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- Cheah, Mun HonUppsala universitet,Molekylär biomimetik (author)
Assessment of the manganese cluster’s oxidation state via photoactivation of photosystem II microcrystals
- Article/chapterEnglish2020
Publisher, publication year, extent ...
- 2019-12-17
- Proceedings of the National Academy of Sciences,2020
- printrdacarrier
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- LIBRIS-ID:oai:DiVA.org:umu-167235
- https://urn.kb.se/resolve?urn=urn:nbn:se:umu:diva-167235URI
- https://doi.org/10.1073/pnas.1915879117DOI
- https://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-403248URI
Supplementary language notes
- Language:English
- Summary in:English
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Notes
- Knowledge of the manganese oxidation states of the oxygen-evolving Mn4CaO5 cluster in photosystem II (PSII) is crucial toward understanding the mechanism of biological water oxidation. There is a 4 decade long debate on this topic that historically originates from the observation of a multiline electron paramagnetic resonance (EPR) signal with effective total spin of S = 1/2 in the singly oxidized S2 state of this cluster. This signal implies an overall oxidation state of either Mn(III)3Mn(IV) or Mn(III)Mn(IV)3 for the S2 state. These 2 competing assignments are commonly known as “low oxidation (LO)” and “high oxidation (HO)” models of the Mn4CaO5 cluster. Recent advanced EPR and Mn K-edge X-ray spectroscopy studies converge upon the HO model. However, doubts about these assignments have been voiced, fueled especially by studies counting the number of flash-driven electron removals required for the assembly of an active Mn4CaO5 cluster starting from Mn(II) and Mn-free PSII. This process, known as photoactivation, appeared to support the LO model since the first oxygen is reported to evolve already after 7 flashes. In this study, we improved the quantum yield and sensitivity of the photoactivation experiment by employing PSII microcrystals that retained all protein subunits after complete manganese removal and by oxygen detection via a custom built thin-layer cell connected to a membrane inlet mass spectrometer. We demonstrate that 9 flashes by a nanosecond laser are required for the production of the first oxygen, which proves that the HO model provides the correct description of the Mn4CaO5 cluster’s oxidation states.
Subject headings and genre
- NATURVETENSKAP Kemi Fysikalisk kemi hsv//swe
- NATURAL SCIENCES Chemical Sciences Physical Chemistry hsv//eng
- NATURVETENSKAP Biologi Biofysik hsv//swe
- NATURAL SCIENCES Biological Sciences Biophysics hsv//eng
- photosynthesis
- oxygen evolving cluster
- photoassembly
- manganese oxidation state
- mechanism of water oxidation
- biologisk kemi
- biological chemistry
- Physical Chemistry
- fysikalisk kemi
Added entries (persons, corporate bodies, meetings, titles ...)
- Zhang, MiaoHumboldt Univ, Inst Biol, D-10115 Berlin, Germany (author)
- Shevela, Dmitriy,1979-Umeå universitet,Kemiska institutionen,Umea Univ, Chem Biol Ctr, Dept Chem, S-90187 Umea, Sweden(Swepub:umu)dmsh0004 (author)
- Mamedov, Fikret,Ph.D., Dr.Sci.Uppsala universitet,Molekylär biomimetik(Swepub:uu)fimam179 (author)
- Zouni, AthinaHumboldt Univ, Inst Biol, D-10115 Berlin, Germany (author)
- Messinger, JohannesUppsala universitet,Umeå universitet,Kemiska institutionen,Molecular Biomimetics, Department of Chemistry–Ångström Laboratory, Uppsala University, 75120 Uppsala, Sweden,Molekylär biomimetik,Umea Univ, Chem Biol Ctr, Dept Chem, S-90187 Umea, Sweden(Swepub:uu)johme269 (author)
- Uppsala universitetMolekylär biomimetik (creator_code:org_t)
Related titles
- In:Proceedings of the National Academy of Sciences of the United States of America: Proceedings of the National Academy of Sciences117:1, s. 141-1450027-84241091-6490
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