Journal
FARADAY DISCUSSIONS
Volume 185, Issue -, Pages 37-50Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c5fd00087d
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Funding
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-FG02-05ER15646]
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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 S-4 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 S-4 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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