Binding multidentate ligands to Ni~(2+): kinetic identi?cation of preferential binding sites

Dilek Nartop; William Clegg; Ross W. Harrington; Richard A. Henderson; Corinne Y. Wills

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Binding multidentate ligands to Ni~(2+): kinetic identi?cation of preferential binding sites

机译：多齿配体与Ni〜（2+）的结合：优先结合位点的动力学鉴定

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The kinetics of the reactions between [Ni(MeOH)_6]~(2+) (hereafter Ni~(2+)) and a variety of neutral Schiff base multidentate ligands have been measured in methanol at 25.0 °C using stopped-flow spectrophotometry. The ligands contain a variety of different potential donor sites (phenolic OH, imine N, pyridyl N and NH groups), different structural components and substituents. The kinetic studies explore how systematic changes to the composition of the ligands affect the rates of binding. The results are consistent with the Eigen-Wilkins mechanism in which the ligand initially forms an outer-sphere association with Ni~(2+) prior to dissociation of a coordinated solvent molecule and binding to the metal ion. The general features that emerge from these studies are as follows. (i) For ligands with the same donor set, the rates of binding are all similar irrespective of changes to the ligand framework (bridge and substituents). (ii) Comparison of structurally analogous ligands shows that the presence of pyridyl or NH groups in the multidentate results in signi?cantly faster reactions. (iii) With ligands containing multiple NH groups, the rate of ligand binding increases as the number of NH groups increases. The extent to which these kinetic features can be attri- buted to preferential binding of particular donor groups is discussed.

机译：使用停止流光度法在甲醇中于25.0°C下测量了[Ni（MeOH）_6]〜（2+）（以下称Ni〜（2+））与多种中性席夫碱多齿配体之间反应的动力学。所述配体包含多种不同的潜在供体位点（酚OH，亚胺N，吡啶基N和NH基团），不同的结构组分和取代基。动力学研究探索了配体组成的系统变化如何影响结合速率。该结果与本征-维金斯机理一致，在该机理中，配体在与配位溶剂分子解离并与金属离子结合之前先与Ni〜（2+）形成外球缔合。从这些研究中得出的一般特征如下。（i）对于具有相同供体组的配体，无论配体构架（桥和取代基）如何变化，结合速率都相似。（ii）结构相似的配体的比较表明，多齿中吡啶基或NH基团的存在导致明显更快的反应。（iii）对于含有多个NH基团的配体，随着NH基团数目的增加，配体结合的速率增加。讨论了这些动力学特征可归因于特定供体基团优先结合的程度。

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《Dalton transactions: An international journal of inorganic chemistry》 |2014年第8期|共11页
作者
Dilek Nartop; William Clegg; Ross W. Harrington; Richard A. Henderson; Corinne Y. Wills;
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正文语种 eng
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Binding; multidentate; sites;

机译：绑定;多齿;站点;

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Binding multidentate ligands to Ni~(2+): kinetic identi?cation of preferential binding sites

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