| 题名 | 典型区域六溴环十二烷(HBCD)的污染水平和分布特征研究 |
| 作者 | 李红华 |
| 学位类别 | 博士 |
| 答辩日期 | 2012 |
| 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 | 六溴环十二烷 HBCD 莱州湾 Laizhou Bay 中国水系 River drainage basins in China 江苏 Jiangsu 南极 Antarctica |
| 其他题名 | Study of the levels and distribution of HBCD in the typical areas |
| 中文摘要 | 六溴环十二烷(HBCD)是一种溴代脂环类化合物，是目前世界上消费量最大的溴代阻燃剂(BFRs)之一。HBCD具有生物富集性、持久性、毒性和潜在的长距离迁移能力，被认为是一种新型的持久性有机污染物(POPs)，引起了各国的高度关注。 本文建立了不同环境介质和生物基质中HBCD的前处理方法，采用液相色谱-三重四极杆串联质谱法(HPLC-MSMS)分析，大气压化学电离负离子源(APCI-)，多重反应监测模式(MRM)，内标法定量。工作曲线线性范围为0.5-200 ng/g，?α-、?β-、γ-HBCD的方法检出限(MDLs)分别为0.23，0.088，0.085 ng/g。 以典型HBCD污染地区莱州湾为研究区域，研究了生产源释放对周围环境的影响。土壤、底泥、植物、水生生物和大气中HBCD的浓度范围分别为0.88-6901 ng/g 干重(dw)，2.93-1029 ng/g dw，8.88-1.60×105 ng/g dw，7.09-815 ng/g 脂肪重(lw)，0.151-47.5 ng/m3。土壤中HBCD的浓度与点源和采样点间的距离呈显著的指数下降关系。芦苇样品中HBCD浓度与对应的土壤浓度呈线性正相关。大气中HBCD的浓度受与点源距离和风向的影响明显。水生生物中?α-，?β-，γ-HBCD的分布有明显的物种特异性和组织特异性。 对中国七个主要水系：长江、黄河、珠江、塔里木河、额尔齐斯河、海河、辽河底泥中HBCD的污染状况进行了调查。HBCD的检出率为54%，浓度范围为未检出(＜检测限(LOD))至206 ng/g dw。HBCD浓度水平呈现出我国东南沿海地区高于我国北方地区，河流下游高于上游地区的趋势，这表明HBCD的污染水平与城市和工业活动密切相关。与其它国家和地区相比，长江流域底泥污染较重，另外6个水系处于相同或较低的水平。 研究了我国江苏、四川两省土壤中HBCD的浓度水平和分布特征。江苏土壤的HBCD检出率为100%，浓度范围为166.9-6276 pg/g dw。四川土壤HBCD的检出率为83.3%，浓度范围为＜LOD-334.3 pg/g dw。位于东部沿海地区的江苏省浓度明显高于位于西部的四川省。按土壤使用类型分析，工业区土壤中HBCD的浓度最高，其次分别为城区土壤、农业和郊区土壤。区域分布表明，HBCD的浓度与城市化和工业化关系密切。成年人通过摄食土壤日均暴露HBCD的量(EDI)为0.84 pg/kg body weight day，儿童暴露风险高于成年人。 对南极菲尔德斯半岛和阿德利岛环境和生物样品中HBCD的浓度水平的调查结果表明，HBCD检出率为77%，环境和植物样品中HBCD的浓度范围为＜LOD-5977 pg/g dw，动物样品的浓度范围为＜LOD-43.29 ng/g lw。菲尔德斯半岛和阿德利岛的土壤、地衣、苔藓中HBCD浓度的空间分布表明，我国南极科学考察站对于该地区HBCD的分布没有明显的影响。 |
| 英文摘要 | Hexabromocyclododecane (HBCD) is a kind of brominated alicyclic hydrocarbon, which is one of the most produced brominated flame retardants (BFRs). Due to its properties of bioaccumulation, persistence, toxicity and potential of long-range atmospheric transport, HBCD was nominated as a persistent organic pollutant (POP). HBCD was found ubiquitous in global environment and has caused growing concern. Pretreatment methods of HBCD in various environmental matrices and biotic species were developed and the instrument parameters were optimized. The samples were analyzed by HPLC-MS/MS using atmospheric pressure chemical ionization (APCI) negative ion mode with multiple reaction monitoring mode (MRM) and the quantification of HBCD were performed by the internal standard method．The linear ranges of the calibration curve for ?α-, ?β-, γ-HBCD were 0.5-200 ng/g, and the method detection limits (MDLs) for ?α-, ?β-, γ-HBCD were 0.23, 0.088, 0.085 ng/g, respectively。 HBCD study was conducted in Laizhou Bay area to investigate the influence of manufacturing facilities on the HBCD levels in the surrounding environment. The range of HBCD concentrations were 0.88-6901 ng/g dw, 2.93-1029 ng/g dw, 8.88-1.60×105 ng/g dw, 7.09-815 ng/g lw and 0.151-47.5 ng/m3 for soils, sediments, plants, aquatic species and atmosphere, respectively. Significant negative correlations were observed between HBCD concentrations in soils and the distance from the manufacturing facilities. HBCD concentrations in the reed were closely related with those in the soil from the same sampling site. The distance from point source and wind direction significantly influenced the levels of HBCD in the atmosphere. Species and tissue-specific bioaccumulation of HBCD were found in the aquatic species. Occurrence and distribution of HBCD in sediments from seven major river drainage basins in China were studied. The detection frequency of HBCD was 54%, with the concentrations ranged from below LOD to 206 ng/g dw. The spacial distribution of HBCD showed apparently increasing trends from North China to Southeast China and from the upper reaches to the lower reaches of the rivers, which suggested that intensive urbanization and industrialization appear to be the major sources of HBCD. HBCD levels was at the relatively high level in Yangtze River, while other six rivers were at the similar or lower level compared with in other regions in the world. HBCD concentrations were investigated in soils from Jiangsu and Sichuan province. The detection frequency of HBCD in Jiangsu, Southeast China was 100% with the concentrations ranged from 166.9 to 6276 pg/g dw, while in Sichuan, West China, it was 83.3% with the concentrations ranged from below LOD to 334.3 pg/g dw. HBCD levels in the soils from Jiangsu were much higher than those from Sichuan. Soils from industrial lands showed high HBCD levels, followed by urban land, farmland and suburban land. The spacial distribution of HBCD levels showed a close relationship with urbanization and industrialization. The study on HBCD in the environmental and biotic samples from Fildes Peninsula and Ardley Island, Antarctica showed that the detection frequency of HBCD was 77%. The concentrations ranged from below LOD to 5977 pg/g dw for environmental and plant samples, and from below LOD to 43.29 ng/g lw for animal samples. The spacial distribution of HBCD levels in soil, lichen and moss samples showed that the presence of research stations did not affected the distribution of HBCDs in the local area. |
| 内容类型 | 学位论文 |
| 源URL | [http://ir.rcees.ac.cn/handle/311016/35103]  |
| 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 | 李红华. 典型区域六溴环十二烷(HBCD)的污染水平和分布特征研究[D]. 北京. 中国科学院研究生院. 2012. |
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