Potential-driven reversible regulation of hierarchical dynamics of nano-entities and functionalization of electrified interfaces

纳米实体分层动力学的势驱动可逆调控和带电界面的功能化

• 批准号: 16350077
• 负责人: SAGARA Takamasa
• 金额: $ 9.66万
• 依托单位: Nagasaki University
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (B)
• 财政年份: 2004
• 资助国家: 日本
• 起止时间: 2004 至 2006
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-16350077/
• 关键词: Electrode surface; Ultra-thin films; Surface and Interfacial Properties; Metal nanoparticle; Dendrimer; Viologen; Dynamics; Phase transition; ナノ材料; 吸脱着; 赤外反射分光法; 蛍光性デンドリマー; 両親媒性長鎖分子; 長鎖分子集合組織

1. In situ characterization methods being indispensable as basic techniques in this research were developed for the measurements of adsorption state, molecular orientation, micro-environment and molecular assembling structure as well as their potential dependent dynamics on electrode surfaces: (1) Electroreflectance methods were sophisticated, for example, to elucidate the adsorption orientation of macromolecules and to track the potential step transients of the surface processes, (2) An 1R reflection instrument was constructed, and (3) The fluorescence spectral analysis and moving imaging microscopic observation were developed.2. The title research targets at electrified interfaces included liquid alkane thin films, surface assemblies of amphiphiles, viologen adsorption layers, a fluorescent dendrimer, and surface-modified Au nanoparticles. Representative achievements are listed below.(1) Alkane molecules were found to be potential-responsible on a Au(III) electrode. The dynamics extended to far distances from the electrode surface to the bulk of the aqueous solution.(2) Systematic understandings of potential-driven assembling structural changes of pyridyl and imidazolyl terminated amphiphiles on a Au(III) electrode surface were established.(3) Two-dimensional faradaic phase transition behavior of various viologen molecules on a HOPG electrode was described in terms of interplay of multiple modes of intermolecular interactions.(4) An anomalous effect of dendrimer adsorption upon redox reaction was found. Potential dependent reshape of dendrimer also was analyzed.(5) Potential-driven dynamics of Au nanoparticles were elucidated, together with adsorption-desorption and charging-discharging processes as well as anion effects.3. These results would be quite useful for design of dynamics and interfacial functionalization in the near future.

1.原位表征方法是本研究中不可缺少的基本技术，用于测量电极表面的吸附状态、分子取向、微环境和分子组装结构以及它们的电位依赖动力学：（1）电反射方法是复杂的，例如，为了阐明大分子的吸附取向和跟踪表面过程的潜在阶跃瞬态，（2）构造了1 R反射仪，（3）开展了荧光光谱分析和移动成像显微观察.在带电界面的研究目标包括液体烷烃薄膜，两亲分子的表面组装，紫精吸附层，荧光树枝状大分子，和表面修饰的Au纳米粒子。代表性成就如下。(1)烷烃分子在Au（III）电极上具有电位响应性。动力学扩展到从电极表面到水溶液主体的很远距离。(2)建立了吡啶基和咪唑基封端的两亲分子在Au（III）电极表面电位驱动组装结构变化的系统认识。(3)根据多种分子间相互作用模式的相互作用，描述了不同紫精分子在HOPG电极上的二维法拉第相变行为。(4)发现了树枝状大分子吸附对氧化还原反应的异常影响，并分析了电位依赖的树枝状大分子的形状改变。(5)阐明了Au纳米粒子的电位驱动动力学，吸附-脱附和充放电过程以及阴离子效应.这些结果将是相当有用的动力学设计和界面功能化在不久的将来。

项目成果

2D Phase Transition of Viologens on HOPG Surfaces inElectrode Processes VII

电极过程中 HOPG 表面紫罗碱的二维相变 VII

• 发表时间: 2005
• 作者: Morita;Y.;Takamasa Sagara;K.Nishiyama;Katsuhiko NISHIYAMA;Ayumi Toyota;Takamasa Sagara;Katsuhiko NISHIYAMA;Toshishiko Sakurai;K.Nishiyama;Takamasa Sagara;Mie Yasuhiro;Takamasa Sagara;Takamasa Sagara;Takamasa Sagara;Katsuhiko NISHIYAMA;Takamasa Sagara;Takamasa Sagara;Katsuhiko NISHIYAMA;Takamasa Sagara;Takamasa Sagara
• 通讯作者: Takamasa Sagara

「有機薄膜(LB、SAM)」、実験化学講座改訂5版、第27巻機能性質、第5章1節1項 (日本化学会編)

《有机薄膜（LB、SAM）》实验化学课程修订第5版第27卷功能特性第5章第1节第1节（日本化学会编）

• 发表时间: 2004
• 作者: Y.Teki;H.Tamekiu i;K.Haruta;J.Takauchi;Y.Miura;Katsuhiko NISHIYAMA;相楽隆正;相樂隆正
• 通讯作者: 相樂隆正

Dynamic Behaviors of Molecular Assemblies and Nano-Substances at Electrified Interfaces in Bottom-up Nanofabrication : Supramolecules, Self-Assemblies, and Organized Films

自下而上纳米加工中带电界面处的分子组装体和纳米物质的动态行为：超分子、自组装体和有序薄膜

• 发表时间: 2007
• 作者: Morita;Y.;Takamasa Sagara;K.Nishiyama;Katsuhiko NISHIYAMA;Ayumi Toyota;Takamasa Sagara;Katsuhiko NISHIYAMA;Toshishiko Sakurai;K.Nishiyama;Takamasa Sagara;Mie Yasuhiro;Takamasa Sagara;Takamasa Sagara;Takamasa Sagara
• 通讯作者: Takamasa Sagara

Dynamic Behaviors of Molecular Assemblies and Nano-Substances at Electrified Interfaces in Bottom-up Nanofabrication : Supramolecules, Self- Assemblies, and Organized Films

自下而上纳米加工中带电界面处的分子组装体和纳米物质的动态行为：超分子、自组装体和组织薄膜

• 发表时间: 2007
• 期刊: American Scientific Publishers (in press)
• 作者: Morita;Y.;Takamasa Sagara
• 通讯作者: Takamasa Sagara

Estimation of the orientation of heme in cytochrome c immobilized on a carboxylate-terminated alkanethiol monolayer on a Au electrode by the use of electroreflectance spectroscopy with polarized light incidence

使用偏振光入射电反射光谱估计固定在 Au 电极上羧酸盐封端的烷硫醇单层上的细胞色素 C 中血红素的方向

• 发表时间: 2006
• 期刊: Journal of Physical Chemistry B 110(3)
• 作者: Morita;Y.;Takamasa Sagara;K.Nishiyama;Katsuhiko NISHIYAMA;Ayumi Toyota;Takamasa Sagara
• 通讯作者: Takamasa Sagara