| 题名 | 北极地区和电子垃圾拆解地典型 POPs生物累积放大效应 |
| 作者 | 朱超飞 |
| 学位类别 | 博士 |
| 答辩日期 | 2015-05 |
| 授予单位 | 中国科学院研究生院 |
| 授予地点 | 北京 |
| 导师 | 张庆华 |
| 关键词 | 持久性有机污染物 北极 电子垃圾拆解地 浓度水平 营养级放大，POPs the Arctic E-waste recycling region concentration level trophic magnification |
| 其他题名 | Bioaccumulation and biomagnification of typical POPs in the Arctic and e-waste recycling regions |
| 学位专业 | 环境科学 |
| 中文摘要 | 持久性有机污染物（Persistent Organic Pollutants，POPs）是一类具有环境持久性、高毒性、生物富集和长距离迁移特性的化合物。进入环境的POPs会沿着食物链（网）进行迁移，最 终在高营养级生物体内富集，从而造成潜在危害。本文以五种典型POPs（PCBs、PCDD/Fs、PBDEs、PBDD/Fs和HBCDs）为研究对 象，分析它们在北极背景区和台州电子垃圾拆解地中的浓度水平、单体分布特征，生物浓缩（富集）及放大效应。 研究了北极新奥尔松地区环境样品中PCBs和PBDEs的浓度水平和生物富集特征。结果显示?25PCBs在土壤、植物和鹿粪中的浓度分别为 0.57-2.52、0.30-1.16和0.56-0.98 ng g-1（干重，dw）。非商品化生产的CB-11是最主要PCBs贡献单体，占?25PCBs的16.0±9.8%。5种手性PCBs（CB-95、- 136、 -149、-174和-176）在土壤和六类植物中的手性特征显示，CB-95表现出明显的对映异构体选择性迁移，而其他几种手性PCBs特征不明 显。?13PBDEs在土壤、植物和鹿粪中的浓度分别为1.7-416、36.7-495和28.1-104 pg g-1 dw。BDE-47、-99和-183是主要的PBDEs贡献单体。污染物的生物富集因子（BAFs）（土壤和植物之间）因PCB和PBDE单体的不同， 以及植物种类的不同有所差异。六类植物样品中?25PCBs和?13PBDEs的BAFs分别为0.28-0.71和2.41-44.3，Log BAFs与土壤中PCBs和PBDEs的浓度呈显著负相关关系（R2=0.73，p<0.0001；R2=0.91，p< 0.0001）。 研究了台州电子垃圾拆解地水生食物网中PCBs、PCDD/Fs、PBDD/Fs和HBCDs的生物累积放大效应。其中PCBs浓度最高，其次是 HBCDs，PCDD/Fs和PBDD/Fs浓度水平较低。PCB的平均总浓度（Σ25PCBs）在60.2（蟾蜍）至2272 ng g-1 dw（黄鳝）之间，毒性当量浓度TEQ为3.02-2351 pg WHO2005-TEQ g-1 dw；指示性PCBs占?25PCBs的58.3-98%，CB-118是dl-PCBs的50.3-61.4%，四至六氯代CBs占?PCBs的 63.7-90.2%。2,3,7,8-位取代的平均PCDD/Fs浓度（?17PCDD/Fs）为31.9-325 pg g-1 dw，对应的TEQ是2.36-12.9 pg WHO2005-TEQ g-1 dw；单体分布以OCDD和OCDF为主（占?17PCDD/Fs的96.7%）。PBDD/Fs的浓度为5.18-69.0 pg g-1 dw，TEQ是0.62-2.58 pg WHO2005-TEQ g-1 dw（基于PCDD/Fs的毒性当量因子进行计算）；1234678-HpBDD和1234678-HpBDF之和占?11PBDD/Fs的 56.3-92.8%。三种HBCD异构体浓度之和（?3HBCDs）在5.02（福寿螺）至147 ng g-1 lw（鲫鱼）之间，对映异构体以α-HBCD为主。PCBs表现出明显的生物浓缩特征，生物浓缩因子（BCF）的对数值在1.0-6.6之间，以CB- 205（鲫鱼）最高，CB-11（青蛙）最低。BCF与KOW和PCBs的氯代水平之间均存在显著的二次曲线关系（R2=0.533，p< 0.001；R2=0.568，p<0.0001）。PCBs和PBDD/Fs均未表现出明显的营养级传递趋势，PCDD/Fs呈现出非显 著性的营养级稀释作用，ln ?3HBCDs与营养级之间存在正的线性相关性（R2=0.54, p=0.17），计算出的TMF为2.29，即HBCDs表现出营养级放大趋势。 研究了台州电子垃圾拆解地陆生食物网中PCBs、PCDD/Fs、PBDD/Fs和HBCDs的生物累积放大效应。PCBs的浓度最高，其次是 HBCDs，PCDD/Fs和PBDD/Fs处于较低水平。珠颈斑鸠体内Σ25PCBs的浓度最高（379-441 ng g-1 dw，均值416），蜻蜓（14.2-138 ng g-1 dw，均值55.0）和蚂蚱（13-65.7 ng g-1 dw，均值34.1）处于较低水平，TEQ值在0.32-305 pg WHO2005-TEQ g-1 dw之间。单体分布以指示性PCBs为主，占?25PCBs的76.4-95.3%，CB-118占dl-PCBs的50.2%-63.2%，三至六氯代 CBs占?PCBs的85.2-98.2%。