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题名: 短链和中链氯化石蜡的人体外暴露水平研究
作者: 黄慧婷1
学位类别: 硕士
答辩日期: 2017-05
授予单位: 中国科学院大学
授予地点: 北京
导师: 高丽荣
关键词: 短链氯化石蜡,中链氯化石蜡,大气颗粒物,鱼,肉和肉制品 ; Short-chain chlorinated paraffins, Medium-chain chlorinated paraffins,Airborne particulate matter, Fish, Meat and meat product
其他题名: Human Exposure to Short- and Medium-Chain Chlorinated Paraffins in China
学位专业: 分析化学
中文摘要: 氯化石蜡(CPs)是一类正构烷烃的氯代衍生物,其中短链氯化石蜡(SCCPs, C10-13)具有持久性、高毒性、生物蓄积性和长距离迁移性。2017年 5月 SCCPs 已经被列入《关于持久性有机污染物的斯德哥尔摩公约》的受控名单,被国际 社会广泛关注。美国、加拿大、日本和欧盟等国家或组织已经制定相关的政策 法规限制 SCCPs的生产、使用和排放,目前我国还没有相关的政策和法规。我 国是 CPs最大的生产国和出口国,在生产和使用过程中 CPs会释放到环境中, CPs长期暴露必然会引起生态风险,因此开展我国环境介质和生物样品中 CPs 的存量研究和人体健康风险评估非常有必要。非职业的人群 CPs暴露的主要途 径是膳食摄入和呼吸摄入,然而当前我国的相关研究很少,因此,本文重点开 展食物和呼吸相关的人体暴露水平研究。本文采用全二维气相色谱-电子捕获负 化学源-飞行时间质谱的分析方法(GC×GC-ECNI-TOFMS)测定了北京大气颗 粒物、鱼和肉类样品中 SCCPs和中链氯化石蜡(MCCPs)的含量水平、污染特 征及其人体暴露水平,得到以下结论: 1.本研究在北京市某一采样点的室外和室内共收集了 30个颗粒物(PM) 样品,研究了 PM10/PM2.5/PM1.0上 SCCPs和 MCCPs的浓度和分布,并初步评 估了它们的呼吸暴露风险。研究结果发现,室外 PM10上 SCCPs和 MCCPs浓度 的平均值分别为 23.9 ng m−3和 3.6 ng m−3,室内 PM10上 SCCPs和 MCCPs浓度 的平均值分别为 61.1 ng m−3和 6.9 ng m-3。与文献中报道的水平比较,本研究中 的 SCCPs和 MCCPs含量相对较高。室内 PM10/PM2.5/PM1.0样品中 SCCPs和 MCCPs的浓度比室外的相应值均高,原因可能是室内一些含 CPs产品的使用, 例如油漆、涂料、皮革和橡胶产品等。在室外和室内空气颗粒物中 SCCPs和 MCCPs主要分布在粒径小于 2.5 μm的颗粒物上。SCCPs和 MCCPs主要的同系 物是 C10-11Cl7-8。根据工业品 CP-42、CP-52和 CP-70中 SCCPs的同系物分布特 征,推测室外和室内 PM样品中 SCCPs可能主要来自 CP-42和 CP-52的生产和 使用。室外和室内暴露边界值( MOEs)远大于不确定性因子(1000),因此 SCCPs并未给人类健康带来明显的健康风险。 2.本研究探索了辽东湾地区不同种类鱼体中 SCCPs和 MCCPs的污染水 平、同系物分布及其生物蓄积情况。SCCPs和 MCCPs浓度范围分别为 376.3–8596 ng g−1 lw和 22.4–5097 ng g−1 lw。ΣSCCPs的生物累积因子的对数值 范围为 4.69–6.05,表明 SCCPs在鱼体内发生了生物蓄积。SCCPs的营养级放 大系数是 2.57,表明 SCCPs在鱼体内发生了生物放大。SCCPs和 MCCPs的碳 链长度、氯原子个数和辛醇/水分配系数(Kow)可能是影响它们在鱼体内生物 累积的重要因素。食用含 SCCPs的鱼体给人类健康带来较低风险。 3.本研究首次调查了我国20个省份的肉和肉制品样品中SCCPs和MCCPs 的含量水平和地理分布情况,并评估我国非职业人群食用肉和肉制品而摄入的 SCCPs和 MCCPs含量。采样点覆盖了我国人口的三分之二,该肉类样品非常 具有代表性,能够真实地反映我国肉类产品中 CPs污染状况。肉类样品中 SCCPs 和 MCCPs的平均浓度分别为 129 ng g−1 ww和 5.7 ng g−1 ww。不同省份样品中 SCCPs和 MCCPs的浓度差别较大。CPs浓度的地理分布与我国 CPs生产工厂 的分布具有一致性。所有样品中 SCCPs主要的同系物为 C10-11Cl6-7,MCCPs主 要的同系物为 C14Cl7-8。我国标准的成年男性食用肉类食物每日 SCCPs和 MCCPs摄入量的中位值分别是 0.13 μg kg−1 bw day−1和 4.7 × 10−3 μg kg-1 bw day−1,远低于可容忍的每日摄入量( TDIs)。食用肉类食物而摄入的 SCCPs 和 MCCPs不会给人类健康带来显著的风险。
英文摘要: Chlorinated paraffins (CPs) are very complex mixtures of chlorinated derivatives of n-alkanes. The short-chain chlorinated paraffins (SCCPs, C10–13) are persistent, have adverse health effects, and can bioaccumulate and undergo long-range transport. Therefore, CPs have been listed as persistent organic pollutants under the Stockholm Convention and are of concern to the international community. CPs are released to the environment during their production and use, and the United States, Canada, Japan, and the European Union have established policies and regulations to limit their production, use, and emission. However, there are no regulations limiting the use of SCCPs in China, which is the largest producer and exporter of CPs in the world. Because long-term exposure to CPs will inevitably lead to a degree of ecological risk, research on the levels of CPs in various environmental matrixes and biological samples is very important. In addition, human health risk assessments should be conducted. The main pathways of exposure to CPs for populations without occupational exposure are the diet and inhaled air. To date, there has been little research on these exposure routes in China. Therefore, this study focused on human exposure to these compounds via the diet and inhaled air. The concentrations of SCCPs and MCCPs in airborne particulate matter (PM), fish, and meat samples were measured using comprehensive two-dimensional gas chromatography electron capture negative ionization high-resolution time-of-flight mass spectrometry. The results were used to evaluate contamination levels and human exposure to SCCPs and MCCPs. The main aspects of this study are detailed below. 