Shedding Light on Proton and Electron Dynamics in [FeFe] Hydrogenases

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dc.contributor.authorLorent, Christian
dc.contributor.authorKatz, Sagie
dc.contributor.authorDuan, Jifu
dc.contributor.authorKulka, Catharina Julia
dc.contributor.authorCaserta, Giorgio
dc.contributor.authorTeutloff, Christian
dc.contributor.authorYadav, Shanika
dc.contributor.authorApfel, Ulf-Peter
dc.contributor.authorWinkler, Martin
dc.contributor.authorHappe, Thomas
dc.contributor.authorHorch, Marius
dc.contributor.authorZebger, Ingo
dc.date.accessioned2023-01-19T12:30:47Z
dc.date.available2023-01-19T12:30:47Z
dc.date.issued2020-03-03
dc.description.abstract[FeFe] hydrogenases are highly efficient catalysts for reversible dihydrogen evolution. H2 turnover involves different catalytic intermediates including a recently characterized hydride state of the active site (H-cluster). Applying cryogenic infrared and electron paramagnetic resonance spectroscopy to an [FeFe] model hydrogenase from Chlamydomonas reinhardtii (CrHydA1), we have discovered two new hydride intermediates and spectroscopic evidence for a bridging CO ligand in two reduced H-cluster states. Our study provides novel insights into these key intermediates, their relevance for the catalytic cycle of [FeFe] hydrogenase, and novel strategies for exploring these aspects in detail.en
dc.description.sponsorshipDFG, 273919336, SPP 1927: Iron-Sulfur for Life
dc.description.sponsorshipDFG, 390540038, EXC 2008: Unifying Systems in Catalysis "UniSysCat"
dc.description.sponsorshipEC/H2020/810856/EU/Twin to Illuminate Metals in Biology and Biocatalysis through Biospectroscopy/TIMB3
dc.description.sponsorshipDFG, 194650850, EXC 1069: RESOLV (Ruhr Explores Solvation) - Verständnis und Design lösungsmittelabhängiger Prozesse
dc.description.sponsorshipDFG, 321933041, GRK 2341: Mikrobielle Substratumsetzung
dc.description.sponsorshipDFG, 390677874, EXC 2033: RESOLV (Ruhr Explores Solvation)
dc.identifier.eissn1520-5126
dc.identifier.issn0002-7863
dc.identifier.urihttps://depositonce.tu-berlin.de/handle/11303/18013
dc.identifier.urihttps://doi.org/10.14279/depositonce-16805
dc.language.isoen
dc.relation.ispartof10.14279/depositonce-16579
dc.rights.urihttp://rightsstatements.org/vocab/InC/1.0/
dc.subject.ddc541 Physikalische Chemiede
dc.subject.otheranionsen
dc.subject.otherelectron paramagnetic resonance spectroscopyen
dc.subject.otherinfrared lighten
dc.subject.otherligandsen
dc.subject.otherreaction mechanismsen
dc.titleShedding Light on Proton and Electron Dynamics in [FeFe] Hydrogenasesen
dc.typeArticle
dc.type.versionacceptedVersion
dcterms.bibliographicCitation.doi10.1021/jacs.9b13075
dcterms.bibliographicCitation.issue12
dcterms.bibliographicCitation.journaltitleJournal of the American Chemical Society
dcterms.bibliographicCitation.originalpublishernameAmerican Chemical Society
dcterms.bibliographicCitation.originalpublisherplaceWashington, DC
dcterms.bibliographicCitation.pageend5497
dcterms.bibliographicCitation.pagestart5493
dcterms.bibliographicCitation.volume142
dcterms.rightsHolder.noteThis document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/jacs.9b13075.
dcterms.rightsHolder.referenceVerlagspolicy
dcterms.rightsHolder.urlhttps://web.archive.org/web/20220813002421/https://publish.acs.org/publish/author_guidelines?coden=jacsat
tub.accessrights.dnbfree
tub.affiliationFak. 2 Mathematik und Naturwissenschaften::Inst. Chemie::FG Physikalische Chemie / Biophysikalische Chemie
tub.publisher.universityorinstitutionTechnische Universität Berlin

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