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

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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