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基于金纳米棒的新型非聚集比色传感器的研究

发布时间:2018-10-29 11:11
【摘要】:金纳米棒(AuNRs)是一种在可见光和近红外区具有独特光学特性的棒状金纳米颗粒,在吸收光谱上同时有横向和纵向表面等离子共振吸收峰。随着金纳米棒长径比、形状、尺寸和环境介质物理性质的改变,其等离子共振吸收峰的位置不同,金纳米棒溶液也呈现出不同的颜色,为新型比色传感器的构筑和开发提供了理想的平台。本文首先采用种子生长法制备金纳米棒,再将其分散于聚乙烯醇溶液中,以戊二醛为交联剂,制备了对二价汞离子(Hg2+)有光学响应性的化学交联金纳米棒-聚乙烯醇(AuNRs-PVA)复合水凝胶。用于Hg2+检测时,在还原剂抗坏血酸的辅助下,溶液中的Hg2+被还原为Hg0,与固定在凝胶网格中的金纳米棒结合形成金汞齐,导致金纳米棒的长径比减小,凝胶的颜色也显著改变。该传感器对Hg2+有良好的响应性和选择性,测量线性范围为0~3.0μM,相关系数为0.997,响应时间为5min。通过对金纳米棒的固定,克服了金纳米棒在复杂检测环境中的稳定性问题,所构建的光学传感器具有制备方法简便、稳定性高等优点,可用于水体中微量汞离子的检测。甲醛是一种具有强烈刺激性的化学物质,对人体健康有严重威胁。本文利用金纳米棒和汞之间的强亲和性,在甲醛检测中引入Hg2+为辅助试剂,利用甲醛在碱性环境中较强的还原性将Hg2+还原为Hg0,通过检测金纳米棒纵向等离子体共振吸收峰的位置和溶液的颜色变化,发展了一种新型的基于金纳米棒等离子体共振特性的非聚集法甲醛比色传感器。将这种传感器用于实际水样中甲醛含量的测定,显示其具有高选择性、高灵敏度等特点,是一种实用性强和应用前景广阔的甲醛检测方法。由于表面活性剂层的存在,用种子生长法制备的金纳米棒在溶液中带正电。本文中以两性聚电解质明胶为稳定剂,利用明胶与金纳米棒的静电相互作用,制备了明胶包覆的金纳米棒(Gelatin-AuNRs)。Zeta电位、透射电镜和紫外-可见光谱分析结果表明,明胶层的存在显著增强了金纳米棒的耐盐稳定性,克服了金纳米棒溶液在高浓度电解质溶液中容易发生聚集和沉降的缺点。同时,研究发现Gelatin-AuNRs对Hg2+的响应行为与未表面改性的金纳米棒不同,其溶液颜色变化更鲜艳,利用吸收光谱进行Hg2+检测的结果也更准确,并对这种现象的机理进行了探讨。
[Abstract]:Gold nanorods (AuNRs) is a kind of rod-shaped gold nanoparticles with unique optical properties in the visible and near infrared region. There are transverse and longitudinal surface plasmon resonance absorption peaks at the same time in the absorption spectra of gold nanorods. With the change of aspect ratio, shape, size and physical properties of the ambient medium, the position of the plasmon resonance absorption peak of gold nanorods is different, and the gold nanorods have different colors. It provides an ideal platform for the construction and development of new colorimetric sensor. In this paper, gold nanorods were prepared by seed growth method, then dispersed in polyvinyl alcohol solution with glutaraldehyde as crosslinking agent. A chemically crosslinked gold nanorod polyvinyl alcohol (AuNRs-PVA) hydrogel with optical response to divalent mercury ion (Hg2) was prepared. When used in Hg2 detection, with the aid of ascorbic acid, the Hg2 in the solution was reduced to Hg0, and the gold nanorods fixed in the gel grid were combined to form gold amalgam, which resulted in the decrease of the aspect ratio of gold nanorods and the change of gel color. The sensor has good response and selectivity to Hg2. The linear range is 0 渭 m, the correlation coefficient is 0.997, and the response time is 5 min. The stability of gold nanorods in complex detection environment is overcome by fixing gold nanorods. The optical sensor has the advantages of simple preparation and high stability. It can be used for the detection of trace mercury ions in water. Formaldehyde is a kind of chemical substance with strong irritation, which is a serious threat to human health. In this paper, the strong affinity between gold nanorods and mercury was used, Hg2 was introduced as auxiliary reagent in formaldehyde detection, and Hg2 was reduced to Hg0, by formaldehyde in alkaline environment. By detecting the position of the longitudinal plasma resonance absorption peak of gold nanorods and the color change of the solution, a new non-aggregated formaldehyde colorimetric sensor based on the plasma resonance characteristics of gold nanorods was developed. The sensor has been applied to the determination of formaldehyde in real water samples. It shows that the sensor has the characteristics of high selectivity and high sensitivity. It is a practical and promising method for the determination of formaldehyde. Due to the existence of surfactant layer, the gold nanorods prepared by seed growth method are positively charged in solution. Using amphoteric polyelectrolyte gelatin as stabilizer, the gelatin coated gold nanorods (Gelatin-AuNRs). Zeta potential, TEM and UV-Vis) were prepared by electrostatic interaction between gelatin and gold nanorods. The existence of gelatin layer enhances the salt resistance stability of gold nanorods and overcomes the shortcoming that gold nanorods are easy to accumulate and settle in high concentration electrolyte solution. At the same time, it is found that the response behavior of Gelatin-AuNRs to Hg2 is different from that of unmodified gold nanorods, the color of the solution changes more brightly, and the results of Hg2 detection by absorption spectra are more accurate. The mechanism of this phenomenon is also discussed.
【学位授予单位】:郑州大学
【学位级别】:硕士
【学位授予年份】:2015
【分类号】:TB383.1;O614.123

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