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Electrochemical Regulation of the Dynamic Behavior of Mososcopic Molecular Assemblies at Solid-Liquid Interfaces

固液界面微观分子组装体动态行为的电化学调节

基本信息

批准号：
11650849
负责人：
SAGARA Takamasa
金额：
$ 2.11万
依托单位：
Nagasaki University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (C)
财政年份：
1999
资助国家：
日本
起止时间：
1999 至 2000
项目状态：
已结题

项目摘要

(1) The dynamic behavior of a viologen monolayer on a Au electrode surface was investigated. It was found that the redox potential is strongly affected by ingress-egress of the counter anion coupled with the binding interaction and that the monolayer memorizes the anion present when forming the monolayer, though the memory is erased by the addition of a softer anion in the electrolyte solution. Significance of the dynamic ion transfer process was demonstrated in the terms of not only charge compensation but also monolayer structure.(2) It was found that a water-insoluble dye, hypericin, undergoes redox reaction on an electrode surface in an aqueous medium when the dye is incorporated into a cationic artificial lipid film. The redox potential was found to be controllable by regulating the lipid structure.(3) Octadecylrhodamine B gave rise to two types of electroreflectance responses, faradaic response due to the redox process and non-faradaic one due to, for example, dynamic adsorption-desorption process. Addition of a surfactant made the redox reaction be more reversible while annihilating the non-faradaic processes.(4) The voltammetric spike response of heptylviologen at a HOPG electrode horizontally-touched to gas/heptylviologen aqueous solution interface was investigated in detail. The conditions of the appearance of the spike were listed up. It was found that the spike response is due to the first-order faradaic phase-transition process between a Gibbs film at a gas/solution interface and a Langmuir monolayer. The dynamics was governed by nucleation-growth-collision kinetics.(5) Dynaunic processes of Au nano-particles immobilized on a monolayer-modified Au electrode were studied using electroreflectance methods. An electroreflectance response due to potential-dependent charging-discharging process of the Au nano-particle was clearly observed at the wavelength of surface plasmon absorption.

(1)研究了紫精单分子膜在Au电极表面的动力学行为。有人发现，氧化还原电位的强烈影响的结合相互作用耦合的反阴离子的进出，单层记忆的阴离子存在时，形成单层，虽然记忆被擦除的电解质溶液中添加一个较软的阴离子。动态离子转移过程的意义不仅表现在电荷补偿方面，而且表现在单层结构方面。(2)结果发现，水不溶性染料，金丝桃素，在水性介质中的电极表面上进行氧化还原反应时，染料被纳入阳离子人工脂质膜。氧化还原电位被发现是可控的，通过调节脂质结构。(3)十八烷基罗丹明B产生了两种类型的电反射响应，法拉第响应由于氧化还原过程和非法拉第响应由于，例如，动态吸附-脱附过程。表面活性剂的加入使氧化还原反应更加可逆，同时消除了非法拉第过程。(4)研究了庚基紫精在水平接触的HOPG电极上的伏安峰响应。列出了出现尖峰的条件。有人发现，尖峰响应是由于一阶法拉第相变过程之间的吉布斯膜在气体/溶液界面和朗缪尔单分子层。动力学受成核-生长-碰撞动力学控制。(5)采用电反射法研究了Au纳米粒子固定在单层修饰Au电极上的动力学过程。在表面等离子体吸收波长处，可以清楚地观察到Au纳米颗粒的电位依赖性充放电过程引起的电反射响应。