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Design and construction of metalloproteins/bilayer film devices and their application

金属蛋白/双层膜器件的设计与构建及其应用

基本信息

批准号：
08455443
负责人：
NAKASHIMA Naotoshi
金额：
$ 4.99万
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：
1996
资助国家：
日本
起止时间：
1996 至 1998
项目状态：
已结题

项目摘要

Results of our research project titled on Design and construction of metalloproteins/bilayer film devices and their application are summarized as follows.1. A ferrocene with double long chains, 2C16GluFc, was synthesized and regulated mediated electron transfer reactions of glucose oxidase immobilized on a lipid film containing ferrocene was examined. A graphite (BPG) electrode modified with a cast of 2CI6GluFc and a synthetic lipid, dihexadecyldimethylammonium bromide (2C16N^+Br^-) gave phase transition dependent cyclic voltammograms. Normal pulse voltammetry proved that the enhancement of the faradaic current at the electrode at temperatures above the phase transition is ascribable to the increase in the apparent diffusion rate constants. Glucose oxidase was immobilized on the film of 2C16GluFc/2C16N^+Br^- on BPG and ferrocene-mediated catalytic electron transfers in the presence of glucose were explored. Temperature experiment has revealed that the phase transition regulates the catalytic electron transfer reaction.2. Thermal stability of the [2Fe-2S] cluster structure of ferredoxin embedded in the films of four artificial ammonium lipid was much improved than that of ferredoxin in solution. Artificial cationic ammonium lipid films were found to provide suitable microenvironments for the incorporation of ferredoxin in a way to undergo electrochemical communication with the underlying electrodes. We have demonstrated for the first time that the diffusion constant, D, and the heterogeneous electron transfer rate constant, k^0', for ferredoxin embedded in a cast film of an artificial lipid, 2C18N^+Br^-, are 4 X 10^-^1^0 cm^2 s^-^1 and 1.4 X 10^-^4 cm s^-^1, respectively. D and k^0' values of ferredoxin in the films of the films were close with those of ferredoxin in 2C18N^+r^- films. The experimentally observed voltammograms of ferredoxin in the film fitted well with the simulated voltammograms using the obtained D and k^0'.

我们的研究项目《金属蛋白/双层膜器件的设计与构建及其应用》的研究成果总结如下。合成了一种双长链二茂铁，2C16GluFc，并研究了葡萄糖氧化酶在含二茂铁的脂膜上的调节电子转移反应。用2Cl6GluFc铸型和合成脂类十六烷基二甲基溴化铵(2C16N+Br^-)修饰的石墨(BPG)电极给出了相变相关的循环伏安曲线。常规脉冲伏安法证明，在高于相变温度时，电极法拉第电流的增强可归因于表观扩散速率常数的增加。将葡萄糖氧化酶固定在BPG上的2C16GluFc/2C16N^+Br^-膜上，研究了葡萄糖存在下二茂铁催化电子转移的情况。温度实验表明，相变对催化电子转移反应有调节作用。铁氧还蛋白[2Fe-2S]团簇结构在四种人工氨脂薄膜中的热稳定性比铁氧还蛋白在溶液中的热稳定性显著提高。人工阳离子铵类脂膜为铁氧还蛋白的掺入提供了合适的微环境，使其与电极发生电化学通信。我们首次证明了铁氧还蛋白在人工脂2C18N^+Br^-铸膜层中的扩散常数D和非均相电子转移速率常数k^0‘分别为4×10^-1×10^-1 cm S^-^1和1.4×10^-4 cm S^-^1。铁氧还蛋白在薄膜中的d和k^0‘值与2C18N^+r^-薄膜中的接近。实验观察到的铁氧还蛋白在薄膜中的伏安图与用得到的D和k^0‘模拟的伏安图符合得很好。