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.

这项研究的目的是发明在液态液体界面上发明单个分子行为和金属络合动力学的新测量方法，并阐明界面的纳米特性以及络合的动力学反应机理。获得了以下有用的结果； 1）通过荧光显微镜将吸附在界面吸附的单分子探针方法评估界面的纳米杂质。从观察到的结果中，首次评估界面处的扩散系数和界面的粘度。还评估了共吸附表面活性剂分子对单分子扩散的影响。2）在各种溶剂提取系统中确认了离心液液膜方法的直接测量方法的发明。为了测量快速界面反应的快速界面反应，构建了新的微型外部流动荧光显微镜。此外，发明了一个离心液膜/拉曼显微镜和微二相质谱。3）当界面上的界面上的界面催化和分子识别在界面上的界面上始终催化，当时是在配体或中间复杂复合物的相互作用时催化的。这些发现可用于考虑界面的催化作用的溶剂提取系统的设计。我们发现，金属配合物的聚集在界面上比在大相位相比受到青睐。同样，界面聚集在核酸碱基和二嗪异构体中表现出新的分子识别能力。4）成功应用了互际分子模拟方法的分子模拟，以估算配体的互化能量。