1. A total of 30 PM samples were collected outdoors and indoors at a sampling site in Beijing. These samples were used to investigate the concentrations and distributions of SCCPs and MCCPs in PM fractions with diameters less than 10 µm, 2.5 µm, and 1 µm (PM10, PM2.5, and PM1.0), and to evaluate inhalation exposure risks. The mean SCCP and MCCP concentrations in the outdoor PM10 fraction were 23.9 ng m–3 and 3.6 ng m–3, respectively. The mean indoor SCCP and MCCP concentrations were 61.1 ng m–3 and 6.9 ng m–3, respectively. Compared with literature data, the levels of SCCPs and MCCPs in the present study were relatively high. SCCP and MCCP concentrations in indoor PM10, PM2.5, and PM1.0 samples were higher than the corresponding outdoor values. This could be attributed to the use of some CP-containing products indoors, such as paints and coatings, leather, and rubber products. In both outdoor and indoor air, CPs were mainly associated with particles ≤ 2.5 μm in diameter. The main homolog groups for both SCCPs and MCCPs were C10–11Cl7–8. According to the congener distribution of CP-42, CP-52, and CP-70, it is assumed that SCCPs in the outdoor and indoor PM samples are mainly derived from the production and use of CP-42 and CP-52. In the present study, the margins of exposure in outdoor and indoor air were larger than the uncertainty factor (1,000). Consequensy, SCCPs might not be a significant risk to human health. 2. The levels, congener group profiles, bioaccumulation, and biomagnification of SCCPs and MCCPs in ten species of fish from Liaodong Bay, North China were investigated. The ranges for the SCCP and MCCP concentrations were 376.3–8596 ng g–1 lipid weight and 22.4–5097 ng g–1 lipid weight, respectively. The logarithms of the bioaccumulation factors for the ΣSCCPs ranged from 4.69 to 6.05, implying that SCCPs bioaccumulated in the fish. The trophic magnification factor of SCCPs was 2.57, indicating that SCCPs could biomagnify in fish. Carbon chain length, the numbers of chlorine atoms, and octanol/water partition coefficients (Kow) of the SCCPs and MCCPs might be important factors affecting the bioaccumulation of these chemicals in fish. The risk posed to human health by consumption of fish containing SCCPs is low. 3. In the present study, for the first time a nation-wide survey will be carried out to investigate the levels and national geographical distribution of SCCPs and MCCPs in meat samples from 20 Chinese provinces in 2011. These samples were used to assess the dietary exposures for the general population to SCCPs and MCCPs. The sampling sites covered about two-thirds of the population, and the meat samples were representative of available meat products. The mean SCCP and MCCP concentrations in all meat samples were 129 ng g–1 wet weight and 5.7 ng g–1 wet weight, respectively. The contents of SCCPs and MCCPs in samples from different provinces varied, and the geographical distribution of CP concentrations was consistent with the distribution of CP manufacturing plants in China. The most abundant groups of SCCPs in all samples were C10–11Cl6–7, and the most abundant groups of MCCPs in most samples were C14Cl7–8. The median values of daily intakes of SCCPs and MCCPs through meat consumption for a ―standard‖ Chinese adult male were 0.13 μg kg–1 bw d–1 and 4.7 × 10–3 μg kg–1 bw d–1, respectively, and much lower than the tolerable daily intakes for SCCPs and MCCPs. Indirect exposure to SCCPs and MCCPs through meat consumption might not be a significant risk to human health in China.
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/38635
Appears in Collections:环境化学与生态毒理学国家重点实验室_学位论文

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作者单位: 1.中国科学院生态环境研究中心

Recommended Citation:
黄慧婷. 短链和中链氯化石蜡的人体外暴露水平研究[D]. 北京. 中国科学院大学. 2017.
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