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二噁英类 POPs的环境污染特征及人体暴露研究
Alternative TitleEnvironmental Pollution Characteristics and Human Exposure to Dioxin-like POPs
韩莹
Subtype博士
Thesis Advisor刘文彬
2018-06
Degree Grantor中国科学院生态环境研究中心
Place of Conferral北京
Degree Name理学博士
Degree Discipline环境科学
Keyword气–固相分配,工业排放源,环境影响,食物暴露,人体健康 Gas-particle Partitioning, Industrial Emission Sources, Environmental Impact, Food Exposure, Human Health
Abstract

      二噁英(PCDD/Fs)和多氯联苯(PCBs)合并称为二噁英类持久性有机污染物 (POPs),是《关于持久性有机污染物的斯德哥尔摩公约》中控制的 POPs,因具有高毒性,难降解性,极易在环境中残留,并随着食物链逐级传递发生生物富集作用,对生态环境和人类产生潜在的风险。本论文开展了二噁英类 POPs的污染源排放-环境污染水平-对环境健康影响的系列研究。以生活垃圾焚烧和钢铁厂铁矿石烧结作为典型工业排放源,开展生活垃圾焚烧过程中PCDD/Fs及PCBs的气–固相分配特征研究,铁矿石烧结过程中 PCDD/Fs及  PCBs的排放水平及对周边环境的影响,基于青海湖周边土壤中 PCDD/Fs及PCBs的污染状况,进一步了解偏远地区 PCDD/Fs及  PCBs的污染水平,此外,还对典型食物及动物、人体血液中 PCDD/Fs及PCBs的浓度水平进行了探索。通过对实验结果的分析,得出以下结论:
1.开展了生活垃圾焚烧过程中二噁英类POPs的气-固相分配特征研究。PCDD/Fs和  PCBs在气相、颗粒相、冷凝水中的含量逐级递减。PCDD/Fs和二噁英类 PCBs(dl-PCBs)在烟气中的排放浓度分别为 0.75–15 ng/m3和0.18–28 ng/m3,在颗粒相中的含量分别为  0.14–8.1 ng/m3和0.041–1.3 ng/m3,与粒径大小呈负相关性。研究结果对于了解生活垃圾焚烧过程中PCDD/Fs及PCBs排放特征和发展相应减排措施提供数据支持。
2.开展了钢铁厂铁矿石烧结车间排放烟气及其周边土壤中二噁英类POPs的分布特征研究。烧结车间烟气中 PCDD/Fs的浓度范围为  0.25–1.53 ng/m3,PCBs(dl-PCBs)的浓度范围为 2.98–8.00(0.58–1.41)ng/m3。A、B、C钢铁厂周边土壤中 PCDD/Fs(dl-PCBs)的浓度分别为 0.068±0.047(0.0088–0.40)、0.12±0.10(0.0047–0.46)、0.05±0.086(0.0016–0.28)ng/g。随着与钢铁厂铁矿石烧结车间烟囱间距离的增加,土壤中 PCDD/Fs和  dl-PCBs的浓度整体呈下降趋势。位于下风向土壤中 PCDD/Fs和  dl-PCBs的浓度显著高于上风向土壤中 PCDD/Fs和  dl-PCBs浓度。当地居民中儿童的暴露风险高于成年人,但均在阈值以下。为进一步了解 PCDD/Fs及  PCBs的大气长距离运输,对环青海湖周边土壤中 PCDD/Fs及  PCBs的污染现状进行了调查,检测到 PCDD/Fs
浓度介于 0.0004–0.020 ng/g,dl-PCBs的浓度为0.0018–0.011  ng/g,低于城区土壤中 PCDD/Fs及PCBs浓度。
3.开展了江苏主要大闸蟹产区中大闸蟹二噁英类POPs的浓度水平研究。蟹肉中PCDD/Fs和 PCBs的平均浓度分别为0.0060±0.012  ng/g和 16.2±19.6ng/g。蟹黄(蟹膏)中 PCDD/Fs和  PCBs的平均浓度分别为0.042±0.041 ng/g和 6.61±2.79 ng/g。评估发现食用少量大闸蟹不会明显增加人体暴露二噁英类 POPs的风险。对蟹塘的物料平衡计算发现沉积物是大闸蟹中 PCDD/Fs和dl-PCBs的主要贡献者,沉积物中PCDD/Fs和dl-PCBs的总毒性当量是饲料输入的77倍,定期清理更换蟹塘中的底泥或者进行底泥修复是解决大闸蟹中二噁英类 POPs超标的主要措施。
4.开展了人类主要消耗的动物肉制品及动物血液(包括鸡、鸭、兔、猪、牛、羊、马、驴)中二噁英类 POPs的暴露水平研究,发现肉制品中PCDD/Fs的浓度范围为 0.00047–1.09 ng/g,dl-PCBs的浓度分别为0.014–0.17 ng/g。动物血液中 PCDD/Fs和  PCBs的平均毒性当量分别为  0.064和0.0035 ng/L。对肉制品的人体暴露估算结果发现,鸡肉的食用使得人体对 PCDD/Fs和  PCBs的年均总暴露量最大。
