Vibrational spectroscopy reveals the initial steps of biological hydrogen evolution

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dc.contributor.authorKatz, Sagie
dc.contributor.authorNoth, Jens
dc.contributor.authorHorch, Marius
dc.contributor.authorShafaat, Hannah
dc.contributor.authorHappe, Thomas
dc.contributor.authorHildebrandt, Peter
dc.contributor.authorZebger, Ingo
dc.date.accessioned2017-10-24T07:15:07Z
dc.date.available2017-10-24T07:15:07Z
dc.date.issued2016
dc.description.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.en
dc.description.sponsorshipDFG, EXC 314, Unifying Concepts in Catalysisen
dc.description.sponsorshipDFG, EXC 1069, RESOLV (Ruhr Explores Solvation) - Verständnis und Design lösungsmittelabhängiger Prozesseen
dc.description.sponsorshipEC/FP7/291728/EU/Development and Coordination of Synthetic Biology in the European Research Area/ERASYNBIOen
dc.identifier.eissn2041-6539
dc.identifier.issn2041-6520
dc.identifier.pmid28451119
dc.identifier.urihttps://depositonce.tu-berlin.de/handle/11303/6891
dc.identifier.urihttp://dx.doi.org/10.14279/depositonce-6230
dc.language.isoen
dc.rights.urihttps://creativecommons.org/licenses/by/3.0/
dc.subject.ddc540 Chemie und zugeordnete Wissenschaftende
dc.titleVibrational spectroscopy reveals the initial steps of biological hydrogen evolutionen
dc.typeArticleen
dc.type.versionpublishedVersionen
dcterms.bibliographicCitation.doi10.1039/c6sc01098a
dcterms.bibliographicCitation.issue11
dcterms.bibliographicCitation.journaltitleChemical Scienceen
dcterms.bibliographicCitation.originalpublishernameRoyal Society of Chemistryde
dcterms.bibliographicCitation.originalpublisherplaceCambridgede
dcterms.bibliographicCitation.pageend6752
dcterms.bibliographicCitation.pagestart6746
dcterms.bibliographicCitation.volume7
tub.accessrights.dnbfree
tub.affiliationFak. 2 Mathematik und Naturwissenschaften::Inst. Chemie::FG Physikalische Chemie / Biophysikalische Chemiede
tub.affiliation.facultyFak. 2 Mathematik und Naturwissenschaftende
tub.affiliation.groupFG Physikalische Chemie / Biophysikalische Chemiede
tub.affiliation.instituteInst. Chemiede
tub.publisher.universityorinstitutionTechnische Universität Berlin

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