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Analysis of the mechanism of charge-transfer coupling in nanometer-scale liquidliquid wo-phase systems and its application to separation science

纳米级液液两相体系电荷转移耦合机理分析及其在分离科学中的应用

基本信息

批准号：
14205120
负责人：
KAKIUCHI Takashi
金额：
$ 35.03万
依托单位：
Kyoto University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (A)
财政年份：
2002
资助国家：
日本
起止时间：
2002 至 2004
项目状态：
已结题

项目摘要

We studied the charge-transfer coupling in nanometer-scale liquid-liquid two-phase systems with emphasis on their fundamental properties and with construction of a variety of liquid-liquid systems that represent the salient features of charge-transfer coupling in nanometer-scale liquid-liquid systems. Furthermore, based on the new findings, phenomena, and laws we found in these systems, we developed the study of the electrochemical instability of interface. First, we proposed systems that represent the fundamental properties of the charge-transfer coupling, using a thin layer of hydrophobic ionic liquid coated on a self-assembled monolayer of a thiol-derivative on gold surface and clarified the electrochemical properties of such systems. Second, we studied the charge transfer processes in micro liquid-liquid systems from four different aspects : i). the mechanism of the way of determining the phase-boundary potential in emulsions of ionic liquids, ii) the determination of the rate of e … More lectron transfer at the micro liquid-liquid interface formed at the tip of a micropipette, making use of the coupling of ion transfer and electron transfer, iii) the solvation dynamics surrounding fluorescent probes in reverse micelles, and iv) the charge transfer across the membrane of a large unilamellar vesicle. We showed that the electrochemical instability is in fact a thermodynamic instability of the interface and demonstrated the generality of this new concept by showing that this instability exists in many different systems. Another important development we made in conducting this project is the opening of a new branch of electrochemistry by showing that a new liquid-liquid interface between a hydrophobic ionic liquid and water can be electrochemically either nonpolarized or polarized, depending on the nature of the ions forming the ionic liquid and also the type of ions dissolved in water. Salt bridges made of a hydrophobic ionic liquid can work as a conceptually new salt bridges relying on the phase-boundary potential and can substitute traditional salt bridges based on the diffusion potential that have been used most imperatively over one hundred years. We also studied the fundamental propertied of nanometer-scale well-defined self-assembled monolayers that can be useful in constructing nanometer-scale structure-controlled systems for studying charge-transfer coupling in confined space and garnered substantial scientific as well as technological knowledge on such systems. Less

我们研究了纳米尺度液-液两相体系中的电荷转移耦合，重点是它们的基本性质，并构建了各种液-液体系，这些体系代表了纳米尺度液-液体系中电荷转移耦合的显著特征。在此基础上，我们进一步开展了界面电化学不稳定性的研究。首先，我们提出了代表电荷转移耦合的基本性质的系统，使用疏水性离子液体的薄层涂覆在金表面上的硫醇衍生物的自组装单层上，并阐明了这样的系统的电化学性质。其次，我们从四个方面研究了微液-液体系中的电荷转移过程：离子液体乳状液中相界电位测定方法的机理; 2）离子液体乳状液中相界电位的测定; ...更多信息利用离子转移和电子转移的耦合，在微量移液器尖端形成的微量液-液界面处的电子转移，iii）在反胶束中围绕荧光探针的溶剂化动力学，和iv）穿过大单层囊泡的膜的电荷转移。我们发现，电化学不稳定性实际上是一个热力学不稳定的界面，并证明了这一新概念的普遍性，表明这种不稳定性存在于许多不同的系统。我们在进行这个项目的另一个重要的发展是开放的一个新的分支的电化学显示，一个新的疏水性离子液体和水之间的液-液界面可以电化学非极化或极化，这取决于形成离子液体的离子的性质，也溶解在水中的离子的类型。由疏水性离子液体制成的盐桥可以作为一种概念上新的盐桥，依赖于相边界势，并可以取代传统的盐桥，基于扩散势已经使用了一百多年。我们还研究了纳米尺度定义良好的自组装单分子膜的基本性质，这些自组装单分子膜可用于构建纳米尺度结构控制系统，用于研究受限空间中的电荷转移耦合，并获得了大量的科学和技术知识。少