5.开展人体血液中二噁英类POPs暴露水平研究,发现居民体内  PCDD/Fs平均浓度是 0.35 ng/L,PCBs和dl-PCBs浓度分别为2.7 ng/L和 0.018 ng/L。任意年龄组女性体内 PCDD/Fs的平均浓度(0.31  ng/L)均高于男性(0.28 ng/L),并且发现 PCDD/Fs和PCBs随着年龄增长的生物累积效应,可能是老年人代谢速率低而使污染物在体内半衰期延长导致。在不同科室参与者的血液中发现骨科参与者血液中 PCDD/Fs的浓度水平(0.95 ng/L)高于其他样品组。

Other Abstract

      Polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) and polychlorinated  biphenyls  (PCBs)   are  classified  as  dioxin-like   persistent  organic pollutants (POPs),  controlled by the  Stockholm Convention  on POPs. They  are well known for their high toxicity, resistance to decomposition, bioaccumulation, and long-range transport in the  environment. PCDD/Fs and PCBs have  become global concern over the last several decades  because of their accumulations in human bodies  through food  chain. The  dissertation  conducted  a series  of  studies  on  the pollution  source emissions, environmental pollution levels, and effects on environmental health. It takes sintering and municipal solid waste incinerators (MSWIs) as typical industrial emission sources, exploring the  gas-particle distribution patterns of  PCDD/Fs and PCBs in  the flue  gas  emitted from  MSWIs,  investigation  release  of  PCDD/Fs  and  PCBs from sintering and soil pollution levels around it. Evaluate the pollutions levels of PCDD/Fs and PCBs in soils around Qinghai Lake to definite the contamination of PCDD/Fs  and PCBs in remote areas. Additionally, we investigate the concentrations of PCDD/Fs and PCBs in typical food, animal and human blood. The results are presented below.
1.   PCDD/Fs and dioxin-like (dl-) PCBs in the flue gas emitted from the MSWIs were presented, in decreasing  order, within gas phases, particulate  phases, and aqueous phases. PCDD/F concentrations in the flue gas ranged from 0.75 to 15 ng/m3  while in  the  particulate   phase  they  ranged  from   0.14  to  8.1  ng/m3. Dl-PCBs  had concentrations  of  0.18–28  ng/m3 in  the  flue  gas,  and  0.041–1.3  ng/m3 in  the particulate phase.  PCDD/F and  dl-PCB levels  were associated with  specific size ranges  of  particles,  increasing  as  particle  size  decreased.  The  results   provide supports  for understanding  the  emission  characteristics of  PCDD/Fs  and  PCBs during the MSWIs and developing corresponding emission reduction measures.