平均?17PCDD/Fs浓度和TEQ分别为22.4-827 pg g-1 dw和3.57-8.76 pg WHO2005-TEQ g-1 dw，OCDF、OCDD和12378-PeCDD占Σ17PCDD/Fs的比例为14、10.8和9.26%。?11PBDD/Fs的浓度和TEQ分别 为9.81-41.8 pg g-1 dw和0.86-1.95 pg WHO2005-TEQ g-1 dw，单体分布以1234678-HpBDD和1234678-HpBDF为主（占?11PBDD/Fs的47.9-81.2%）。?3HBCDs浓度在 0.91（蜻蜓）至40.3 ng g-1 lw（老鼠）之间，低营养级生物以α-HBCD为主，高营养级以γ-HBCD为主。?25PCBs的生物富集因子（BAF）为2.24-380，单体中以 CB-126的平均BAF最大（322），物种中一珠颈斑鸠体内的平均BAF最大（177）。17种2,3,7,8-取代的PCDD/Fs单体 中，123478-HxCDD的平均BAF最大（33.9），其次为OCDF（17.1）和2378-TCDD（14）。PCBs和PBDD/Fs均未表 现出明显的营养级传递趋势；PCDD/Fs呈现显著性的营养级放大趋势，TMF为14.8；α-HBCD和?3HBCDs的TMF为0.05和0.08， 显示出营养级稀释趋势。 |
| 英文摘要 | Persistent Organic Pollutants (POPs) are chemical substances that persist in the environment, possess toxic properties, bioaccumulate through the food web, and can be transported over long distance. Once released into the environment, they will move along food chain/web, and finally bioaccumulate in the upper trophic species, causing potential hazard. In this paper, five typical POPs (PCBs, PCDD/Fs, PBDEs, PBDD/Fs and HBCDs) were selected to investigate the concentration level, congener distribution, homologue profile, bioconcentration, bioaccumulation and trophic magnification in the Arctic and e-waste recycling region. PCBs and PBDEs were determined in environmental samples collected from Ny-?lesund, Svalbard, the Arctic. Total PCB concentrations (?25PCBs) varied from 0.57 to 2.52 ng g-1 dry weight (dw) in soil, 0.30 to 1.16 ng g-1 dw in plants and 0.56 to 0.98 ng g-1 dw in reindeer dung. The non-Aroclor congener CB-11 was predominant in most samples compared to other congeners, accounting for 16.0 ± 9.8% to the ?25PCBs. The indicator CB-28, -101, -138 and -153 were also the dominant congeners. Five chiral PCBs (CB-95, -136, -149, -174 and -176) were also anylized. The signature of enantioselective biotransformation was observed in all samples for chiral CB-95. ?13PBDEs concentrations were 1.7-416, 36.7-495 and 28.1-104 pg g-1 dw in soil, plants and reindeer dung, respectively. BDE-47, -99 and -183 were the dominant congeners. Bioaccumulation factors (BAFs) in six plant species varied within individual contaminant congeners and plant species. The BAFs of ?25PCBs and ?13PBDEs in plants were 0.28-0.71 and 2.41-44.3. There were significant correlations between log BAFs and PCBs and PBDEs concentrations in soil (R2=0.73, p<0.0001 for PCBs; R2=0.91, p<0.0001 forr PBDEs). The aquatic food web in an e-waste recycling