Novel Electro-generated Chemiluminescence Reaction at Boron-doped Diamond Electrode and Application for Selective Detection of Bio-related Compounds

硼掺杂金刚石电极新型电致化学发光反应及其在生物相关化合物选择性检测中的应用

基本信息

批准号：
16550157
负责人：
HONDA Kensuke
金额：
$ 2.43万
依托单位：
Yamaguchi University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (C)
财政年份：
2004
资助国家：
日本
起止时间：
2004 至 2005
项目状态：
已结题

项目摘要

The objective of this study is to explore the novel electro-generated chemi-luminescence (ECL) reaction at the boron-doped diamond (BDD) surface and to realize the new analyzing system, especially for medical purpose, using the novel ECL reaction at BDD electrodes.[1]The exploration of the novel ECL reaction at boron-doped diamond surface.For the ECL system of [Ru(bpy)_3]^<2+> at the boron-doped diamond electrodes, the strong ECL emission was observed in the extremely higher potential regions of approximately 3.5 V vs. Ag/AgCl in the presence of ascorbic acid as a co-reactant molecule. The peak potentials of this ECL reaction show the linear relation with the concentration of the co-reactant, and the ECL intensities were correlated with the rates for hydrogen abstraction reaction by OH radicals from the co-reactant. Therefore, it was clarified that the ECL reaction in the extremely higher potential region includes the process of the co-reactant radical formation by OH radicals generate … More d at the BDD surface during water discharge.By applying this novel ECL reaction for the electrochemical analysis, it is possible to selectively detect the compounds that easily form the reducing radicals with OH radicals (e.g.2-propanol or tetrahydrofuran).[2]The development of the diamond ECL sensor for medical application 〜 Analysis System for oxalic acid in urineThe ECL system using [Ru(bpy)_3]^<2+> was the analytical method that enable to selectively detect oxalic acid in urine including numerous electrochemically active compounds by controlling the pH value of the sample. In order to realize the photo-fictionalized electrode material that enable oxalic acid detection, the development of the method of the direct modification of [Ru(bpy)_3]^<2+> on the diamond surface with high density and high durability was carried out. As the modification method, it was selected the methods to form C-C bonding between carbon atoms on diamond surface and terminus of dodecyl groups introduced in the bypyridil legend. Modified BDD electrode was installed into the ECL detector in HPLC system, and the real urine was analyzed. ECL emission was obtained only for oxalic acid in real urine, and ECL intensity for HPLC and that for FIA were in the same range, indicating that this modified BDD electrode can selectively detect oxalic acid in real urine with high sensitivity (S/N=3,5μm). Moreover, this modified electrode did not show the degradation of ECL intensities during continuous analysis over 3 hours. Therefore, we could successfully fabricate the photo-functionalized electrode materials for the selective detection of oxalic acid in real urine with high durability. Less

本研究的目的是探索掺硼金刚石 (BDD) 表面的新型电致化学发光 (ECL) 反应，并利用 BDD 上的新型 ECL 反应实现新的分析系统，特别是用于医疗目的[1]硼掺杂金刚石表面新型ECL反应的探索。对于[Ru(bpy)_3]^<2+>在硼掺杂金刚石电极上的ECL体系，强在抗坏血酸作为共反应物分子存在的情况下，在相对于 Ag/AgCl 的极高电势区域观察到 ECL 发射。该 ECL 反应的峰值电势与共反应物的浓度呈线性关系。反应物，并且ECL强度与OH自由基从共反应物夺氢反应的速率相关，因此，澄清了极高电势区域中的ECL反应包括OH自由基形成共反应自由基的过程在水排放过程中在BDD表面产生d。通过将这种新颖的ECL反应应用于电化学分析，可以选择性地检测容易与OH形成还原自由基的化合物自由基（例如2-丙醇或四氢呋喃）。[2]医疗用金刚石ECL传感器的开发〜尿液中草酸的分析系统使用ECL系统[Ru(bpy)_3]^<2+>是通过控制样品的pH值来选择性检测尿液中包含多种电化学活性化合物的草酸的分析方法，从而实现光虚构电极材料。为了能够检测草酸，开发了高密度和高耐久性的[Ru(bpy)_3]^<2+>直接修饰金刚石表面的方法作为修饰方法。形成方法将吡啶基图例中引入的金刚石表面碳原子与十二烷基末端之间的C-C键安装到HPLC系统的ECL检测器中，仅对真实尿液中的草酸进行了ECL发射分析。，且 HPLC 和 FIA 的 ECL 强度在同一范围内，表明该改进的 BDD 电极可以高灵敏度选择性地检测真实尿液中的草酸(S/N=3,5μm)，该修饰电极在连续分析超过3小时的过程中没有表现出ECL强度的下降，因此，我们可以成功地制备用于选择性检测草酸的光功能化电极材料。真实尿量少，耐久性高。