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首页> 外文期刊>Coordination chemistry reviews >Reflections on small molecule manganese models that seek to mimic photosynthetic water oxidation chemistry
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Reflections on small molecule manganese models that seek to mimic photosynthetic water oxidation chemistry

机译：关于模仿光合水氧化化学的小分子锰模型的思考

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Recent advances in the study of the oxygen evolving complex (OEC) of photosystem II (PSII) include structural information attained from several X-ray crystallographic (XRD) and spectroscopic (XANES and EXAFS) investigations. The possible structural features gleaned from these studies have enabled synthetic chemists to design more accurate model complexes, which in turn, offer better insight into the possible pathways used by PSII to drive photosynthetic water oxidation catalysis. Mononuclear model compounds have been used to advance the knowledge base regarding the physical properties and reactivity of high-valent (Mn~(IV) or Mn~V) complexes. Such investigations have been especially important in regard to the manganyl (Mn~(IV)=O or Mn~V(O) species, as there are no reports, to date, of any structurally characterized multinuclear model compounds that incorporate such a functionality. Dinuclear and trinuclear model compounds have also been thoroughly studied in attempts to draw further comparison to the physical properties observed in the natural system and to design systems of catalytic relevance. As the reactive center of the OEC has been shown to contain an oxo-Mn_4Ca cluster, exact structural models necessitate a tetranuclear Mn core. The number of models that make use of Mn_4 clusters has risen substantially in recent years, and these models have provided evidence to support and refute certain mechanistic proposals. Further work is needed to adequately address the rationale for Ca (and Cl) in the OEC and to determine the sequence of events that lead to O_2 evolution.
机译：光系统II（PSII）的析氧复合物（OEC）研究的最新进展包括从X射线晶体学（XRD）和光谱学（XANES和EXAFS）研究获得的结构信息。从这些研究中收集到的可能的结构特征使合成化学家能够设计出更准确的模型配合物，从而为PSII用于驱动光合水氧化催化作用的可能途径提供了更好的见识。单核模型化合物已被用于提高有关高价（Mn〜（IV）或Mn〜V）配合物的物理性质和反应性的知识库。对于锰（Mn_（IV）= O或Mn〜V（O））物种而言，此类研究尤为重要，因为迄今为止，尚无关于结合这种功能的任何结构表征的多核模型化合物的报道。还已经对双核和三核模型化合物进行了深入研究，试图与天然系统中观察到的物理性质进行进一步比较，并设计具有催化相关性的系统，因为OEC的反应中心已显示出oxo-Mn_4Ca团簇精确的结构模型需要四核Mn核，近年来使用Mn_4团簇的模型数量大量增加，这些模型为支持和驳斥某些机械学建议提供了证据，还需要进一步的工作来充分说明其原理。确定OEC中的Ca（和Cl），并确定导致O_2演化的事件顺序。

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