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A Hydrophilic Channel Is Involved in Oxidative Inactivation of a [NiFeSe] Hydrogenase

2019-09-06Artigo científico Acesso aberto
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dc.contributor.authorZacarias, Sónia
dc.contributor.authorTemporão, Adriana
dc.contributor.authorBarrio, Melisa Del
dc.contributor.authorFourmond, Vincent
dc.contributor.authorLéger, Christophe
dc.contributor.authorMatias, Pedro M.
dc.contributor.authorPereira, Inês A.C.
dc.contributor.institutionInstituto de Tecnologia Química e Biológica António Xavier (ITQB)
dc.contributor.pblACS - American Chemical Society
dc.date.accessioned2020-01-22T23:39:06Z
dc.date.available2023-02-08T01:31:51Z
dc.date.embargoedUntil2023-01-22
dc.date.issued2019-09-06
dc.description.abstractHydrogenases are metalloenzymes that catalyze the redox conversion between H2 and protons. The so-called [NiFeSe] hydrogenases are highly active for both H2 production and oxidation, but like all hydrogenases, they are inhibited by O2. In the [NiFeSe] enzyme from Desulfovibrio vulgaris Hildenborough this inhibition results from the oxidation of an active site cysteine ligand. We designed mutations that constrict a hydrophilic channel which connects the protein surface to this active site cysteine. Two of the variants show markedly increased tolerance to O2 inactivation, while they retain high catalytic activities in both directions of the reaction, and structural studies confirm that these mutations prevent the oxidation of the cysteine. Our results indicate that the diffusion of O2 or ROS to the active site can occur through a hydrophilic water channel, in contrast to the widely held assumption that only hydrophobic channels are involved in active site inactivation. This provides an original strategy for optimizing the enzyme by protein engineering.en
dc.description.versionpublishersversion
dc.description.versionpublished
dc.format.extent11
dc.format.extent6907750
dc.identifier.doi10.1021/acscatal.9b02347
dc.identifier.issn2155-5435
dc.identifier.otherPURE: 16380660
dc.identifier.otherPURE UUID: 3e2ff496-c637-44dc-b2f6-7171ad5f3853
dc.identifier.otherScopus: 85071939114
dc.identifier.otherORCID: /0000-0001-6170-451X/work/68084840
dc.identifier.urihttp://hdl.handle.net/10362/91637
dc.identifier.urlhttps://www.scopus.com/pages/publications/85071939114
dc.language.isoeng
dc.peerreviewedyes
dc.subjecthydrogen
dc.subjecthydrogenases
dc.subjecthydrophilic channel
dc.subjectselenium
dc.subjectsulfenate
dc.subjectsulfinate
dc.subjectCatalysis
dc.subjectGeneral Chemistry
dc.titleA Hydrophilic Channel Is Involved in Oxidative Inactivation of a [NiFeSe] Hydrogenaseen
dc.typejournal article
degois.publication.firstPage8509
degois.publication.issue9
degois.publication.lastPage8519
degois.publication.titleACS Catalysis
degois.publication.volume9
dspace.entity.typePublication
rcaap.rightsopenAccess

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