期刊
INORGANIC CHEMISTRY
卷 52, 期 10, 页码 5642-5644出版社
AMER CHEMICAL SOC
DOI: 10.1021/ic4005938
关键词
-
资金
- NIH [GM 55302]
- DOE, Office of Science, Office of Basic Energy Sciences (OBES), Chemical Sciences, Geosciences, and Biosciences Division [DE-AC02-05CH11231]
The oxygen-evolving complex (OEC) in photosystem II (PS II) was studied in the S-0 through S-3 states using 1s2p resonant inelastic X-ray scattering spectroscopy. The spectral changes of the OEC during the S-state transitions are subtle, indicating that the electrons are strongly delocalized throughout the cluster. The result suggests that, in addition to the Mn ions, ligands are also playing an important role in the redox reactions. A series of Mn-IV coordination complexes were compared, particularly with the PS II S-3 state spectrum to understand its oxidation state. We find strong variations of the electronic structure within the series of Mn-IV model systems. The spectrum of the S-3 state best resembles those of the Mn-IV complexes (Mn3Ca2)-Ca-IV and saplnMn(2)(IV)(OH)(2). The current result emphasizes that the assignment of formal oxidation states alone is not sufficient for understanding the detailed electronic structural changes that govern the catalytic reaction in the OEC.
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