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.
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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 -