Structural and spectroscopic characterization of a HdrA-like subunit from Hyphomicrobium denitrificans

Bibliographic Details
Main Author: Ernst, Corvin
Publication Date: 2021
Other Authors: Kayastha, Kanwal, Koch, Tobias, Venceslau, Sofia S., Pereira, Inês A.C., Demmer, Ulrike, Ermler, Ulrich, Dahl, Christiane
Format: Article
Language: eng
Source: Repositórios Científicos de Acesso Aberto de Portugal (RCAAP)
Download full: http://hdl.handle.net/10362/120787
Summary: Funding Information: We thank Laurenz Heidrich for help with statistical analyses. This work was supported by grant Da 351/8‐1 (to CD) from the Deutsche Forschungsgemeinschaft and Fundação para a Ciência e Tecnologia (Portugal) (grant PTDC/BIA‐BQM/29118 and R&D units MOSTMICRO‐ITQB (UIDB/04612/2020 and UIDP/04612/2020), and European Union's Horizon 2020 research and innovation program (grant agreement No 810856). Open access funding enabled and organized by Projekt DEAL. Publisher Copyright: © 2020 The Authors. The FEBS Journal published by John Wiley & Sons Ltd on behalf of Federation of European Biochemical Societies Copyright: Copyright 2021 Elsevier B.V., All rights reserved.
id RCAP_a6b00b59cdefedf171c95b6149fcf7a0
oai_identifier_str oai:run.unl.pt:10362/120787
network_acronym_str RCAP
network_name_str Repositórios Científicos de Acesso Aberto de Portugal (RCAAP)
repository_id_str https://opendoar.ac.uk/repository/7160
spelling Structural and spectroscopic characterization of a HdrA-like subunit from Hyphomicrobium denitrificansdissimilatory sulfur oxidationelectron bifurcationheterodisulfide reductaseHyphomicrobium denitrificansBiochemistryMolecular BiologyCell BiologyFunding Information: We thank Laurenz Heidrich for help with statistical analyses. This work was supported by grant Da 351/8‐1 (to CD) from the Deutsche Forschungsgemeinschaft and Fundação para a Ciência e Tecnologia (Portugal) (grant PTDC/BIA‐BQM/29118 and R&D units MOSTMICRO‐ITQB (UIDB/04612/2020 and UIDP/04612/2020), and European Union's Horizon 2020 research and innovation program (grant agreement No 810856). Open access funding enabled and organized by Projekt DEAL. Publisher Copyright: © 2020 The Authors. The FEBS Journal published by John Wiley & Sons Ltd on behalf of Federation of European Biochemical Societies Copyright: Copyright 2021 Elsevier B.V., All rights reserved.Many bacteria and archaea employ a novel pathway of sulfur oxidation involving an enzyme complex that is related to the heterodisulfide reductase (Hdr or HdrABC) of methanogens. As a first step in the biochemical characterization of Hdr-like proteins from sulfur oxidizers (sHdr), we structurally analyzed the recombinant sHdrA protein from the Alphaproteobacterium Hyphomicrobium denitrificans at 1.4 Å resolution. The sHdrA core structure is similar to that of methanogenic HdrA (mHdrA) which binds the electron-bifurcating flavin adenine dinucleotide (FAD), the heart of the HdrABC-[NiFe]-hydrogenase catalyzed reaction. Each sHdrA homodimer carries two FADs and two [4Fe–4S] clusters being linked by electron conductivity. Redox titrations monitored by electron paramagnetic resonance and visible spectroscopy revealed a redox potential between −203 and −188 mV for the [4Fe–4S] center. The potentials for the FADH•/FADH− and FAD/FADH• pairs reside between −174 and −156 mV and between −81 and −19 mV, respectively. The resulting stable semiquinone FADH• species already detectable in the visible and electron paramagnetic resonance spectra of the as-isolated state of sHdrA is incompatible with basic principles of flavin-based electron bifurcation such that the sHdr complex does not apply this new mode of energy coupling. The inverted one-electron FAD redox potentials of sHdr and mHdr are clearly reflected in the different FAD-polypeptide interactions. According to this finding and the assumption that the sHdr complex forms an asymmetric HdrAA′B1C1B2C2 hexamer, we tentatively propose a mechanism that links protein-bound sulfane oxidation to sulfite on HdrB1 with NAD+ reduction via lipoamide disulfide reduction on HdrB2. The FAD of HdrA thereby serves as an electron storage unit. Database: Structural data are available in PDB database under the accession number 6TJR.Instituto de Tecnologia Química e Biológica António Xavier (ITQB)RUNErnst, CorvinKayastha, KanwalKoch, TobiasVenceslau, Sofia S.Pereira, Inês A.C.Demmer, UlrikeErmler, UlrichDahl, Christiane2021-07-09T22:17:55Z2021-032021-03-01T00:00:00Zinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/article15application/pdfhttp://hdl.handle.net/10362/120787eng1742-464XPURE: 32440692https://doi.org/10.1111/febs.15505info:eu-repo/semantics/openAccessreponame:Repositórios Científicos de Acesso Aberto de Portugal (RCAAP)instname:FCCN, serviços digitais da FCT – Fundação para a Ciência e a Tecnologiainstacron:RCAAP2024-05-22T17:54:32Zoai:run.unl.pt:10362/120787Portal AgregadorONGhttps://www.rcaap.pt/oai/openaireinfo@rcaap.ptopendoar:https://opendoar.ac.uk/repository/71602025-05-28T17:25:25.316604Repositórios Científicos de Acesso Aberto de Portugal (RCAAP) - FCCN, serviços digitais da FCT – Fundação para a Ciência e a Tecnologiafalse
