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2022-02-08Zeitschriftenartikel DOI: 10.18452/26149
A Morphing [4Fe-3S-nO]-Cluster within a Carbon Monoxide Dehydrogenase Scaffold
dc.contributor.authorJeoung, Jae-Hun
dc.contributor.authorFesseler, Jochen
dc.contributor.authorDomnik, Lilith
dc.contributor.authorKlemke, Friederike
dc.contributor.authorSinnreich, Malte
dc.contributor.authorTeutloff, Christian
dc.contributor.authorDobbek, Holger
dc.date.accessioned2023-02-28T13:11:55Z
dc.date.available2023-02-28T13:11:55Z
dc.date.issued2022-02-08none
dc.identifier.urihttp://edoc.hu-berlin.de/18452/26813
dc.description.abstractNi,Fe-containing carbon monoxide dehydrogenases (CODHs) catalyze the reversible reduction of CO2 to CO. Several anaerobic microorganisms encode multiple CODHs in their genome, of which some, despite being annotated as CODHs, lack a cysteine of the canonical binding motif for the active site Ni,Fe-cluster. Here, we report on the structure and reactivity of such a deviant enzyme, termed CooS-VCh. Its structure reveals the typical CODH scaffold, but contains an iron-sulfur-oxo hybrid-cluster. Although closely related to true CODHs, CooS-VCh catalyzes neither CO oxidation, nor CO2 reduction. The active site of CooS-VCh undergoes a redox-dependent restructuring between a reduced [4Fe-3S]-cluster and an oxidized [4Fe-2S-S*-2O-2(H2O)]-cluster. Hydroxylamine, a slow-turnover substrate of CooS-VCh, oxidizes the hybrid-cluster in two structurally distinct steps. Overall, minor changes in CODHs are sufficient to accommodate a Fe/S/O-cluster in place of the Ni,Fe-heterocubane-cluster of CODHs.eng
dc.language.isoengnone
dc.publisherHumboldt-Universität zu Berlin
dc.rights(CC BY 4.0) Attribution 4.0 Internationalger
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/
dc.subjectCODH Evolutioneng
dc.subjectEnzymeseng
dc.subjectHydroxylamineeng
dc.subjectReductioneng
dc.subjectIron-Sulfur-Oxo Clustereng
dc.subjectStructural Biologyeng
dc.subject.ddc540 Chemie und zugeordnete Wissenschaftennone
dc.subject.ddc660 Chemische Verfahrenstechnik und verwandte Technologiennone
dc.titleA Morphing [4Fe-3S-nO]-Cluster within a Carbon Monoxide Dehydrogenase Scaffoldnone
dc.typearticle
dc.identifier.urnurn:nbn:de:kobv:11-110-18452/26813-1
dc.identifier.doihttp://dx.doi.org/10.18452/26149
dc.type.versionpublishedVersionnone
local.edoc.pages8none
local.edoc.type-nameZeitschriftenartikel
local.edoc.container-typeperiodical
local.edoc.container-type-nameZeitschrift
dc.description.versionPeer Reviewednone
dc.identifier.eissn1521-3773
dcterms.bibliographicCitation.doi10.1002/anie.202117000
dcterms.bibliographicCitation.journaltitleAngewandte Chemienone
dcterms.bibliographicCitation.volume61none
dcterms.bibliographicCitation.issue18none
dcterms.bibliographicCitation.articlenumbere202117000none
dcterms.bibliographicCitation.originalpublishernameWiley-VCHnone
dcterms.bibliographicCitation.originalpublisherplaceWeinheimnone
bua.departmentMathematisch-Naturwissenschaftliche Fakultätnone

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