Abstract
Photosynthetic water oxidation is catalyzed by the Mn4CaO5 cluster of photosystem II (PSII) with linear progression through five S-state intermediates (S0 to S4). To reveal the mechanism of water oxidation, we analyzed structures of PSII in the S1, S2, and S3 states by x-ray free-electron laser serial crystallography. No insertion of water was found in S2, but flipping of D1 Glu189 upon transition to S3 leads to the opening of a water channel and provides a space for incorporation of an additional oxygen ligand, resulting in an open cubane Mn4CaO6 cluster with an oxyl/oxo bridge. Structural changes of PSII between the different S states reve cooperative action of substrate water access, proton release, and dioxygen formation in photosynthetic water oxidation.
| Original language | English |
|---|---|
| Pages (from-to) | 334-338 |
| Number of pages | 5 |
| Journal | Science |
| Volume | 366 |
| Issue number | 6463 |
| DOIs | |
| Publication status | Published - Oct 18 2019 |
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ASJC Scopus subject areas
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Cite this
An oxyl/oxo mechanism for oxygen-oxygen coupling in PSII revealed by an x-ray free-electron laser. / Suga, Michihiro; Akita, Fusamichi; Yamashita, Keitaro; Nakajima, Yoshiki; Ueno, Go; Li, Hongjie; Yamane, Takahiro; Hirata, Kunio; Umena, Yasufumi; Yonekura, Shinichiro; Yu, Long Jiang; Murakami, Hironori; Nomura, Takashi; Kimura, Tetsunari; Kubo, Minoru; Baba, Seiki; Kumasaka, Takashi; Tono, Kensuke; Yabashi, Makina; Isobe, Hiroshi; Yamaguchi, Kizashi; Yamamoto, Masaki; Ago, Hideo; Shen, Jian Ren.
In: Science, Vol. 366, No. 6463, 18.10.2019, p. 334-338.Research output: Contribution to journal › Article
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TY - JOUR
T1 - An oxyl/oxo mechanism for oxygen-oxygen coupling in PSII revealed by an x-ray free-electron laser
AU - Suga, Michihiro
AU - Akita, Fusamichi
AU - Yamashita, Keitaro
AU - Nakajima, Yoshiki
AU - Ueno, Go
AU - Li, Hongjie
AU - Yamane, Takahiro
AU - Hirata, Kunio
AU - Umena, Yasufumi
AU - Yonekura, Shinichiro
AU - Yu, Long Jiang
AU - Murakami, Hironori
AU - Nomura, Takashi
AU - Kimura, Tetsunari
AU - Kubo, Minoru
AU - Baba, Seiki
AU - Kumasaka, Takashi
AU - Tono, Kensuke
AU - Yabashi, Makina
AU - Isobe, Hiroshi
AU - Yamaguchi, Kizashi
AU - Yamamoto, Masaki
AU - Ago, Hideo
AU - Shen, Jian Ren
PY - 2019/10/18
Y1 - 2019/10/18
N2 - Photosynthetic water oxidation is catalyzed by the Mn4CaO5 cluster of photosystem II (PSII) with linear progression through five S-state intermediates (S0 to S4). To reveal the mechanism of water oxidation, we analyzed structures of PSII in the S1, S2, and S3 states by x-ray free-electron laser serial crystallography. No insertion of water was found in S2, but flipping of D1 Glu189 upon transition to S3 leads to the opening of a water channel and provides a space for incorporation of an additional oxygen ligand, resulting in an open cubane Mn4CaO6 cluster with an oxyl/oxo bridge. Structural changes of PSII between the different S states reve cooperative action of substrate water access, proton release, and dioxygen formation in photosynthetic water oxidation.
AB - Photosynthetic water oxidation is catalyzed by the Mn4CaO5 cluster of photosystem II (PSII) with linear progression through five S-state intermediates (S0 to S4). To reveal the mechanism of water oxidation, we analyzed structures of PSII in the S1, S2, and S3 states by x-ray free-electron laser serial crystallography. No insertion of water was found in S2, but flipping of D1 Glu189 upon transition to S3 leads to the opening of a water channel and provides a space for incorporation of an additional oxygen ligand, resulting in an open cubane Mn4CaO6 cluster with an oxyl/oxo bridge. Structural changes of PSII between the different S states reve cooperative action of substrate water access, proton release, and dioxygen formation in photosynthetic water oxidation.
UR - http://www.scopus.com/inward/record.url?scp=85073603536&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85073603536&partnerID=8YFLogxK
U2 - 10.1126/science.aax6998
DO - 10.1126/science.aax6998
M3 - Article
C2 - 31624207
AN - SCOPUS:85073603536
VL - 366
SP - 334
EP - 338
JO - Science
JF - Science
SN - 0036-8075
IS - 6463
ER -