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  Closing Kok’s cycle of nature’s water oxidation catalysis

Guo, Y., He, L., Ding, Y., Kloo, L., Pantazis, D. A., Messinger, J., et al. (2024). Closing Kok’s cycle of nature’s water oxidation catalysis. Nature Communications, 15: 5982. doi:10.1038/s41467-024-50210-6.

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 Creators:
Guo, Yu1, 2, Author
He, Lanlan1, 2, Author
Ding, Yunxuan1, 2, Author
Kloo, Lars3, Author
Pantazis, Dimitrios A.4, Author           
Messinger, Johannes5, 6, Author
Sun, Licheng1, 2, 7, Author
Affiliations:
1Center of Artificial Photosynthesis for Solar Fuels and Department of Chemistry, School of Science, Westlake University, Hangzhou, 310024, China, ou_persistent22              
2Institute of Natural Sciences, Westlake Institute for Advanced Study, Hangzhou, 310024, China, ou_persistent22              
3Department of Chemistry, School of Engineering Sciences in Chemistry, Biotechnology and Health, KTH Royal Institute of Technology, SE-10044, Stockholm, Sweden, ou_persistent22              
4Research Group Pantazis, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541711              
5Department of Plant Physiology, Umeå University, Linnaeus väg 6 (KBC huset), SE-90187, Umeå, Sweden, ou_persistent22              
6Molecular Biomimetics, Department of Chemistry – Ångström Laboratory, Uppsala University, SE-75120, Uppsala, Sweden, ou_persistent22              
7Division of Solar Energy Conversion and Catalysis at Westlake University, Zhejiang Baima Lake Laboratory Co., Ltd., Hangzhou, 310000, Zhejiang, China, ou_persistent22              

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 Abstract: The Mn4CaO5(6) cluster in photosystem II catalyzes water splitting through the Si state cycle (i = 0–4). Molecular O2 is formed and the natural catalyst is reset during the final S3 → (S4) → S0 transition. Only recently experimental breakthroughs have emerged for this transition but without explicit information on the S0-state reconstitution, thus the progression after O2 release remains elusive. In this report, our molecular dynamics simulations combined with density functional calculations suggest a likely missing link for closing the cycle, i.e., restoring the first catalytic state. Specifically, the formation of closed-cubane intermediates with all hexa-coordinate Mn is observed, which would undergo proton release, water dissociation, and ligand transfer to produce the open-cubane structure of the S0 state. Thereby, we theoretically identify the previously unknown structural isomerism in the S0 state that acts as the origin of the proposed structural flexibility prevailing in the cycle, which may be functionally important for nature’s water oxidation catalysis.

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Language(s): eng - English
 Dates: 2023-08-302024-07-162024-07-16
 Publication Status: Issued
 Pages: 11
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1038/s41467-024-50210-6
 Degree: -

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Title: Nature Communications
  Abbreviation : Nat. Commun.
Source Genre: Journal
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Publ. Info: London : Nature Publishing Group
Pages: - Volume / Issue: 15 Sequence Number: 5982 Start / End Page: - Identifier: ISSN: 2041-1723
CoNE: https://pure.mpg.de/cone/journals/resource/2041-1723