In Vitro Assembly as a Tool to Investigate Catalytic Intermediates of [NiFe]-Hydrogenase

dc.contributor.authorCaserta, Giorgio
dc.contributor.authorLorent, Christian
dc.contributor.authorPelmenschikov, Vladimir
dc.contributor.authorSchoknecht, Janna
dc.contributor.authorYoda, Yoshitaka
dc.contributor.authorHildebrandt, Peter
dc.contributor.authorCramer, Stephen P.
dc.contributor.authorZebger, Ingo
dc.contributor.authorLenz, Oliver
dc.date.accessioned2023-01-19T12:46:13Z
dc.date.available2023-01-19T12:46:13Z
dc.date.issued2020-11-16
dc.description.abstract[NiFe]-hydrogenases catalyze the reversible reaction H2 ⇄ 2H+ + 2e–. Their basic module consists of a large subunit, coordinating the NiFe(CO)(CN)2 center, and a small subunit that carries electron-transferring iron–sulfur clusters. Here, we report the in vitro assembly of fully functional [NiFe]-hydrogenase starting from the isolated large and small subunits. Activity assays complemented by spectroscopic measurements revealed a native-like hydrogenase. This approach was used to label exclusively the NiFe(CO)(CN)2 center with 57Fe, enabling a clear view of the catalytic site by means of nuclear resonance vibrational spectroscopy. This strategy paves the way for in-depth studies of [NiFe]-hydrogenase catalytic intermediates.en
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.identifier.eissn2155-5435
dc.identifier.urihttps://depositonce.tu-berlin.de/handle/11303/18014
dc.identifier.urihttps://doi.org/10.14279/depositonce-16806
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.othermetalloenzymeen
dc.subject.otherhydrogenaseen
dc.subject.otherhydrogenen
dc.subject.othernickelen
dc.subject.otherironen
dc.subject.othercatalytic cycleen
dc.subject.otherspectroscopyen
dc.titleIn Vitro Assembly as a Tool to Investigate Catalytic Intermediates of [NiFe]-Hydrogenaseen
dc.typeArticle
dc.type.versionacceptedVersion
dcterms.bibliographicCitation.doi10.1021/acscatal.0c04079
dcterms.bibliographicCitation.issue23
dcterms.bibliographicCitation.journaltitleACS Catalysis
dcterms.bibliographicCitation.originalpublishernameAmerican Chemical Society
dcterms.bibliographicCitation.originalpublisherplaceWashington, DC
dcterms.bibliographicCitation.pageend13894
dcterms.bibliographicCitation.pagestart13890
dcterms.bibliographicCitation.volume10
dcterms.rightsHolder.noteThis document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, 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/acscatal.0c04079.
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

Files

Original bundle
Now showing 1 - 1 of 1
Loading…
Thumbnail Image
Name:
Caserta_etal_Vitro_2020.pdf
Size:
1.55 MB
Format:
Adobe Portable Document Format
License bundle
Now showing 1 - 1 of 1
No Thumbnail Available
Name:
license.txt
Size:
4.23 KB
Format:
Item-specific license agreed upon to submission
Description:

Collections