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
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
收藏
页码:6439 / 6442
页数:4
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