2.   Dioxin-like POPs  released from  iron ore  sintering plant  in steel factory  and soil pollution levels around it were investigated. Concentrations of PCDD/Fs in the flue gas were 0.25–1.53 ng/m3 . PCBs and dl-PCBs in  the flue gas were 2.98–8.00  and 0.58–1.41 ng/m3, respectively. PCDD/Fs  (dl-PCBs) in soils  around A, B,  C were
0.068 ± 0.047 (0.0088–0.40), 0.12 ± 0.10 (0.0047–0.46) and 0.05 ± 0.086 (0.0016–0.28)  ng/g,   respectively.  The  contaminant  concentrations   in  the  environment typically decrease with increasing distance from the emission source. The PCDD/F and dl-PCB concentrations to downwind of the industrial sites were higher than the concentrations  to the  upwind of  the  industrial sites.  Children  were found  to  be exposed to  higher amounts of  contaminant effects than  adults, not  exceeding the safety  threshold. The  concentrations  and  distribution patterns  of  PCDD/Fs  and PCBs in surface soil samples collected from  around Qinghai Lake were quantified to  further know  long range  transport. Concentrations  of  PCDD/Fs and  dl-PCBs were 0.0004–0.020 and 0.0018–0.011 ng/g, respectively, below the urban soils.
3.   Dioxin-like POPs  in Chinese  mitten crabs  collected from Jiangsu  Province were investigated. Concentrations of PCDD/Fs and PCBs in white crabmeat were 0.0060 ±  0.012 ng/g  and 16.2±    19.6  ng/g, respectively. And  PCDD/Fs and  PCBs in brown  crabmeat  were  0.042±0.041   ng/g  and  6.61±2.79    ng/g,  respectively.Consuming  smaller amounts  of  crabs  would not  singnificantly  increase  human exposure risks to dioxin-like POPs. PCDD/F and PCB sources in the crab food web were assessed. The contribution from sediment was around 77 times that from feed,and sediment may be the most important source of PCDD/Fs and PCBs in cultured crabs. Regular cleaning,  replacement and remediation of  sediments in crab ponds will effectively reduce the exposure of crabs to PCDD/Fs and PCBs.
4.   The concentrations and distributions of dioxin-like POPs  in the meat products and whole blood  of eight  typical terrestrial  meat animals (chicken,  duck, rabbit,  pig,cattle,  sheep, horse  and  donkey)  consumed daily  in  our life  were  investigated.PCDD/F  and  dl-PCB  concentrations  in  meat products  were  0.00047–1.09  and 0.014–0.17ng/g, respectively. The mean TEQ of PCDD/Fs and PCBs in bloods were 0.064 and 0.0035 ng/L. Meat products of chicken consumed by humans induced the largest annual exposure to PCDD/Fs and PCBs.
5.   Exposure  levels  of  PCDD/Fs  and  PCBs  in  the  blood  of  local  residents  were estimated.  Concentrations of  PCDD/Fs and  PCBs  (dl-PCBs) were  0.35  and 2.7(0.018) ng/L, respectively. Higher 17 PCDD/F levels were found in females than in males from different ages. Mean levels of 17 PCDD/Fs in males were 0.28 ng/L and 0.31 ng/L in females. Besides, higher 17 PCDD/F and dl-PCB concentrations were detected in  the elder  than in  the young  and increased  with age,  which might  be caused by  the longer  half-lives of  these compounds  and lower metabolic  rate of elder people. Further,  mass quantities (0.95 ng/L)  of higher chlorinated PCDD/Fs were the highest in blood from orthopedics  compared with participants from other departments, which may be associated with the bone properties.

Pages151
Language中文
Document Type学位论文
Identifierhttp://ir.rcees.ac.cn/handle/311016/41457
Collection环境化学与生态毒理学国家重点实验室
Recommended Citation
GB/T 7714
韩莹. 二噁英类 POPs的环境污染特征及人体暴露研究[D]. 北京. 中国科学院生态环境研究中心,2018.
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