An oxyl/oxo mechanism for oxygen-oxygen coupling in PSII revealed by an x-ray free-electron laser | Zendy

Michihiro Suga | Zendy; Fusamichi Akita | Zendy; Keitaro Yamashita | Zendy; Yoshiki Nakajima | Zendy; Go Ueno | Zendy; Hongjie Li | Zendy; Takahiro Yamane | Zendy; Kunio Hirata | Zendy; Yasufumi Umena | Zendy; ShinIchiro Yonekura | Zendy; LongJiang Yu | Zendy; Hironori Murakami | Zendy; Takashi Nomura | Zendy; Tetsunari Kimura | Zendy; Minoru Kubo | Zendy; Seiki Baba | Zendy; Takashi Kumasaka | Zendy; Kensuke Tono | Zendy; Makina Yabashi | Zendy; Hiroshi Isobe | Zendy; K. Yamaguchi | Zendy; Masaki Yamamoto | Zendy; Hideo Ago | Zendy; JianRen Shen | Zendy

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An oxyl/oxo mechanism for oxygen-oxygen coupling in PSII revealed by an x-ray free-electron laser

Author(s) -

Michihiro Suga,

Fusamichi Akita,

Keitaro Yamashita,

Yoshiki Nakajima,

Go Ueno,

Hongjie Li,

Takahiro Yamane,

Kunio Hirata,

Yasufumi Umena,

ShinIchiro Yonekura,

LongJiang Yu,

Hironori Murakami,

Takashi Nomura,

Tetsunari Kimura,

Minoru Kubo,

Seiki Baba,

Takashi Kumasaka,

Kensuke Tono,

Makina Yabashi,

Hiroshi Isobe,

K. Yamaguchi,

Masaki Yamamoto,

Hideo Ago,

JianRen Shen

Publication year - 2019

Publication title -

science

Language(s) - English

Resource type - Journals

SCImago Journal Rank - 12.556

H-Index - 1186

eISSN - 1095-9203

pISSN - 0036-8075

DOI - 10.1126/science.aax6998

Subject(s) - oxygen evolving complex , photosystem ii , chemistry , oxygen evolution , photochemistry , photosynthesis , oxygen , cubane , electron transport chain , photodissociation , crystallography , ligand (biochemistry) , oxidation state , catalysis , crystal structure , electrochemistry , biochemistry , receptor , organic chemistry , electrode

Photosynthetic water oxidation is catalyzed by the Mn 4 CaO 5 cluster of photosystem II (PSII) with linear progression through five S-state intermediates (S 0 o S 4 ). To reveal the mechanism of water oxidation, we analyzed structures of PSII in the S 1 , S 2 , and S 3 states by x-ray free-electron laser serial crystallography. No insertion of water was found in S 2 , but flipping of D1 Glu 189 upon transition to S 3 leads to the opening of a water channel and provides a space for incorporation of an additional oxygen ligand, resulting in an open cubane Mn 4 CaO 6 cluster with an oxyl/oxo bridge. Structural changes of PSII between the different S states reveal cooperative action of substrate water access, proton release, and dioxygen formation in photosynthetic water oxidation.

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