11
Publisher DOI: 10.1039/c6sc01098a
Page Start: 6746
Page End: 6752
EISSN: 2041-6539
ISSN: 2041-6520
Appears in Collections:Fachgebiet Physikalische Chemie / Biophysikalische Chemie » Publications

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