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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Double-level 'orthogonal' dynamic combinatorial libraries on transition metal template
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Double-level 'orthogonal' dynamic combinatorial libraries on transition metal template

机译：过渡金属模板上的双层“正交”动态组合库

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摘要

Dynamic combinatorial libraries are mixtures of compounds that exist in a dynamic equilibrium and can be driven to compositional self adaptation via selective binding of a specific assembly of certain components to a molecular target. We present here an extension of this initial concept to dynamic librarise that consists of two levels,the first formed by the coordination of terpyridine-based ligands to the transition metal template, and the second, by the imine formation with the aldehyde substituents on the terpyridine moieties. Dialde- hyde 7 has been synthesized, converted into a variety of ligands, oxime ethers L_11-L_33 and acyl hydrazones L_44-L_77, and subsequently into corresponding cobalt complexes. A typical complex,Co(L_22)~2+_2 is shown to engage in rapid exchange with a competing ligand L_11 and with another complex, Co(L_22)~2+_2 in 30/100 acetonitrile/water at PH 7.0 and 25℃. The exchange in the corresponding Co(Ⅲ) complexes is shown to be much slower. Imine exchange in the acyl hydrazone complexes (L_44-L_77) is strongly controlled by PH and temperature. The two types of exchange, ligand and imine, can thus be used as independent equilibrium process controlled by different types of external intervention, i.e., via oxidation/reduction of the metal tem- plate and/or change in the PH/temperature of the medium. The resulting double-level dynamic libraries are therefore named orthog- onal, in similarity with the orthogonal protecting groups in organic synthesis. Sample libraries of this type have been synthesized and showed the complete expected set of components in electrospray ionization MS.
机译：动态组合库是存在于动态平衡中的化合物的混合物，可以通过将某些组分的特定组件选择性结合到分子靶标上来驱动组分的自我适应。在这里，我们提出了从初始概念到动态自由度的扩展，它包括两个层次，第一个层次是基于三联吡啶的配体与过渡金属模板的配位，第二个层次是通过在亚吡啶上带有醛取代基的亚胺形成部分。已经合成了二醛7，将其转化为各种配体，肟醚L_11-L_33和酰基L_44-L_77，随后转化为相应的钴配合物。典型的配合物Co（L_22）〜2 + _2与竞争性配体L_11以及另一种配合物Co（L_22）〜2 + _2在30/100乙腈/水中在pH 7.0和25℃时快速交换。 。相应的Co（Ⅲ）配合物中的交换被证明要慢得多。酰基配合物（L_44-L_77）中的亚胺交换受PH和温度的强烈控制。因此，两种交换类型（配体和亚胺）可以用作独立的平衡过程，可以通过不同类型的外部干预（例如，通过金属模板的氧化/还原和/或介质的PH /温度变化）来控制。因此，与有机合成中的正交保护基团相似，由此产生的双层动态库被称为正交库。已经合成了这种类型的样品库，并显示了电喷雾电离质谱仪中完整的预期组分集。

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