Meyer Thomas J, Huynh My Hang V, Thorp H Holden
Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599, USA.
Angew Chem Int Ed Engl. 2007;46(28):5284-304. doi: 10.1002/anie.200600917.
All higher life forms use oxygen and respiration as their primary energy source. The oxygen comes from water by solar-energy conversion in photosynthetic membranes. In green plants, light absorption in photosystem II (PSII) drives electron-transfer activation of the oxygen-evolving complex (OEC). The mechanism of water oxidation by the OEC has long been a subject of great interest to biologists and chemists. With the availability of new molecular-level protein structures from X-ray crystallography and EXAFS, as well as the accumulated results from numerous experiments and theoretical studies, it is possible to suggest how water may be oxidized at the OEC. An integrated sequence of light-driven reactions that exploit coupled electron-proton transfer (EPT) could be the key to water oxidation. When these reactions are combined with long-range proton transfer (by sequential local proton transfers), it may be possible to view the OEC as an intricate structure that is "wired for protons".
所有高等生命形式都将氧气和呼吸作用作为其主要能量来源。氧气通过光合膜中的太阳能转化从水中获取。在绿色植物中，光系统II（PSII）中的光吸收驱动了析氧复合体（OEC）的电子转移活化。OEC氧化水的机制长期以来一直是生物学家和化学家极为感兴趣的课题。随着X射线晶体学和扩展X射线吸收精细结构（EXAFS）提供新的分子水平蛋白质结构，以及众多实验和理论研究积累的结果，现在有可能提出水在OEC处如何被氧化。利用耦合电子-质子转移（EPT）的一系列光驱动反应可能是水氧化的关键。当这些反应与长程质子转移（通过连续的局部质子转移）相结合时，有可能将OEC视为一个“为质子布线”的复杂结构。
