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Molecular mechanism of liquid-liquid interfacial complexation and development of its function

液-液界面络合的分子机制及其功能发展

基本信息

批准号：
12304045
负责人：
WATARAI Hitoshi
金额：
$ 28.85万
依托单位：
OSAKA UNIVERSITY
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (A)
财政年份：
2000
资助国家：
日本
起止时间：
2000 至 2002
项目状态：
已结题

来源：
https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-12304045/
关键词：
liquid-liquid interface Complex formation Interfacial aggregation Interfacial molecular recognition Solvent extraction Two-phase micro-sheath flow method Molecular dynamics simulation Centrifugal liquid membrane method 錯体生成反応分子認識二相マイ

项目摘要

The aim of this study was to invent new measurement methods of a single molecule behavior and metal complexation kinetics at the liquid-liquid interface and to elucidate the nano property of the interface and the kinetic reaction mechanisms of the complexation. Following useful results were obtained;1) Evaluation of nanoproperty of the interface by the single molecule probe methodA single fluorescent molecule adsorbed at the interface was chased by a fluorescent microscopy. From observed results, the diffusion coefficient at the interface and the viscosity of the interface was evaluated for the first time. The effect of co-adsorbed surfactant molecules on the single molecule diffusion was also evaluated.2) Invention of direct measurement method of interfacial reactionsThe utility of the centrifugal liquid membrane method was confirmed in various solvent extraction systems. To measure fast interfacial reaction as rapid as a few micro second, a new micro-sheath flow fluorescence microscopy was constructed. Furthermore, a centrifugal liquid membrane/ Raman microscopy and a micro-two phase mass spectrometry were invented.3) Interfacial catalysis and molecular recognition at the interfaceComplexation at the interface was always catalyzed when the adsorption of the ligand or the intermediate complex took place in the process of the reaction. These findings are useful for the design of solvent extraction systems taking into account the catalytic role of the interface. We find out that the aggregation of metal complex was favored at the interface than in bulk phase. Also, the interfacial aggregation exhibited novel molecular recognition ability for nucletic acid bases and diazine isomers.4) Molecular simulation of the interfaceMolecular simulation method was successfully applied for the estimation of the interfacial adsorption energy of ligand.

本研究的目的是发明液-液界面单分子行为和金属络合动力学的新测量方法，并阐明界面的纳米性质和络合的动力学反应机制。得到了以下有用的结果： 1）单分子探针法评价界面的纳米性能用荧光显微镜追踪吸附在界面上的单个荧光分子。根据观测结果，首次评价了界面扩散系数和界面粘度。还评估了共吸附表面活性剂分子对单分子扩散的影响。2）界面反应直接测量方法的发明离心液膜法在各种溶剂萃取系统中的实用性得到证实。为了测量快至几微秒的快速界面反应，构建了一种新的微鞘流荧光显微镜。此外，还发明了离心液膜/拉曼显微镜和微两相质谱仪。3）界面催化和界面分子识别反应过程中，配体或中间络合物发生吸附时，界面处的络合总是受到催化。这些发现对于考虑界面的催化作用的溶剂萃取系统的设计很有用。我们发现金属络合物在界面处比在体相中更有利于聚集。此外，界面聚集对核酸碱基和二嗪异构体表现出新颖的分子识别能力。4）界面的分子模拟分子模拟方法成功地应用于配体界面吸附能的估计。