region from Taizhou, South China were selected to investigate the concentration level, bioaccumulation potential and trophic transfer of PCBs, PCDD/Fs, PBDD/Fs and HBCDs. The mean PCBs cocnentrations were the highest; the next was HBCDs; PCDD/Fs and PBDD/Fs were the lowest. The mean PCBs concentrations (?25PCBs) varied from 60.2 ng g-1 dw in toad to 2272 ng g-1 dw in eel, and the corresponding TEQ concentrations were 3.02-2351 pg WHO2005-TEQ g-1 dw. Six indicator PCBs were the dominant congeners, occupied 58.3-98% of ?25PCBs, and the percentage of CB-118 in dioxin-like PCBs were 50.3-61.4%. Tetra-CBs to hexa-CBs were the main homologues (63.7-90.2%). ?17PCDD/Fs concentrations were 31.9-325 pg g-1 dw, with TEQ concentrations of 2.36-12.9 pg WHO2005-TEQg-1 dw. The sum of OCDD and OCDF occupied 96.7% of ?17PCDD/Fs. ?11PBDD/Fs concentrations were 5.18-69.0 pg g-1 dw with TEQ concentrations of 0.62-2.58 pg WHO2005-TEQg-1 dw (based on TEFs of PCDD/Fs). The sum of 1234678-HpBDD and 1234678-HpBDF accounted for 56.3-92.8% of ?11PBDD/Fs. The sum concentrations of three HBCD isomers varied from 5.02 ng g-1 lw in apple snail to 147 ng g-1 lw in crucian carp, and α-HBCD was the dominant isomer. The bioconcentration of PCBs was found in aquatic species, and the bioconcentration factors (BCFs) were 1.0-6.6, with largest BCF of CB-205 in crucian carp and smallest BCF of CB-11 in frog. The correlations between log BCFs and log KOW and the numbers of chlorine were adequately described by species-specific parabolic models (R2=0.533, p<0.001; R2=0.568，p<0.0001). The trophic transfer of PCBs and PBDD/Fs was not found. Non-significant correlation between log ?17PCDD/Fs and trophic level suggested trophic dilution of PCDD/Fs. Positive linear correlations were observed in the plots of ln ?3HBCDs versus TLs (R2=0.54, p=0.17). The calculated trophic magnification factor for ?3HBCDs was 3.86, indicating a trophic magnification. The terrestrial food web in the e-waste recycling region from Taizhou, South China were also selected to investigate the concentration level, bioaccumulation potential and trophic transfer of PCBs, PCDD/Fs, |
| 内容类型 | 学位论文 |
| 源URL | [http://ir.rcees.ac.cn/handle/311016/34485]  |
| 专题 | 生态环境研究中心_环境化学与生态毒理学国家重点实验室 |
| 推荐引用方式 GB/T 7714 | 朱超飞. 北极地区和电子垃圾拆解地典型 POPs生物累积放大效应[D]. 北京. 中国科学院研究生院. 2015. |
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