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Volume 185, 2015

Photosynthetic water oxidation: binding and activation of substrate waters for O–O bond formation

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Abstract

Photosynthetic water oxidation occurs at the oxygen-evolving complex (OEC) of Photosystem II (PSII). The OEC, which contains a Mn4CaO5 inorganic cluster ligated by oxides, waters and amino-acid residues, cycles through five redox intermediates known as Si states (i = 0–4). The electronic and structural properties of the transient S4 intermediate that forms the O–O bond are not well understood. In order to gain insight into how water is activated for O–O bond formation in the S4 intermediate, we have performed a detailed analysis of S-state dependent substrate water binding kinetics taking into consideration data from Mn coordination complexes. This analysis supports a model in which the substrate waters are both bound as terminal ligands and react via a water-nucleophile attack mechanism.

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Submitted
21 May 2015
Accepted
01 Jun 2015
First published
01 Jun 2015

This article is Open Access

Faraday Discuss., 2015,185, 37-50
Article type
Paper

Photosynthetic water oxidation: binding and activation of substrate waters for O–O bond formation

D. J. Vinyard, S. Khan and G. W. Brudvig, Faraday Discuss., 2015, 185, 37 DOI: 10.1039/C5FD00087D

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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