解離不活性ランタノイドーポリアミノカルボン酸錯体を用いる高性能分析法の開発

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Analytical methods of Ln^III were developed in which the kinetic inertness of Ln^III complexes with acyclic polyaminocarboxylate (PAC) on the dissociation reaction was the key to establishing detection systems. First, a pre-derivatization HPLC method with fluorescent detection was developed for closedshell Ln^III using an aromatic octadentate PAC as the derivatizing reagent. Selective detection at ppb levels was achieved. Second, the factors to form inert Ln-pac complexes were investigated on the dissociation reaction. The rate constants and activation parameters were determined for a series of Ln^III-hexadentate and octadentate PAC complexes. Interestingly, an unusually large negative activation entropy for solvolysis governed the kinetic inertness, and was probably derived from metal envelopment in the complex and hydration on the activation state. Third, a novel measurement method of the dissociation rate was developed using capillary electrophoresis (CE). The dissociation rate constant for the Ce^III-PAC complex was determined for the first time. Fourth, based on the result of the second study, a sensitive pre-derivatizing CE method for Ln^III at the fmol level was developed using an aromatic EDTA derivative. In this method, a high resolution was achieved by introducing a ternary complex equilibrium in the carrier. Finally, the energy-transfer luminescence of a Tb^III complex with a PAC possessing phenol function was studied. The detection limit at the ppt level was achieved, and the photophysics was also investigated.
社団法人日本分析化学会の論文
2003-01-05

解離不活性ランタノイドーポリアミノカルボン酸錯体を用いる高性能分析法の開発

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