A Synthetic Model of the Mn3Ca Subsite of the Oxygen-Evolving Complex in Photosystem II
A Synthetic Model of the Mn3Ca Subsite of the Oxygen-Evolving Complex in Photosystem II
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DOI：
10.1126/science.1206036
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发表时间：
2011-08-05
期刊：
影响因子：
56.9
通讯作者：
Agapie, Theodor
中科院分区：
文献类型：
--
作者：
Kanady, Jacob S.;Tsui, Emily Y.;Agapie, Theodor
在光合生物体内，光系统II的进化氧复合体（OEC）利用催化的Mn4CaOn簇从水中生成双氧（n随中间体的机制和性质而变化）。我们在这里报道了一种[Mn3CaO4]（6+）立方烷的合理合成，它在结构上模拟了OEC的三锰-钙-立方烷亚位。Mn3CaO4和相关的Mn4O4立方烷的结构和电化学比较以及中间钙-锰多核配合物的表征揭示了钙在促进锰的高氧化态和生物簇组装中的潜在作用。
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.