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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Impact of ligand protonation on eigen-type metal complexation kinetics in aqueous systems
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Impact of ligand protonation on eigen-type metal complexation kinetics in aqueous systems

机译：配体质子化对水体系中本征型金属络合动力学的影响

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摘要

The impact of ligand protonation on metal speciation dynamics is quantitatively described. Starting from the usual situation for metal complex formation reactions in aqueous systems, i.e., exchange of water for the ligand in the inner coordination sphere as the rate-determining step (Eigen mechanism), expressions are derived for the lability of metal complexes with protonated and unprotonated ligand species being involved in formation of the precursor outer-sphere complex. A differentiated approach is developed whereby the contributions from all outer-sphere complexes are included in the rate of complex formation, to an extent weighted by their respective stabilities. The stability of the ion pair type outer-sphere complex is given particular attention, especially for the case of multidentate ligands containing several charged sites. It turns out that in such cases, the effective ligand charge can be considerably different from the formal charge. The lability of Cd(II) complexes with 1,2-diaminoethane-N,N'-diethanoic acid at a microelectrode is reasonably well predicted by the new approach.
机译：定量描述了配体质子化对金属形态动力学的影响。从水体系中金属配合物形成反应的通常情况开始，即，将水交换为内配位体中的配体作为决定速率的步骤（本征机理），得出具有质子化和氢键的金属配合物的不稳定性的表达式。未质子化的配体物质参与前体外球络合物的形成。提出了一种差异化的方法，其中所有外圈复合物的贡献都包括在复合物的形成速率中，并在一定程度上由它们各自的稳定性加权。特别要注意离子对型外球络合物的稳定性，特别是对于含有多个带电位点的多齿配体的情况。事实证明，在这种情况下，有效的配体电荷可能与形式电荷大不相同。新方法可以很好地预测Cd（II）与1,2-二氨基乙烷-N，N'-二硫辛酸在微电极上的不稳定性。

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