羧基化纳米碳球固相萃取分析水中痕量全氟类化合物

发布时间：2018-02-11 05:28

本文关键词： 羧基化纳米碳球固相萃取全氟类化合物液相色谱串联质谱仪　出处：《山东农业大学》2017年硕士论文　论文类型：学位论文

【摘要】：全氟化合物(Perfluorochemicals,PFCs)是一类持久存在于环境中的新型有机污染物。近年来,大量的研究显示,全氟化合物已被发现在食品、土壤、水、空气、接触材料等介质中。由于PFCs在环境的长久污染性和在生物体内的积累性,使其越来越受到人们的关注。由于近几年中国的氟化工行业的快速发展,在中国一些城市的饮用水污染现状均高于其他国家。所以在食品安全领域对水中痕量全氟类化合物的分析测定一直是研究的热点。在本研究中,使用了一种表面经羧基修饰过的新型功能化纳米碳球-羧基化纳米碳球(CNSs-COOH),使之作为固相萃取(SPE)吸附剂,联合液相色谱串联质谱仪(LC-MS/MS)建立了一种测定水中六种全氟类化合物的新方法,并对不同地方的实际水样品基质进行了检测分析,验证了该方法的实用性。本研究主要结果如下:1.通过对萃取条件(萃取时间、pH值)、解吸条件(解吸溶剂种类、解吸溶剂体积)、水样品的体积及羧基化纳米碳球的用量进行优化等条件优化,得到了最优实验条件为:400 mL pH=2的水样品,流速为6 mL/min,解吸溶剂为pH=10的丙酮7 m L,羧基化纳米碳球用量为300 mg。2.在最优实验参数下,建立的方法对于全氟癸酸(PFDA)、全氟壬酸(PFNA)、全氟辛酸(PFOA)、全氟庚酸(PFHpA)、全氟己烷磺酸(PFHxS)和全氟辛烷磺酸(PFOS)拥有0.01~1.20 ng L-1的低检出限,在0.5~200 ng L-1的线性范围内线性关系良好,相关系数(R2)为0.997~0.999,相对标准偏差介于3.70~8.80%。3.该方法被应用于桶装饮用水、自来水及池塘水样品的分析检测,在自来水样品中有PFHxS被检测出,在池塘水样品中有PFHxS和PFOS被检测出,而在桶装饮用水中6种全氟类化合物均未被检出。在100 ng L-1、50 ng L-1、10 ng L-1三个浓度下加标试验,回收率为82.2~109.7%。
[Abstract]:Perfluorochemical compounds (PFCs) are new organic pollutants that persist in the environment. In recent years, a large number of studies have shown that perfluorides have been found in food, soil, water, air, In contact materials and other mediums, PFCs has attracted more and more attention due to its long-term pollution in the environment and accumulation in organisms. Due to the rapid development of fluorine chemical industry in China in recent years, The status quo of drinking water pollution in some cities in China is higher than that in other countries. Therefore, the analysis and determination of trace perfluorides in water in the field of food safety has always been a hot topic. A new functionalized carbon nanospheres, CNSs-COOHN, modified by carboxyl group, was used as a solid phase extraction (SPE) adsorbent. A new method for the determination of six perfluorinated compounds in water was established by combined liquid chromatography tandem mass spectrometer (LC-MS / MS). The main results of this study are as follows: 1. The extraction conditions (extraction time and pH value), desorption conditions (kinds of desorption solvents) were determined. The desorption solvent volume, the volume of water sample and the amount of carboxylated carbon nanospheres were optimized. The optimal experimental conditions were obtained for water sample with 1: 400 mL pH=2. The flow rate is 6 mL / min, the desorption solvent is 7 mL of acetone of pH=10 and the amount of carboxylated carbon nanospheres is 300 mg 路2. Under the optimum experimental parameters, The established method has a low detection limit of 0.01 ~ 1.20 ng 路L ~ (-1) for PFDAA, PFNAA, PFOAA, PFHpAX, PFHxSand PFOS of perfluorooctanesulfonic acid, and a good linearity in the linear range of 0.5 ~ 200 ng 路L ~ (-1). The relative standard deviation was between 3.70 and 8.80. The method was applied to the analysis of bottled drinking water, tap water and pond water samples. PFHxS was detected in tap water samples and PFHxS and PFOS were detected in pond water samples. Six perfluorinated compounds were not detected in barrelled drinking water, and the recovery was 82.2% 109.7% at the concentration of 100 ng / L ~ (50) ng / L ~ (-1) and 10 ng / L ~ (10) ng 路L ~ (-1) ~ (-1).
【学位授予单位】：山东农业大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O658.2;X832

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