磁性石墨烯复合材料的合成及其在环境水样中农药和抗生素残留分析中的应用

发布时间：2018-03-09 04:19

本文选题：磁性氧化石墨烯　切入点：羧基化　出处：《苏州科技大学》2017年硕士论文　论文类型：学位论文

【摘要】：农药和抗生素被广泛使用于农业种植业和畜牧养殖业中,它们良好的水溶性和稳定的化学结构,使其能够快速扩散到环境水体中并长期存在而不被降解。一定浓度的农药和抗生素残留会对动植物和人类健康产生危害,因而,建立环境水样中农药和抗生素残留的测定方法具有十分重要的意义。磁性石墨烯复合材料集便捷的磁分离和高效的吸附性于一身,是一种极具潜力的新型吸附剂,近年来在环境、食品和生物等方面的应用已有文献报道。本论文制备出磁性石墨烯复合材料,应用于磁性固相萃取中并与高效液相色谱-串联质谱法相结合,完成对环境水样中三嗪类除草剂和磺胺类抗生素残留的分析测定。本论文主要内容包括以下几点:1、介绍了农药和抗生素的基本情况和常见的几种样品预处理技术,着重阐述了磁性固相萃取的概况和应用,以及磁性固相萃取剂的研究进展。2、采用一步合成法制备磁性氧化石墨烯材料(GO-Fe3O4),将其用作磁性固相吸附剂对环境水样中的6种三嗪类除草剂进行萃取和富集,并与高效液相色谱-串联质谱法相结合进行测定。合成的材料用扫描电镜和傅里叶红外光谱表征。为提高萃取效率,优化了GO-Fe3O4用量、萃取时间、水样的p H及离子强度和解吸条件等影响因素。6种三嗪类除草剂的检出限为0.1~1.0 ng/L,富集倍数可达616~902。将本方法应用于苏州地区的太湖水、运河水和护城河水等实际水样的分析,得到加标回收率范围在85.4%~117.6%之间,相对标准偏差为1.2%~10.0%。该方法操作简单快速,富集倍数较高,检出限低,可用于水样中痕量三嗪类除草剂残留的检测分析。3、成功合成出羧基化的磁性氧化石墨烯材料(CGO/Fe3O4),作为磁性固相吸附剂用于萃取环境水样中的磺胺类抗生素。运用改进的共沉淀法制备出CGO/Fe3O4,并通过扫描电子显微镜和傅里叶红外光谱仪进行表征。8种磺胺类抗生素作为目标分析物来评估方法的萃取效率,并使用高效液相色谱-串联质谱法进行测定。对CGO/Fe3O4用量、萃取时间、样品溶液的p H及离子强度和解吸条件几个影响因素进行了优化来提高萃取效率,还将CGO/Fe3O4与GO/Fe3O4对磺胺类抗生素的吸附和萃取能力作了对比。在最优萃取条件下,得到了良好的线性范围,相关系数大于0.9983,方法的检出限为0.49~1.59 ng/L,富集倍数达1320~1702。将该方法应用于苏州地区的废水、河水和自来水等实际水样的分析,得到加标回收率范围在83.2%~109.2%之间,相对标准偏差为1.8%~11.2%。由于其简单快速的操作,高浓缩倍数和低检出限,本方法可用于环境水样中痕量磺胺类抗生素残留的分析。4、对论文作出总结,概述实验得出的主要结论。
[Abstract]:Pesticides and antibiotics are widely used in farming and animal husbandry. They have good water solubility and stable chemical structure. So that it can spread rapidly into environmental waters and exist for a long time without being degraded. Certain concentrations of pesticides and antibiotic residues can cause harm to animal, plant and human health, thus, It is of great significance to establish a method for the determination of pesticide and antibiotic residues in environmental water samples. Magnetic graphene composite is a new type of adsorbent with great potential because of its convenient magnetic separation and high efficiency adsorption. In recent years, the applications in environment, food and biology have been reported. In this paper, magnetic graphene composites were prepared and used in magnetic solid phase extraction (MSPE) and combined with high performance liquid chromatography-tandem mass spectrometry (HPLC-MS). The residues of triazine herbicides and sulfonamides in environmental water samples were determined. The main contents of this paper include the following points: 1. The basic situation of pesticides and antibiotics and some common sample pretreatment techniques were introduced. The general situation and application of magnetic solid phase extraction (SPE) are described. The magnetic graphene oxide (GO-Fe _ 3O _ 4) was prepared by one-step synthesis method. It was used as a magnetic solid phase adsorbent to extract and enrich six triazine herbicides in environmental water. The synthesized materials were characterized by scanning electron microscope (SEM) and Fourier transform infrared spectroscopy (FTIR). In order to improve the extraction efficiency, the amount of GO-Fe3O4 and the extraction time were optimized. The detection limit of 6 kinds of triazine herbicides was 0.1 ~ 1.0 ng / L for pH, ion strength and desorption conditions, and the enrichment ratio could reach 616 ~ 902. The method was applied to the analysis of actual water samples such as Taihu Lake, canal water and moat water in Suzhou area, such as Taihu Lake, canal water and moat water. The recovery range was between 85.4% and 117.6%, and the relative standard deviation was 1.2% and 10.0. The method was simple and rapid, with high enrichment ratio and low detection limit. It can be used for the determination and analysis of trace triazine herbicide residues in water samples. The carboxylated magnetic graphene oxide material (CGO / Fe 3O 4) has been successfully synthesized and used as a magnetic solid phase adsorbent for the extraction of sulfanilamide antibiotics in environmental water samples. CGO / Fe _ 3O _ 4 was prepared by co-precipitation method, and the extraction efficiency of the method was evaluated by scanning electron microscope and Fourier transform infrared spectroscopy (FTIR). The CGO/Fe3O4 dosage, extraction time, pH of the sample solution, ion strength and desorption conditions were optimized to improve the extraction efficiency. The adsorption and extraction ability of sulfanilamide antibiotics by CGO/Fe3O4 and GO/Fe3O4 were compared. Under the optimum extraction conditions, a good linear range was obtained. The correlation coefficient is greater than 0.9983, the detection limit of the method is 0.49 ~ 1.59 ng / L, and the enrichment ratio is 1320 ~ 1702. The method has been applied to the analysis of waste water, river water and tap water in Suzhou area. The recoveries of the method are in the range of 83.2% and 109.2%. The relative standard deviation is 1.8 and 11.2. Because of its simple and rapid operation, high concentration ratio and low detection limit, this method can be used for the analysis of trace sulfanilamides residues in environmental water samples. The paper is summarized and the main conclusions of the experiments are summarized.
【学位授予单位】：苏州科技大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X832

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