基于对金属纳米粒子催化刻蚀作用的小分子比色分析法

发布时间：2018-11-03 21:28

【摘要】：由于经济的快速发展所出现的越来越多的环境污染问题已经严重影响了生态环境的可持续发展和人类的生存健康。因此,探究灵敏、迅速地检测环境污染物的分析方法显得愈发重要。纳米材料凭借其优良的性能,已被广泛地应用于环境和生物检测。由于金属纳米粒子具有独特的光学性质,所以可以将其作为光学传感信号来发展高灵敏的检测污染物的光化学分析法。其基本原理是通过金属纳米粒子(含功能化的纳米粒子)与待测物发生化学反应,改变其光学性质,从而实现对待测分子的选择性检测。本论文利用某些小分子在特定条件下催化刻蚀金属纳米粒子,从而使纳米粒子的颜色发生改变的性质,研发了两种小分子的快速检测方法。具体内容如下:1.基于对金纳米棒催化刻蚀作用的锰离子比色分析法。本方法利用金纳米棒作为比色试剂,通过金纳米棒的形貌变化实现锰离子的检测。在氨三乙酸(NTA)存在的情况下,二价锰Mn(II)与高碘酸钾(KIO4)反应,生成Mn(III)-NTA络合物。而这种Mn(III)-NTA络合物可以氧化刻蚀金纳米棒,同时自身被还原为Mn(II)。在这个过程中,金纳米棒的形貌发生了变化,其溶液颜色由蓝绿色变成红色,最后变成浅黄色。根据这一原理,实现了对于锰离子高灵敏度、高选择性的检测,检出限为1.0 nM。另外,我们利用这一方法成功地实现了实际水样中锰离子的检测。2.基于对纳米二氧化锰催化刻蚀作用的抗坏血酸比色分析法。在弱碱性溶液中,抗坏血酸将二氧化锰纳米粒子还原为二价锰离子,而自身转化为可被三(2-羧乙基)膦(TCEP)还原的脱氢抗坏血酸。还原而成的抗坏血酸进一步刻蚀二氧化锰纳米粒子,从而实现抗坏血酸对二氧化锰纳米粒子的催化刻蚀。在这个过程中,由于二氧化锰纳米粒子逐渐变小,溶液颜色由黄色逐渐变成无色。根据这个现象,我们研发了一种检测尿样中抗坏血酸的简便方法。
[Abstract]:Due to the rapid development of economy, more and more environmental pollution problems have seriously affected the sustainable development of ecological environment and human survival and health. Therefore, it is more and more important to explore the analytical method of sensitive and rapid detection of environmental pollutants. Nanomaterials have been widely used in environmental and biological detection because of their excellent properties. Metal nanoparticles have unique optical properties, so they can be used as optical sensing signals to develop a highly sensitive photochemical analysis method for the detection of pollutants. The basic principle is to change the optical properties of metal nanoparticles (including functional nanoparticles) by chemical reaction with the object to be tested, so as to realize the selective detection of the tested molecules. In this paper, two rapid detection methods for metal nanoparticles were developed by using some small molecules to catalyze the etching of metal nanoparticles under certain conditions, thus changing the color of nanoparticles. The specific contents are as follows: 1. Manganese ion colorimetric analysis based on catalytic etching of gold nanorods. Using gold nanorods as colorimetric reagent, manganese ions can be detected by changing the morphology of gold nanorods. In the presence of (NTA), manganese divalent Mn (II) reacts with potassium periodate (KIO4) to form Mn (III) NTA complex. The Mn (III)-NTA complex can oxidize and etch gold nanorods and be reduced to Mn (II). During this process, the morphology of the gold nanorods changed from blue-green to red, and finally to light yellow. According to this principle, the detection limit of manganese ion is 1.0 nM. with high sensitivity and selectivity. In addition, we have successfully realized the detection of manganese ions in real water samples by using this method. 2. 2. Ascorbic acid colorimetric analysis based on catalytic etching of nanometer manganese dioxide. In a weak alkaline solution, ascorbic acid reduced manganese dioxide nanoparticles to divalent manganese ions and converted itself to dehydroascorbic acid, which can be reduced by tris (2-carboxyethyl) phosphine (TCEP). The reduced ascorbic acid further etched manganese dioxide nanoparticles, thus realizing the catalytic etching of manganese dioxide nanoparticles by ascorbic acid. In the process, the color of the solution gradually changed from yellow to colorless because the manganese dioxide nanoparticles became smaller. Based on this phenomenon, we developed a simple method for the detection of ascorbic acid in urine samples.
【学位授予单位】：中国科学院烟台海岸带研究所
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X830.2

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