期刊
ENERGY & ENVIRONMENTAL SCIENCE
卷 4, 期 7, 页码 2520-2524出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c1ee01408k
关键词
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资金
- JSPS/CNRS
- EU [212508]
- Ministry of Education, Science, Sports, Culture and Technology [21612007]
- Grants-in-Aid for Scientific Research [21612007] Funding Source: KAKEN
The role of Ca2+ in the Photosystem II water oxidation mechanism has been investigated in the higher redox states of the enzyme. The involvement of Ca2+ in structuring the environment of the tyrosine Y-Z in the S-3 state has been investigated by studying the effect of a Ca/Sr exchange by pulse-EPR spectroscopy. It is shown that Ca and Yz are involved in a common hydrogen bond network in S-3. The comparison of the temperature dependence of the rate of the water oxidation reaction shows that the slowdown of the S3YZ center dot -> S-0 transition in Sr-PSII mainly arises from a decrease of the entropic part of the Delta G(#) of the reaction. This suggests that Ca/Sr exchange perturbs the distribution of the conformational microstates and thereby hinders the overall water splitting process.
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