持久性有机卤素化合物对生产源区人体暴露影响的研究
发布时间:2018-10-26 11:20
【摘要】:持久性有机卤素化合物(Persistent halogenated organic compounds)所引起的环境污染问题已经受到全球的广泛关注。本研究中探讨的有机卤素化合物是多溴联苯醚(PBDEs)、多氯联苯(PCBs)、有机氯农药(OCPs)、德克隆(DP)、五溴苯(PBBz)和五溴甲苯(PBT)这几类曾经大量使用或者正在使用的化合物。由于PCBs和OCPs的环境持久性与生物毒性已被陆续发现,目前这些物质已在全球或部分地区禁止生产或使用。PBDEs因其优越的阻燃性能而被大量用作阻燃剂,但由于其具有环境持久性和潜在生物毒性,目前全球范围内已禁止生产和使用五溴联苯醚和八溴联苯醚,欧盟及美国部分地区也已开始禁止十溴联苯醚的生产和使用。DP作为灭蚁灵和BDE-209的替代品已经在部分国家开始生产和使用,但目前关于其毒性的研究较少。目前关于PBBz和PBT的生产现状与毒性作用均缺乏具体的数据与研究。近年来,关于这些持久性有机卤素化合物对人体暴露的影响引起了公众的广泛关注。本研究测定了溴代阻燃剂生产源区山东潍坊地区大气样本中PCBs、 OCPs、PBDEs、DP、PBBz和PBT的浓度分别为1.7 pg/m3、330 pg/m3、140000 pg/m3、1.4 pg/m3、100 pg/m3和250 pg/m3。其中,PBDEs是潍坊地区大气样本中最主要的有机卤素化合物,其含量高出其他有机卤素化合物含量三个数量级,与其他国家和地区相比,潍坊地区大气中PBDEs水平较高。新型有机卤素化合物DP、PBBz和PBT在潍坊地区大气样本中的检出率为100%,表明新型有机卤素化合物污染的普遍性。同时,本研究测定了潍坊地区混合人血清样本中PCBs、OCPs、PBDEs. DP、PBBz和PBT的含量。其中,OCPs和PBDEs为两种主要的有机卤素化合物,其含量平均值分别为1500 ng/g lipid和240 ng/g lipid。DP、PBT和PBBz在所有混合血清样本中均有检出率,其含量平均值分别为3.6 ng/g lipid, 4.9 ng/g lipid和1.4 ng/g lipid。各有机卤素化合物在不同年龄段混合血清样本中的暴露水平不同,其暴露趋势与各有机卤素化合物的生产使用历史有关。此外,本研究发现,潍坊地区混合血清样本与潍坊地区大气气相样本、大气颗粒相样本及大气总(气相±颗粒相)样本中各有机卤素化合物含量均呈显著正相关关系(r0,p0.01),表明呼吸是生产源区居民摄入PCBs、OCPs、 PBDEs、DP、PBBz和PBT的重要途径。此外,本研究测定了生产源区山东潍坊地区和对照区广西南宁地区的单个血清样本中PCBs、PBDEs和DP的水平。结果显示,潍坊地区单个血清样本中的各物质的含量均高于南宁地区相应物质的水平。本研究同时检测了两个地区血清样本中的5项甲状腺指标,在此基础上,分别研究了两个地区各有机卤素化合物对甲状腺指标的影响。多元线性回归的分析结果显示:潍坊地区单个血清样本中T3的水平受∑DP和BDE-99浓度的影响,fT3的水平受anti-DP浓度的影响,T4的水平受ΣDL-PCBs浓度的影响,fT4与TSH的水平未显示出与所检测的各有机卤素化合物浓度具有关联性;南宁地区单个血清样本中T3的水平受BDE-153和Σ10PBDEs浓度的影响,fT3的水平受PCB-118和PCB-170浓度的影响,T4的水平受PCB-156浓度的影响,TSH的水平受Σ10PBDEs浓度的影响。潍坊地区和南宁地区单个血清样本中各有机卤素化合物和甲状腺指标间均存在着不同的关联性,即各有机卤素化合物对潍坊地区和南宁地区单个血清样本中甲状腺指标的影响不同,这种差异可能是由于两个地区人群的自身特征及暴露水平不同造成的。
[Abstract]:The environmental pollution caused by persistent organic halogen compounds has attracted worldwide attention. The organic halogen compounds discussed in this study are polybrominated diphenyl ethers (PBDEs), PCBs (PCBs), organochlorine pesticides (OCPs), German clones (DP), pentabromoene (PBBZ) and pentabromotoluene (PBT), which have been used in large quantities or are in use. Because of the environmental persistence and biotoxicity of PCBs and OCPs, these substances have been banned from production or use in the global or partial regions. PBDEs are widely used as flame retardants due to their superior flame retardant properties, but because of their environmental durability and potential biotoxicity, the production and use of pentaBDE and ocbrominated diphenyl ethers worldwide have been banned worldwide, The EU and some parts of the United States have also begun to ban the production and use of decaBDE. The DP, which is a substitute for mirex and BDE-209, has been produced and used in some countries, but there are few studies on its toxicity. At present, the production status and toxicity of PBBz and PBT are lack of specific data and research. In recent years, the effects of these persistent organic halogen compounds on human exposure have caused widespread public concern. In this study, the concentrations of PCBs, OCPs, PBDEs, DP, PBBz and PBT in the atmosphere samples from the production source area of Bromine fire retardant were 1. 7 pg/ m 3, 330 pg/ m 3, 140000 pg/ m 3, 1. 