广东省农耕土壤中TBBPA与HBCDs的含量、分布调查及蓄积水平估算

发布时间：2018-01-18 08:00

  本文关键词：广东省农耕土壤中TBBPA与HBCDs的含量、分布调查及蓄积水平估算　出处：《南方医科大学》2017年硕士论文　论文类型：学位论文

  更多相关文章： 高效液相色谱-质谱联用仪 四溴双酚A 六溴环十二烷 农耕土壤分布特征 广东省

【摘要】：研究背景和目的:四溴双酚A(Tetrabromobisphenol A,TBBPA)和六溴环十二烷(Hexabromocyclododecane,HBCDs)是目前使用量最大的有机阻燃剂,被广泛应用于工业生产,已有研究证明二者对人体健康具有神经毒性、发育毒性、内分泌毒性等影响,作为新型的持续性有机污染物被广泛关注,在空气、水、河底泥等自然介质中均有相关的检出报导,而土壤尤其是农业土壤中的研究相对较少.本研究旨在考查并建立土壤中TBBPA以及HBCDs的3种异构体(α-HBCD、β-HBCD、y-HBCD)的提取方法以及HPLC-MS-MS检测方法,并用该方法对广东省的农耕土壤进行检测,目的是探明广东省农耕土壤中两种阻燃剂的含量、分布、异构体的构成特征,并对广东省农耕土壤中TBBPA与HBCDs的蓄积情况进行评估,以期为两者的污染防治提供依据。研究方法:1.建立土壤中TBBPA以及HBCDs的3种异构体(α-HBCD、β-HBCD、γ-HBCD)的提取方法以及HPLC-MS-MS检测方法,并作方法学考查;2.广东省农耕土壤的采样;3.用HPLC-MS-MS对样品进行检测;4.用SPSS软件对检测结果进行统计分析。研究结果:1.建立了快速、简便、稳定的HPLC-MS-MS检测大批量土壤中的TBBPA和HBCDs的方法,TBBPA以及α-HBCD、β-HBCD、γ-HBCD的定量限分别为0.01、0.02、0.01、0.03 pg·g-1dw,回收率均在 85%～115%之间;2.采集了粤北、粤东、粤西、珠三角地区6个市18个县的360份土壤样品;3.广东省农耕土壤中TBBPA与∑HBCDs(α、β、γ-HBCD之和)的含量范围分别为ND～7.43 ng·g-1dw 和 ND～3.84 ng·g-1dw,均值分别为 0.61 ng·g-1dw 和 0.68 ng·g-1dw;4.在采样涉及的6个市中,TBBPA平均含量高低顺序为佛山(0.91 ng·g-1dw)湛江(0.90 ng·g-1dw)汕头(0.82 ng·g-1dw)肇庆(0.44 ng·g-1dw)惠州(0.34 ng·g-1dw)韶关(0.24 ng·g-1dw),∑HBCDs 平均含量高低顺序为汕头(0.98 ng·g-1dw)惠州(0.97 ng·g-1dw)佛山(0.77 ng·g-1dw)湛江(0.72 ng·g-1dw)肇庆(0.35 ng·g-1dw)韶关(0.28 ng·g-1dw);各采样市之间的农耕土壤中TBBPA浓度和HBCDs浓度均有显著的地区差异(方差分析,P0.001),工业和经济更发达的珠三角地区农耕土壤中的TBBPA与HBCDs浓度明显高于粤北山区;当地阻燃剂使用相关工业年产值与∑HBCDs在农耕土壤中的污染浓度均有强相关性(P =0.021,Spearman 相关系数=0.829);5.广东省农耕土壤中α、β、γ-HBCD的平均丰度分别为36.1%、9.0%、54.9%,与工业产品中三者的比例有所不同,说明HBCDs在环境蓄积过程中发生了转化与重排;6.广东省农耕土壤中的TBBPA蓄积量为4.57 t,HBCDs的蓄积量为5.10 t,说明该两种化合物在广东省农耕土壤中已经达到一定程度的蓄积。研究结论:1.广东省农耕土壤中广泛检出TBBPA和HBCDs,且二者的浓度要高于工业不发达地区,但蓄积量还未达到PBDEs的程度;2.TBBPA与HBCDs的分布有明显的地区差异,且HBCDs的浓度与阻燃剂相关工业的年产值有正相关性;3.HBCDs的三种异构体在环境中会发生转化。
[Abstract]:Background and objective: Tetrabromobisphenol A. TBBPA) and Hexabromocyclododecane (HBCDs) are the most widely used organic flame retardants, which are widely used in industrial production. It has been proved that both have neurotoxicity, developmental toxicity, endocrine toxicity and other effects on human health. As a new type of persistent organic pollutants, they are widely concerned in air and water. There are related reports of detection in natural media such as river bottom mud. The purpose of this study was to investigate and establish three isomers of TBBPA and HBCDs (伪 -HBCD, 尾 -HBCD) in soil, especially in agricultural soil. The extraction method and HPLC-MS-MS detection method of y-HBCD were used to detect the content of two kinds of flame retardants in agricultural soil of Guangdong province. Distribution, composition of isomers, and the accumulation of TBBPA and HBCDs in agricultural soils of Guangdong Province were evaluated. Methods: 1. To establish three isomers of TBBPA and HBCDs (伪 -HBCD, 尾 -HBCD) in soil. The extraction method and HPLC-MS-MS detection method of 纬 -HBCD, and the methodological examination; 2. Sampling of agricultural soil in Guangdong Province; 3. HPLC-MS-MS was used to detect the samples. 4. The test results were analyzed by SPSS software. The result of the study was: 1.The rapid and simple method was established. Stable HPLC-MS-MS was used to detect TBBPA and HBCDs in large quantities of soil, and 伪 -HBCD, 尾 -HBCD. The quantitative limit of 纬 -HBCD was 0.01g 路g-1dw. the recoveries of 纬 -HBCD were between 85% and 115%. 2. 360 soil samples were collected from 18 counties of 6 cities in northern Guangdong, eastern Guangdong, western Guangdong and Pearl River Delta. 3. TBBPA and 鈭，

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