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O2 evolution and recovery of the water-oxidizing enzyme

Author

Listed:
  • Keisuke Kawashima

    (The University of Tokyo, 7-3-1 Hongo)

  • Tomohiro Takaoka

    (The University of Tokyo, 7-3-1 Hongo)

  • Hiroki Kimura

    (The University of Tokyo, 7-3-1 Hongo)

  • Keisuke Saito

    (The University of Tokyo, 7-3-1 Hongo
    The University of Tokyo, 4-6-1 Komaba)

  • Hiroshi Ishikita

    (The University of Tokyo, 7-3-1 Hongo
    The University of Tokyo, 4-6-1 Komaba)

Abstract

In photosystem II, light-induced water oxidation occurs at the Mn4CaO5 cluster. Here we demonstrate proton releases, dioxygen formation, and substrate water incorporation in response to Mn4CaO5 oxidation in the protein environment, using a quantum mechanical/molecular mechanical approach and molecular dynamics simulations. In S2, H2O at the W1 site forms a low-barrier H-bond with D1-Asp61. In the S2-to-S3 transition, oxidation of OW1H– to OW1•–, concerted proton transfer from OW1H– to D1-Asp61, and binding of a water molecule Wn-W1 at OW1•– are observed. In S4, W n -W1 facilitates oxo-oxyl radical coupling between OW1•– and corner μ-oxo O4. Deprotonation via D1-Asp61 leads to formation of OW1=O4. As OW1=O4 moves away from Mn, H2O at W539 is incorporated into the vacant O4 site of the O2-evolved Mn4CaO4 cluster, forming a μ-oxo bridge (Mn3–OW539–Mn4) in an exergonic process. Simultaneously, Wn-W1 is incorporated as W1, recovering the Mn4CaO5 cluster.

Suggested Citation

  • Keisuke Kawashima & Tomohiro Takaoka & Hiroki Kimura & Keisuke Saito & Hiroshi Ishikita, 2018. "O2 evolution and recovery of the water-oxidizing enzyme," Nature Communications, Nature, vol. 9(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-03545-w
    DOI: 10.1038/s41467-018-03545-w
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    Cited by:

    1. Rana Hussein & Mohamed Ibrahim & Asmit Bhowmick & Philipp S. Simon & Ruchira Chatterjee & Louise Lassalle & Margaret Doyle & Isabel Bogacz & In-Sik Kim & Mun Hon Cheah & Sheraz Gul & Casper Lichtenber, 2021. "Structural dynamics in the water and proton channels of photosystem II during the S2 to S3 transition," Nature Communications, Nature, vol. 12(1), pages 1-16, December.
    2. Yu Guo & Lanlan He & Yunxuan Ding & Lars Kloo & Dimitrios A. Pantazis & Johannes Messinger & Licheng Sun, 2024. "Closing Kok’s cycle of nature’s water oxidation catalysis," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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