4 pg/ m 3, 100 pg/ m3 and 250 pg/ m 3, respectively. Among them, PBDEs are the most important organic halogen compounds in the atmospheric samples of the Songhua area, and the content of PBDEs is three orders of magnitude higher than that of other organic halogen compounds, and the PBDEs in the atmosphere are higher than those in other countries and regions. The detection rate of the novel organic halogen compounds DP, PBBz and PBT in the atmospheric samples in the Daya Bay area was 100%, indicating the universality of the new organic halogen compound pollution. At the same time, PCBs, OCPs, PBDEs in serum samples of mixed human serum were determined in this study. DP, PBBz and PBT. Among them, OCPs and PBDEs were two major organic halogen compounds with an average content of 1500 ng/ g lipoid and 240 ng/ g lipoid. DP, PBT and PBBz had detectable rates in all mixed serum samples with an average content of 3.6 ng/ g lipoid, 4.9ng/ g lipoid and 1. 4 ng/ g lipoid, respectively. The exposure levels of organic halogen compounds in mixed serum samples at different age groups were different, and their exposure trends were related to the history of production use of organic halogen compounds. in addition, that content of organic halogen compounds in the sample of mixed serum and atmospheric gas phase, atmospheric particle phase and total atmospheric gas phase (gas phase) were significantly positive correlation (r0, log10. 01). It is shown that breathing is an important way for the residents to take PCBs, OCPs, PBDEs, DP, PBBz and PBT. In addition, the levels of PCBs, PBDEs and DP were measured in the single serum samples in the area of the production source and in the Nanning area in the control area. The results showed that the contents of each substance in a single serum sample of the Han nationality region were higher than that of the corresponding substances in the Southern Ningxia region. In this study, five thyroid indexes in serum samples of two regions were tested, and the effects of organic halogen compounds on thyroid indexes were studied. The results of multivariate linear regression showed that the level of T3 in a single serum sample was affected by the concentration of CDDP and BDE-99, the level of fT3 was affected by the anti-DP concentration, and the level of T4 was affected by the concentration of DPDLs-PCBs. The level of fT4 and TSH did not show an association with the detected concentrations of organic halogen compounds; levels of T3 in a single serum sample in the Southern Ningxia region were affected by the concentrations of BDE-153 and F10PBDEs, the level of fT3 was affected by PCB-118 and PCB-170 concentrations, T4 levels were affected by PCB-156 concentrations, The level of TSH was affected by the concentration of palbociclib 10PBDEs. There is a different correlation between the organic halogen compounds and the thyroid indexes in the individual serum samples in the Southern and Southern Ningxia regions, that is, the effect of each organic halogen compound on the thyroid index in the individual serum samples in the Southern and Southern Ningxia regions is different. This difference may be due to the differences in their own characteristics and exposure levels in both regions.
