Umeå universitets logga

umu.sePublikationer
Ändra sökning
RefereraExporteraLänk till posten
Permanent länk

Direktlänk
Referera
Referensformat
  • apa
  • ieee
  • vancouver
  • Annat format
Fler format
Språk
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Annat språk
Fler språk
Utmatningsformat
  • html
  • text
  • asciidoc
  • rtf
The exchange of the fast substrate water in the S2 state of photosystem II is limited by diffusion of bulk water through channels - implications for the water oxidation mechanism
Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Molecular Biomimetics, Department of Chemistry-Ångström Laboratory, Uppsala University, Uppsala, Sweden.ORCID-id: 0000-0003-2975-8395
Department of Biochemistry, University of California, CA, Riverside, United States.
Molecular Biomimetics, Department of Chemistry-Ångström Laboratory, Uppsala University, Uppsala, Sweden.
Department of Biochemistry, University of California, CA, Riverside, United States.
Visa övriga samt affilieringar
2021 (Engelska)Ingår i: Chemical Science, ISSN 2041-6520, E-ISSN 2041-6539, Vol. 12, nr 38, s. 12763-12775Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

The molecular oxygen we breathe is produced from water-derived oxygen species bound to the Mn4CaO5 cluster in photosystem II (PSII). Present research points to the central oxo-bridge O5 as the 'slow exchanging substrate water (Ws)', while, in the S2 state, the terminal water ligands W2 and W3 are both discussed as the 'fast exchanging substrate water (Wf)'. A critical point for the assignment of Wf is whether or not its exchange with bulk water is limited by barriers in the channels leading to the Mn4CaO5 cluster. In this study, we measured the rates of H2 16O/H2 18O substrate water exchange in the S2 and S3 states of PSII core complexes from wild-type (WT) Synechocystis sp. PCC 6803, and from two mutants, D1-D61A and D1-E189Q, that are expected to alter water access via the Cl1/O4 channels and the O1 channel, respectively. We found that the exchange rates of Wf and Ws were unaffected by the E189Q mutation (O1 channel), but strongly perturbed by the D61A mutation (Cl1/O4 channel). It is concluded that all channels have restrictions limiting the isotopic equilibration of the inner water pool near the Mn4CaO5 cluster, and that D61 participates in one such barrier. In the D61A mutant this barrier is lowered so that Wf exchange occurs more rapidly. This finding removes the main argument against Ca-bound W3 as fast substrate water in the S2 state, namely the indifference of the rate of Wf exchange towards Ca/Sr substitution.

Ort, förlag, år, upplaga, sidor
Royal Society of Chemistry, 2021. Vol. 12, nr 38, s. 12763-12775
Nationell ämneskategori
Biokemi Molekylärbiologi
Forskningsämne
biokemi
Identifikatorer
URN: urn:nbn:se:umu:diva-188865DOI: 10.1039/d1sc02265bISI: 000692833600001PubMedID: 34703563Scopus ID: 2-s2.0-85117138951OAI: oai:DiVA.org:umu-188865DiVA, id: diva2:1607793
Forskningsfinansiär
Vetenskapsrådet, 2016-05183Vetenskapsrådet, 2020-03809Tillgänglig från: 2021-11-02 Skapad: 2021-11-02 Senast uppdaterad: 2025-02-20Bibliografiskt granskad

Open Access i DiVA

fulltext(2203 kB)134 nedladdningar
Filinformation
Filnamn FULLTEXT01.pdfFilstorlek 2203 kBChecksumma SHA-512
58591a052425c5fa373c8e938d06956ac9d8db9ffe4664f637d7175fdf9115149bcc952af9294981621fa69ad03b272b60c47b7089b7bfb17cb8b08fcea490e8
Typ fulltextMimetyp application/pdf

Övriga länkar

Förlagets fulltextPubMedScopus

Person

de Lichtenberg, CasperMessinger, Johannes

Sök vidare i DiVA

Av författaren/redaktören
de Lichtenberg, CasperMessinger, Johannes
Av organisationen
Kemiska institutionen
I samma tidskrift
Chemical Science
BiokemiMolekylärbiologi

Sök vidare utanför DiVA

GoogleGoogle Scholar
Totalt: 134 nedladdningar
Antalet nedladdningar är summan av nedladdningar för alla fulltexter. Det kan inkludera t.ex tidigare versioner som nu inte längre är tillgängliga.

doi
pubmed
urn-nbn

Altmetricpoäng

doi
pubmed
urn-nbn
Totalt: 350 träffar
RefereraExporteraLänk till posten
Permanent länk

Direktlänk
Referera
Referensformat
  • apa
  • ieee
  • vancouver
  • Annat format
Fler format
Språk
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Annat språk
Fler språk
Utmatningsformat
  • html
  • text
  • asciidoc
  • rtf