In Vitro Assembly as a Tool to Investigate Catalytic Intermediates of [NiFe]-Hydrogenase
dc.contributor.author | Caserta, Giorgio | |
dc.contributor.author | Lorent, Christian | |
dc.contributor.author | Pelmenschikov, Vladimir | |
dc.contributor.author | Schoknecht, Janna | |
dc.contributor.author | Yoda, Yoshitaka | |
dc.contributor.author | Hildebrandt, Peter | |
dc.contributor.author | Cramer, Stephen P. | |
dc.contributor.author | Zebger, Ingo | |
dc.contributor.author | Lenz, Oliver | |
dc.date.accessioned | 2023-01-19T12:46:13Z | |
dc.date.available | 2023-01-19T12:46:13Z | |
dc.date.issued | 2020-11-16 | |
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.sponsorship | DFG, 390540038, EXC 2008: Unifying Systems in Catalysis "UniSysCat" | |
dc.description.sponsorship | EC/H2020/810856/EU/Twin to Illuminate Metals in Biology and Biocatalysis through Biospectroscopy/TIMB3 | |
dc.identifier.eissn | 2155-5435 | |
dc.identifier.uri | https://depositonce.tu-berlin.de/handle/11303/18014 | |
dc.identifier.uri | https://doi.org/10.14279/depositonce-16806 | |
dc.language.iso | en | |
dc.relation.ispartof | 10.14279/depositonce-16579 | |
dc.rights.uri | http://rightsstatements.org/vocab/InC/1.0/ | |
dc.subject.ddc | 541 Physikalische Chemie | de |
dc.subject.other | metalloenzyme | en |
dc.subject.other | hydrogenase | en |
dc.subject.other | hydrogen | en |
dc.subject.other | nickel | en |
dc.subject.other | iron | en |
dc.subject.other | catalytic cycle | en |
dc.subject.other | spectroscopy | en |
dc.title | In Vitro Assembly as a Tool to Investigate Catalytic Intermediates of [NiFe]-Hydrogenase | en |
dc.type | Article | |
dc.type.version | acceptedVersion | |
dcterms.bibliographicCitation.doi | 10.1021/acscatal.0c04079 | |
dcterms.bibliographicCitation.issue | 23 | |
dcterms.bibliographicCitation.journaltitle | ACS Catalysis | |
dcterms.bibliographicCitation.originalpublishername | American Chemical Society | |
dcterms.bibliographicCitation.originalpublisherplace | Washington, DC | |
dcterms.bibliographicCitation.pageend | 13894 | |
dcterms.bibliographicCitation.pagestart | 13890 | |
dcterms.bibliographicCitation.volume | 10 | |
dcterms.rightsHolder.note | This 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.reference | Verlagspolicy | |
dcterms.rightsHolder.url | https://web.archive.org/web/20220813002421/https://publish.acs.org/publish/author_guidelines?coden=jacsat | |
tub.accessrights.dnb | free | |
tub.affiliation | Fak. 2 Mathematik und Naturwissenschaften::Inst. Chemie::FG Physikalische Chemie / Biophysikalische Chemie | |
tub.publisher.universityorinstitution | Technische Universität Berlin |