高效液相色谱—串联质谱法测定蜂蜜中20种全氟烷基化合物

发布时间：2018-03-03 15:20

  本文选题：蜂蜜　切入点：全氟烷基化合物　出处：《山东农业大学》2017年硕士论文　论文类型：学位论文

【摘要】：全氟烷基化合物(Perfluorinated alkyl substances,PFASs)是人工合成的一类新型持久性有机污染物,由亲水基末端和不同长度的疏水烷基碳链组成的,疏水烷基碳链上的氢原子全部被氟原子替代,形成含有极高化学能的C-F键(约为110 kcal/mol),其稳定性极强,具有化学惰性和耐热性等优良性能。在20世纪50年代就广泛被用作杀虫剂、表面活性剂、润滑剂、催化剂、以及合成药物、氟橡胶、树脂的中间体。PFASs难以被新陈代谢、水解、光解、生物降解,在生物体内随着时间的推移可不断富集,PFASs在生物体内的蓄积浓度远高于已知的二VA英和有机氯等持久性环境污染物。大量研究发现,全氟辛酸(PFOA)与全氟辛烷磺酸(PFOS)具有生殖毒性、心血管毒性、肝脏毒性、甲状腺毒性和神经毒性。目前,国内外学者相继在水产品、动物肝脏、蛋、奶、母乳中检测出了PFASs,而通过膳食摄入PFASs已成为人体内PFASs的来源之一。本文采用高效液相色谱-串联质谱技术结合QuEChERS方法对蜂蜜中的PFASs残留检测方法进行了研究。主要研究内容如下:采用高效液相色谱-串联质谱(HPLC-MS/MS)技术结合改进QuEChERS预处理方法建立了同时蜂蜜中20种全氟烷基化合物(全氟丁酸、全氟戊酸、全氟丁烷磺酸、全氟己酸、全氟戊烷磺酸钠、全氟庚酸、全氟己烷磺酸、全氟庚烷磺酸钠、全氟辛酸、全氟辛烷磺酸钠、全氟壬酸、全氟壬烷磺酸钠、全氟癸酸、全氟癸烷磺酸钠、全氟十一烷酸、全氟十二烷酸、全氟十三烷酸、全氟十四烷酸、全氟十六烷酸、全氟十八烷酸)的残留检测方法。称取5.0 g蜂蜜样品于50 mL聚丙烯(PP)离心管中,加入5μL 2μg/mL混合内标标准溶液和5 m L水,然后加入10 mL含1.5%甲酸(v/v)的乙腈,漩涡1 min后,加入1 g氯化钠和4 g无水硫酸镁,振摇10 min后,以10000 r/min离心10 min。取上层乙腈7 mL转移到装有40 mg PSA、80 mg C18和900mg无水MgSO4的15 mL离心管中,振摇10 min后,以10000 r/min离心10 min,最后取4 m L(相当于2 g试样提取液)上清液于玻璃氮吹管中,40℃水浴氮吹至干,以1 mL甲醇定容后,过0.22μm滤膜,HPLC-MS/MS分析。Atlantis T3 C18色谱柱分离,以含5 mmol/L乙酸铵的甲醇溶液和5 mmol/L乙酸铵溶液溶液为流动相进行梯度洗脱。电喷雾离子(ESI)源负离子模式下以多反应监测(MRM)扫描,采用同位素内标法进行定量分析。实验结果表明,20种PFASs在0.2~10μg/L浓度范围内线性相关系数均大于0.995;检出限范围为0.04~0.1μg/kg;定量限范围为0.1~0.2μg/kg。在0.1、0.5、1和2μg/kg添加浓度下(n=6),20种PFASs加标回收率范围为72.56%~112.98%,相对标准偏差(RSD)范围为0.73%~15.73%。结果表明,该方法快速、高效、准确,适用于蜂蜜样品中20种PFASs的同时分析检测。
[Abstract]:Perfluorinated alkyl substrates (PFASs) are a new class of synthetic persistent organic pollutants, which are composed of hydrophilic end groups and hydrophobic alkyl carbon chains of different lengths. All hydrogen atoms in hydrophobic alkyl carbon chains are replaced by fluorine atoms. Forming C-F bonds with extremely high chemical energy (about 110kcal / mol / mol) with excellent stability, chemical inertia and heat resistance. In 1950s, C-F bonds were widely used as insecticides, surfactants, lubricants, catalysts, etc. And the intermediates of synthetic drugs, fluorocarbons, resins. PFASs are difficult to metabolize, hydrolyze, photolysis, biodegrade, The accumulation of PFASs in organisms over time is much higher than that of known persistent environmental pollutants such as diVA and organochlorine. Perfluorooctanoic acid (PFOAA) and perfluorooctane sulfonate (PFOS) have reproductive toxicity, cardiovascular toxicity, liver toxicity, thyroid toxicity and neurotoxicity. PFASs were detected in breast milk, and dietary PFASs intake has become one of the sources of PFASs in human body. In this paper, the detection of PFASs residues in honey by high performance liquid chromatography-tandem mass spectrometry (HPLC / MS) combined with QuEChERS method was studied. The main contents are as follows: 20 perfluoroalkyl compounds (perfluorobutyric acid, perfluorobutyric acid, perfluorobutyric acid, perfluorobutyric acid, perfluorobutyric acid, perfluorobutyric acid, perfluorobutyric acid) in simultaneous honey were. Perfluoropentanoic acid, perfluorobutane sulfonic acid, perfluorohexanoic acid, perfluoropentane sulfonate, perfluoroheptanesulfonate, perfluorooctanesulfonate, perfluorooctanesulfonate, perfluorononane sulfonate, perfluorovaleric acid, perfluorononane sulfonate, perfluorodecanoic acid, perfluoroheptanesulfonate, perfluorooctanesulfonate. Perfluorodecane sulfonate, perfluorodecanoic acid, perfluorohexadecanoic acid, perfluorohexadecanoic acid, perfluorinated 13 alkanoic acid, perfluorinated 14 alkanoic acid, perfluorohexadecanoic acid, Determination of perfluoroalkanoic acid in 50 mL PP centrifuge tube with 5.0 g honey, 5 渭 L 2 渭 g / mL mixed internal standard solution and 5 mL water was added, then 10 mL acetonitrile containing 1.5% formic acid v / v) was added for 1 min. Adding 1 g sodium chloride and 4 g anhydrous magnesium sulfate, shaking for 10 min, centrifuging for 10 mins at 10000 r / min. The upper layer acetonitrile was transferred to 15 mL centrifuge tube containing 40 mg PSA-80 mg C18 and 900mg anhydrous MgSO4 for 10 min, and the upper acetonitrile was transferred to 15 mL centrifuge tube containing 40 mg PSA-80 mg C18 and 900mg anhydrous MgSO4. The supernatant of 4 mL (equivalent to 2 g sample extract) was centrifuged at 10000 r / min for 10 min. The supernatant was blown to dry in the glass nitrogen blowing tube at 40 鈩，

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