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首页> 外文期刊>Chemistry: A European journal >Using Remote Substituents to Control Solution Structure and Anion Binding in Lanthanide Complexes
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Using Remote Substituents to Control Solution Structure and Anion Binding in Lanthanide Complexes

机译：使用远程取代基控制镧系元素络合物的溶液结构和阴离子结合

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摘要

A study of the anion-binding properties of three structurally related lanthanide complexes, which all contain chemically identical anion-binding motifs, has revealed dramatic differences in their anion affinity. These arise as a consequence of changes in the substitution pattern on the periphery of the molecule, at a substantial distance from the binding pocket. Herein, we explore these remote substituent effects and explain the observed behaviour through discussion of the way in which remote substituents can influence and control the global structure of a molecule through their demands upon conformational space. Peripheral modifications to a binuclear lanthanide motif derived from a,a'-bis(DO3Ayl)-m-xylene are shown to result in dramatic changes to the binding constant for isophthalate. In this system, the parent compound displays considerable conformational flexibility, yet can be assumed to bind to isophthalate through a well-defined conformer. Addition of steric bulk remote from the binding site restricts conformational mobility, giving rise to an increase in binding constant on entropic grounds as long as the ideal binding conformation is not excluded from the available range of conformers.
机译：对三种结构相关的镧系元素络合物（均包含化学上相同的阴离子结合基序）的阴离子结合性质的研究表明，它们的阴离子亲和力存在显着差异。这些是由于在距结合袋相当远的距离处分子外围上的取代模式变化的结果而产生的。在本文中，我们探索了这些远程取代基效应，并通过讨论远程取代基可以通过其对构象空间的要求影响和控制分子的整体结构的方式来解释观察到的行为。显示对衍生自α，a′-双（DO 3 Ayl）-间二甲苯的双核镧系元素基序的外围修饰导致间苯二甲酸酯的结合常数的显着变化。在该系统中，母体化合物显示出相当的构象柔韧性，但仍可以假定它通过定义明确的构象异构体与间苯二甲酸酯结合。只要不从构象异构体的可用范围内排除理想的结合构象，远离结合位点的位阻本体的加入会限制构象的迁移性，从而导致熵基础上的结合常数增加。

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