Reorganization of Substrate Waters between the Closed and Open Cubane Conformers during the S2 to S3 Transition in the Oxygen Evolving Complex

被引：66

作者：

Capone, Matteo ^{[1
]}

Bovi, Daniele ^{[2
]}

Narzi, Daniele ^{[2
]}

Guidoni, Leonardo ^{[2
]}

机构：

[1] Univ Roma La Sapienza, Dipartimento Chim, I-00185 Rome, Italy

[2] Univ Aquila, Dipartimento Sci Fis & Chim, I-67100 Laquila, Italy

来源：

BIOCHEMISTRY | 2015年 / 54卷 / 42期

基金：

欧洲研究理事会;

关键词：

O BOND FORMATION; PHOTOSYSTEM-II; MANGANESE COMPLEX; RESOLUTION; OXIDATION; EXCHANGE; BINDING; CONVERSION; STATE; MECHANISM;

D O I：

10.1021/acs.biochem.5b00782

中图分类号：

Q5 [生物化学]; Q7 [分子生物学];

学科分类号：

071010 ; 081704 ;

摘要：

A crucial step in the mechanism for oxygen evolution in the Photosystem II complex resides in the transition from the S-2 state to the S-3 state of Kok-Joliot's cycle, in which an additional water molecule binds to the cluster. On the basis of computational chemistry calculations on Photosystem II models, we propose a reorganization mechanism involving a hydroxyl (W2) and a mu(2)-oxo bridge (O5) that is able to link the closed cubane S-2(B) intermediate conformer to the S-3 open cubane structure. This mechanism can reconcile the apparent conflict between recently reported water exchange and electron paramagnetic resonance experiments, and theoretical studies.

引用

页码：6439 / 6442

页数：4

共 44 条

[1] NH3 Binding to the S2 State of the O2-Evolving Complex of Photosystem II: Analogue to H2O Binding during the S2→S3 Transition
Askerka, Mikhail
Vinyard, David J.
Brudvig, Gary W.
Batista, Victor S.
[J]. BIOCHEMISTRY, 2015, 54 (38) : 5783 - 5786
[2] Analysis of the Radiation-Damage-Free X-ray Structure of Photosystem II in Light of EXAFS and QM/MM Data
Askerka, Mikhail
Vinyard, David J.
Wang, Jimin
Brudvig, Gary W.
Batista, Victor S.
[J]. BIOCHEMISTRY, 2015, 54 (09) : 1713 - 1716
[3] Photosynthetic energy conversion: natural and artificial
Barber, James
[J]. CHEMICAL SOCIETY REVIEWS, 2009, 38 (01) : 185 - 196
[4] Electrochemical water splitting by layered and 3D cross-linked manganese oxides: correlating structural motifs and catalytic activity
Bergmann, Arno
Zaharieva, Ivelina
Dau, Holger
Strasser, Peter
[J]. ENERGY & ENVIRONMENTAL SCIENCE, 2013, 6 (09) : 2745 - 2755
[5] Conversion of the spin state of the manganese complex in photosystem II induced by near-infrared light
Boussac, A
Girerd, JJ
Rutherford, AW
[J]. BIOCHEMISTRY, 1996, 35 (22) : 6984 - 6989
[6] Electron transfer pathways from the S2-states to the S3-states either after a Ca2+/Sr2+ or a Cl-/I- exchange in Photosystem II from
Boussac, Alain
Rutherford, A. William
Sugiura, Miwa
[J]. BIOCHIMICA ET BIOPHYSICA ACTA-BIOENERGETICS, 2015, 1847 (6-7): : 576 - 586
[7] Magnetic interactions in the catalyst used by nature to split water: a DFT plus U multiscale study on the Mn4CaO5 core in photosystem II
Bovi, Daniele
Narzi, Daniele
Guidoni, Leonardo
[J]. NEW JOURNAL OF PHYSICS, 2014, 16
[8] The S2 State of the Oxygen-Evolving Complex of Photosystem II Explored by QM/MM Dynamics: Spin Surfaces and Metastable States Suggest a Reaction Path Towards the S3 State
Bovi, Daniele
Narzi, Daniele
Guidoni, Leonardo
[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2013, 52 (45) : 11744 - 11749
[9] Conversion of the g=4.1 EPR signal to the multiline conformation during the S2 to S3 transition of the oxygen evolving complex of Photosystem II
Chrysina, Maria
Zahariou, Georgia
Ioannidis, Nikolaos
Petrouleas, Vasili
[J]. BIOCHIMICA ET BIOPHYSICA ACTA-BIOENERGETICS, 2010, 1797 (04): : 487 - 493
[10] Electronic structure of the oxygenevolving complex in photosystem II prior to O-O bond formation
Cox, Nicholas
Retegan, Marius
Neese, Frank
Pantazis, Dimitrios A.
Boussac, Alain
Lubitz, Wolfgang
[J]. SCIENCE, 2014, 345 (6198) : 804 - 808

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