A Synthetic Model of the Mn3Ca Subsite of the Oxygen-Evolving Complex in Photosystem II

被引:472
作者
Kanady, Jacob S. [1 ]
Tsui, Emily Y. [1 ]
Day, Michael W. [1 ]
Agapie, Theodor [1 ]
机构
[1] CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
关键词
WATER-OXIDIZING COMPLEX; CRYSTAL-STRUCTURE; MANGANESE COMPLEX; MN4CA CLUSTER; OXIDATION; RESOLUTION; CHEMISTRY; DIOXYGEN; COBALT; MN;
D O I
10.1126/science.1206036
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Within photosynthetic organisms, the oxygen-evolving complex (OEC) of photosystem II generates dioxygen from water using a catalytic Mn4CaOn cluster (n varies with the mechanism and nature of the intermediate). We report here the rational synthesis of a [Mn3CaO4](6+) cubane that structurally models the trimanganese-calcium-cubane subsite of the OEC. Structural and electrochemical comparison between Mn3CaO4 and a related Mn4O4 cubane alongside characterization of an intermediate calcium-manganese multinuclear complex reveals potential roles of calcium in facilitating high oxidation states at manganese and in the assembly of the biological cluster.
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页码:733 / 736
页数:4
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