dc.title.none.fl_str_mv Structural and spectroscopic characterization of a HdrA-like subunit from Hyphomicrobium denitrificans
title Structural and spectroscopic characterization of a HdrA-like subunit from Hyphomicrobium denitrificans
spellingShingle Structural and spectroscopic characterization of a HdrA-like subunit from Hyphomicrobium denitrificans
Ernst, Corvin
dissimilatory sulfur oxidation
electron bifurcation
heterodisulfide reductase
Hyphomicrobium denitrificans
Biochemistry
Molecular Biology
Cell Biology
title_short Structural and spectroscopic characterization of a HdrA-like subunit from Hyphomicrobium denitrificans
title_full Structural and spectroscopic characterization of a HdrA-like subunit from Hyphomicrobium denitrificans
title_fullStr Structural and spectroscopic characterization of a HdrA-like subunit from Hyphomicrobium denitrificans
title_full_unstemmed Structural and spectroscopic characterization of a HdrA-like subunit from Hyphomicrobium denitrificans
title_sort Structural and spectroscopic characterization of a HdrA-like subunit from Hyphomicrobium denitrificans
author Ernst, Corvin
author_facet Ernst, Corvin
Kayastha, Kanwal
Koch, Tobias
Venceslau, Sofia S.
Pereira, Inês A.C.
Demmer, Ulrike
Ermler, Ulrich
Dahl, Christiane
author_role author
author2 Kayastha, Kanwal
Koch, Tobias
Venceslau, Sofia S.
Pereira, Inês A.C.
Demmer, Ulrike
Ermler, Ulrich
Dahl, Christiane
author2_role author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Instituto de Tecnologia Química e Biológica António Xavier (ITQB)
RUN
dc.contributor.author.fl_str_mv Ernst, Corvin
Kayastha, Kanwal
Koch, Tobias
Venceslau, Sofia S.
Pereira, Inês A.C.
Demmer, Ulrike
Ermler, Ulrich
Dahl, Christiane
dc.subject.por.fl_str_mv dissimilatory sulfur oxidation
electron bifurcation
heterodisulfide reductase
Hyphomicrobium denitrificans
Biochemistry
Molecular Biology
Cell Biology
topic dissimilatory sulfur oxidation
electron bifurcation
heterodisulfide reductase
Hyphomicrobium denitrificans
Biochemistry
Molecular Biology
Cell Biology
description Funding Information: We thank Laurenz Heidrich for help with statistical analyses. This work was supported by grant Da 351/8‐1 (to CD) from the Deutsche Forschungsgemeinschaft and Fundação para a Ciência e Tecnologia (Portugal) (grant PTDC/BIA‐BQM/29118 and R&D units MOSTMICRO‐ITQB (UIDB/04612/2020 and UIDP/04612/2020), and European Union's Horizon 2020 research and innovation program (grant agreement No 810856). Open access funding enabled and organized by Projekt DEAL. Publisher Copyright: © 2020 The Authors. The FEBS Journal published by John Wiley & Sons Ltd on behalf of Federation of European Biochemical Societies Copyright: Copyright 2021 Elsevier B.V., All rights reserved.
publishDate 2021
dc.date.none.fl_str_mv 2021-07-09T22:17:55Z
2021-03
2021-03-01T00:00:00Z
dc.type.status.fl_str_mv info:eu-repo/semantics/publishedVersion
dc.type.driver.fl_str_mv info:eu-repo/semantics/article
format article
status_str publishedVersion
dc.identifier.uri.fl_str_mv http://hdl.handle.net/10362/120787
url http://hdl.handle.net/10362/120787
dc.language.iso.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv 1742-464X
PURE: 32440692
https://doi.org/10.1111/febs.15505
dc.rights.driver.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 15
application/pdf
dc.source.none.fl_str_mv reponame:Repositórios Científicos de Acesso Aberto de Portugal (RCAAP)
instname:FCCN, serviços digitais da FCT – Fundação para a Ciência e a Tecnologia
instacron:RCAAP
instname_str FCCN, serviços digitais da FCT – Fundação para a Ciência e a Tecnologia
instacron_str RCAAP
institution RCAAP
reponame_str Repositórios Científicos de Acesso Aberto de Portugal (RCAAP)
collection Repositórios Científicos de Acesso Aberto de Portugal (RCAAP)
repository.name.fl_str_mv Repositórios Científicos de Acesso Aberto de Portugal (RCAAP) - FCCN, serviços digitais da FCT – Fundação para a Ciência e a Tecnologia
repository.mail.fl_str_mv info@rcaap.pt
_version_ 1833596686085128192

Similar Items