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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Stepwise assembly of heterobimetallic complexes: synthesis, structure, and physical properties
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Stepwise assembly of heterobimetallic complexes: synthesis, structure, and physical properties

机译：逐步组装异质物质复合物：合成，结构和物理性质

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Bimetallic active sites are ubiquitous in metalloenzymes and have sparked investigations of synthetic models to aid in the establishment of structure-function relationship. We previously reported a series of discrete bimetallic complexes with [Fe-III-(mu-OH)-M-II] cores in which the ligand framework provides distinct binding sites for two metal centers. The formation of these complexes relied on a stepwise synthetic approach in which an Fe-III-OH complex containing a sulfonamido tripodal ligand served as a synthon that promoted assembly. We have utilized this approach in the present study to produce a new series of bimetallic complexes with [Fe-III-(mu-OH)-M-II] cores (M = Ni, Cu, Zn) by using an ancillary ligand to the Fe-III center that contains phosphinic amido groups. Assembly began with formation of an Fe-III-OH that was subsequently used to bind the M-II fragment that contained a triazacyclononane ligand. The series of bimetallic complexes were charactered structurally by X-ray diffraction methods, spectroscopically by absorption, vibrational, electron paramagnetic resonance spectroscopies, and electrochemically by cyclic voltammetry. A notable finding is that these new [Fe-III-(mu-OH)-M-II] complexes displayed significantly lower reduction potentials than their sulfonamido counterparts, which paves way for future studies on high valent bimetallic complexes in this scaffold.
机译：双金属活性位点在金属酶中普遍存在，并引发了对合成模型的研究，以帮助建立结构-功能关系。我们之前报道了一系列具有[Fe III-（mu OH）-M-II]核的离散双金属配合物，其中配体框架为两个金属中心提供了不同的结合位点。这些配合物的形成依赖于逐步合成方法，其中含有磺胺基三脚架配体的Fe III OH配合物作为促进组装的合成子。在本研究中，我们利用这种方法，通过使用含有膦酰胺基的Fe III中心的辅助配体，制备了一系列具有[Fe III-（mu OH）-M-II]核（M=Ni，Cu，Zn）的新双金属配合物。组装始于形成Fe III OH，随后用于结合含有三氮杂环壬烷配体的M-II片段。用X射线衍射法、吸收光谱法、振动光谱法、电子顺磁共振光谱法和循环伏安法对该系列双金属配合物进行了结构表征。一个值得注意的发现是，这些新的[Fe III-（mu-OH）-M-II]络合物比它们的磺胺基络合物显示出显著更低的还原电位，这为将来研究这种支架中的高价双金属络合物铺平了道路。

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