几种农药的表面分子印迹聚合物的合成和表征及其在化学发光技术中的应用

发布时间：2018-12-09 18:25

【摘要】：随着工农业的迅速发展,人们向环境排放的污染物也越来越多,超出了其自净能力,其中在农业中过度使用农药造成的环境污染不容忽视。这些有毒有害的有机物流入河流,会使我们赖以生存的水体受到污染,危害人们的身体健康。目前,水污染治理已经迫在眉睫,但水体中污染物含量低且成分复杂,需要建立一种对目标分子分离富集的简便的样品预处理方法,消除干扰杂质的影响,便于后续检测。分子印迹技术(MIT)是通过合成对目标物有特异选择性和亲和力的聚合物,从而进行分离和富集的一种分子识别技术。MIT具有成本低、操作简单、特异选择性高、物理化学性质稳定和寿命长等优点,目前已被广泛应用于诸多领域,如食品安全、药物分析、环境科学及临床医学等。MIT与选择性差的化学发光分析联用,其在线检测复杂样品具有消除干扰、响应速度快、灵敏度高、重现性好等优点。本文主要从事以下研究工作:1、采用表面分子印迹技术、以氧化石墨烯为载体,坐果安为模板分子,通过聚合反应制备坐果安表面分子印迹聚合物(CMIP),同时作为对比实验,制备了空白分子印迹聚合物(CNIP),通过扫描电镜对坐果安表面分子印迹聚合物的结构和形貌进行表征;考察溶液的pH、吸附时间、温度和坐果安的初始浓度等对CMIP吸附模板分子的影响;也对CMIP进行了吸附动力学、吸附热力学研究及选择性和循环使用情况研究。实验表明CMIP对坐果安分子有良好的选择吸附性能,可应用于检测样品中坐果安农药的前处理。2、以氧化石墨烯为载体,采用表面分子印迹的方法合成烟嘧磺隆分子印迹聚合物(NSMIP),通过表征及一系列的实验表明NSMIP对烟嘧磺隆有选择吸附性,其吸附容量可达108.24 mg/g。因此NSMIP可用于对烟嘧磺隆的分离与富集。3、以灭蝇胺为模板分子,氧化石墨烯为载体,采用表面分子印迹方法制备灭蝇胺分子印迹聚合物(CYMIP),将其与灵敏度高且重现性好的化学发光法结合,组成分子印迹-流动注射化学发光联用的分析方法可以即选择性识别灭蝇胺又能对灭蝇胺进行高灵敏的测定,此方法可以应用于检测河水中的灭蝇胺,并取得满意结果。本文利用表面分子印迹技术,解决了农药残留分析中由于生物样品基质复杂而干扰检测的问题,有效的分离和富集目标分子,为检测提供了一个操作简便,成本低的前处理方法。而分子印迹-流动注射化学发光联用技术则用分子印迹技术弥补了化学发光分析方法的缺点,增加了灵敏度、使线性范围变宽、选择性更好。
[Abstract]:With the rapid development of industry and agriculture, people discharge more and more pollutants to the environment, which exceeds their self-purification ability, and the environmental pollution caused by excessive use of pesticides in agriculture can not be ignored. These toxic and harmful organic matter flowing into the river will pollute the water we depend on and endanger people's health. At present, water pollution treatment is urgent, but the pollutant content in water is low and the composition is complex. It is necessary to establish a simple sample pretreatment method to separate and enrich the target molecule, to eliminate the influence of interference impurities, and to facilitate the subsequent detection. Molecular imprinting technique (MIT) is a molecular recognition technique for separation and enrichment by synthesizing polymers with specific selectivity and affinity to the target. MIT has the advantages of low cost, simple operation and high selectivity. Physical and chemical properties such as stability and long life have been widely used in many fields, such as food safety, drug analysis, environmental science and clinical medicine, etc. MIT is combined with chemiluminescence analysis with poor selectivity. The on-line detection of complex samples has the advantages of eliminating interference, fast response, high sensitivity and good reproducibility. The main work of this paper is as follows: 1. Surface molecularly imprinted polymer (CMIP),) was prepared by polymerization with graphene oxide as the carrier and scion as template molecule. At the same time, the structure and morphology of the molecularly imprinted polymer were characterized by scanning electron microscope (SEM). The effects of pH, adsorption time, temperature and initial concentration on the adsorption of CMIP template molecules were investigated, and the adsorption kinetics, adsorption thermodynamics, selectivity and recycling of CMIP were also studied. The experimental results show that CMIP has a good selective adsorption property for the seed-fruit amine molecule, and can be used in the pre-treatment of the pesticide in the sample. 2. The graphene oxide is used as the carrier. Surface Molecular imprinting Synthesis of Nicosulfuron Molecular imprinted Polymer (NSMIP), by characterization and a series of experiments show that NSMIP has selective adsorption ability for niposulfuron, and its adsorption capacity can be up to 108.24 mg/g.. Therefore, NSMIP can be used for the separation and enrichment of niosulfuron. 3The imprinted polymer (CYMIP), was prepared by surface molecular imprinting method using methomide as template molecule, graphene oxide as carrier and surface molecular imprinting method. By combining it with chemiluminescence method with high sensitivity and reproducibility, the method of molecular imprinting and flow injection chemiluminescence analysis can not only selectively recognize methylamine, but also can be used for the highly sensitive determination of methomidamine. The method can be applied to the detection of fly amine in river water with satisfactory results. In this paper, the surface molecular imprinting technique is used to solve the problem of interference detection in pesticide residue analysis due to the complex matrix of biological samples. The target molecules are effectively separated and enriched, which provides a simple and convenient operation for the detection. Low cost pretreatment. The combination of molecular imprinting and flow injection chemiluminescence makes up the shortcoming of chemiluminescence analysis, increases the sensitivity, broadens the linear range and improves the selectivity.
【学位授予单位】：西华师范大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O631.3;O657.3

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