【学位授予单位】:中央民族大学
【学位级别】:硕士
【学位授予年份】:2015
【分类号】:X592
本文编号:2295552
[Abstract]:The environmental pollution caused by persistent organic halogen compounds has attracted worldwide attention. The organic halogen compounds discussed in this study are polybrominated diphenyl ethers (PBDEs), PCBs (PCBs), organochlorine pesticides (OCPs), German clones (DP), pentabromoene (PBBZ) and pentabromotoluene (PBT), which have been used in large quantities or are in use. Because of the environmental persistence and biotoxicity of PCBs and OCPs, these substances have been banned from production or use in the global or partial regions. PBDEs are widely used as flame retardants due to their superior flame retardant properties, but because of their environmental durability and potential biotoxicity, the production and use of pentaBDE and ocbrominated diphenyl ethers worldwide have been banned worldwide, The EU and some parts of the United States have also begun to ban the production and use of decaBDE. The DP, which is a substitute for mirex and BDE-209, has been produced and used in some countries, but there are few studies on its toxicity. At present, the production status and toxicity of PBBz and PBT are lack of specific data and research. In recent years, the effects of these persistent organic halogen compounds on human exposure have caused widespread public concern. In this study, the concentrations of PCBs, OCPs, PBDEs, DP, PBBz and PBT in the atmosphere samples from the production source area of Bromine fire retardant were 1. 7 pg/ m 3, 330 pg/ m 3, 140000 pg/ m 3, 1. 4 pg/ m 3, 100 pg/ m3 and 250 pg/ m 3, respectively. Among them, PBDEs are the most important organic halogen compounds in the atmospheric samples of the Songhua area, and the content of PBDEs is three orders of magnitude higher than that of other organic halogen compounds, and the PBDEs in the atmosphere are higher than those in other countries and regions. The detection rate of the novel organic halogen compounds DP, PBBz and PBT in the atmospheric samples in the Daya Bay area was 100%, indicating the universality of the new organic halogen compound pollution. At the same time, PCBs, OCPs, PBDEs in serum samples of mixed human serum were determined in this study. DP, PBBz and PBT. Among them, OCPs and PBDEs were two major organic halogen compounds with an average content of 1500 ng/ g lipoid and 240 ng/ g lipoid. DP, PBT and PBBz had detectable rates in all mixed serum samples with an average content of 3.6 ng/ g lipoid, 4.9ng/ g lipoid and 1. 4 ng/ g lipoid, respectively. The exposure levels of organic halogen compounds in mixed serum samples at different age groups were different, and their exposure trends were related to the history of production use of organic halogen compounds. in addition, that content of organic halogen compounds in the sample of mixed serum and atmospheric gas phase, atmospheric particle phase and total atmospheric gas phase (gas phase) were significantly positive correlation (r0, log10. 01). It is shown that breathing is an important way for the residents to take PCBs, OCPs, PBDEs, DP, PBBz and PBT. In addition, the levels of PCBs, PBDEs and DP were measured in the single serum samples in the area of the production source and in the Nanning area in the control area. The results showed that the contents of each substance in a single serum sample of the Han nationality region were higher than that of the corresponding substances in the Southern Ningxia region. In this study, five thyroid indexes in serum samples of two regions were tested, and the effects of organic halogen compounds on thyroid indexes were studied. The results of multivariate linear regression showed that the level of T3 in a single serum sample was affected by the concentration of CDDP and BDE-99, the level of fT3 was affected by the anti-DP concentration, and the level of T4 was affected by the concentration of DPDLs-PCBs. The level of fT4 and TSH did not show an association with the detected concentrations of organic halogen compounds; levels of T3 in a single serum sample in the Southern Ningxia region were affected by the concentrations of BDE-153 and F10PBDEs, the level of fT3 was affected by PCB-118 and PCB-170 concentrations, T4 levels were affected by PCB-156 concentrations, The level of TSH was affected by the concentration of palbociclib 10PBDEs. There is a different correlation between the organic halogen compounds and the thyroid indexes in the individual serum samples in the Southern and Southern Ningxia regions, that is, the effect of each organic halogen compound on the thyroid index in the individual serum samples in the Southern and Southern Ningxia regions is different. This difference may be due to the differences in their own characteristics and exposure levels in both regions.
【学位授予单位】:中央民族大学
【学位级别】:硕士
【学位授予年份】:2015
【分类号】:X592
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