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题名: PCB 11在国产有机颜料中的来源及其在我国部分地区土壤及河流沉积物中的分布特征研究
作者: 商红涛
学位类别: 博士
答辩日期: 2013
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: PCB 11 ; PCB 11 ; 黄色有机颜料 ; Yellow organic pigment ; 土壤 ; Soil ; 河流沉积物 ; Sediment ; 蚯蚓 ; Earthworm
其他题名: Study on the sources of PCB 11 in the organic pigments and its distribution in the soil and sediment of China
中文摘要:       多氯联苯(PCBs)是环境中典型的持久性有机污染物(POPs)。因其具有生物毒性、生物富集性、环境持久性并且可以在全球范围内进行长距离传输等特征被人们广泛关注。近年来PCBs在全球大部分地区都已呈现显著下降的趋势,然而一种非有意生产的PCB单体3, 3’-二氯联苯(PCB11)却因在环境中被普遍检出而引起了特别关注。本论文主要围绕PCB 11在我国可能的源、环境中的分布特征及环境行为进行了相关研究。论文主要开展了以下四个方面的工作: 首先针对PCB 11的可能来源,分别从北京、上海及江苏三地颜料生产厂家采集了24个黄色有机颜料样品进行分析检测。结果表明颜料中PCBs总浓度及PCB 11浓度分别在50.7-9.19×105 ng/g及41.7-9.18×105 ng/g之间,远高于其他相关报道。作为颜料中PCBs的主要检出单体,PCB 11约占PCBs总量的85.5%。此外PCB 11在不同类型的黄色有机颜料中浓度差异较大,以3, 3’-二氯联苯胺重氮化生产的联苯胺黄颜料中最高。研究结果表明黄色有机颜料生产过程不仅是PCB 11的重要源也是其他PCBs重要的排放源。此外研究了印染废水处理过程中PCB 11的分布特征。结果表明印染废水处理过程中水体及污泥中PCB 11的浓度分别为1.43-62.0 ng/L及7.68-7702 ng/g dw,且随着处理过程的进行PCB 11浓度呈现上升的趋势,这可能与处理过程中微生物尤其是厌氧微生物的降解活动有关。 针对我国部分土壤中PCBs及PCB 11的分布特征进行了研究。对浙江、江苏及四川三个不同经济发展水平及地理位置的土壤分析结果表明,土壤样品中的PCBs及PCB 11浓度分别为0.14-6.36 ng/g dw(0.001-1.40 pg WHO-TEQ/g dw)及0.03-0.65 ng/g dw。其中PCB 11在各省份土壤中均被检出,部分地区浓度占∑20PCBs的80%以上。PCBs及PCB 11在各省份土壤中的分布无明显相关性。此外PCB 11在三个省份土壤中浓度间不存在显著性差异,可能PCB 11在三省土壤中具有相似的排放源。 研究了PCBs及PCB 11在黄河、塔里木河、额尔齐斯河、长江、珠江、海河及辽河流域河流沉积物中的浓度水平及分布特征。结果表明PCBs及PCB 11在我国7个流域沉积物中的浓度分别为0.29-21.7 ng/g dw及0.036-2.57 ng/g dw,其中PCB 11平均浓度占∑20PCBs检出单体浓度的47%。对其分布特征研究发现PCBs在我国东部及南部地区河流沉积物中具有较高的检出水平,而PCB 11除在珠江地区具有较高浓度之外,在其他流域沉积物中不具有显著性差异。 最后对PCBs及PCB 11在生物体内富集特征进行了研究。对采自于我国东部某典型电子垃圾拆解地的蚯蚓及周围土壤及粪便分析表明,∑20PCBs在蚯蚓、土壤及蚯蚓粪便中的浓度分别为0.74-30.94,0.57-21.6及1.30-78.8 ng/g dw,PCB 11在三者中相应的浓度为0.05-0.42,0.14-0.76以及0.19-1.67 ng/g dw,分别占∑20PCBs的3.97%,17.4%,20.3%。生物/土壤富集因子(BSAF)计算结果表明,单体的logKOW在6.5左右时,BSAF值最大,在蚯蚓体内更容易被富集。而PCB 11的BSAF值在0.03-0.60之间,低于其他单体的BSAF值,表明PCB 11在蚯蚓体内的生物富集作用并不明显。
英文摘要:       Polychlorinated biphenyls (PCBs) is a typical persistent organic pollutants (POPs) that are toxic and could persist in the environment, bioaccumulate through the food web, and undergo long-range atmospheric transport. As a non-Aroclor PCB congener, PCB 11 attracted wide concerns because of its environmental ubiquity and specific sources. This study was dedicated to investigating the source, distribution in the environment and biota matrices of PCB 11 in China. Four parts are as follows: Firstly, we investigated the potential source of PCB 11 in yellow organic pigment. 24 yellow pigment samples were collected from three different manufacturing plants in China. ∑20PCBs and PCB 11 were in the range of 50.7-9.19×105 ng/g and 41.7-9.18×105 ng/g, respectively, which was much higher than those reported in previous study. The corresponding TEQ values ranged between 0.19-3683 ng WHO1998-TEQ kg-1. The contribution of PCB 11 to ∑20PCBs reached up to 85.5%. Significant differences were observed for PCB 11 concentrations among the different types of yellow pigment from the same plant, as well as among the same sample types from different plants. The highest PCB 11 concentrations were obtained in diarylide yellow pigments produced from 3, 3′-dichlorbenzidine. The result suggested that yellow pigment is an important emission source PCB 11. Considering that the general chemical structure of dyes is the same or similar to that of pigments in many cases, we also investigated the distribution of PCB 11 in dye wastewater sewage disposal plant. The concentrations of PCB 11 in wastewater and sludge were 1.43-62.0 ng/L and 7.68-7702 ng/g dw, respectively, and the concentrations of PCB 11 showed the increasing trend with the treating processes going, which was probably due to the degration of dyes by microbes. Then, the distribution of PCB 11 was studied in typical soils of Zhejiang, Jiangsu and Sichuan province. The concentrations of PCBs and PCB 11 were in the range of 0.14-6.36 ng/g dw (0.001-1.40 pg WHO-TEQ/g dw), and 0.03-0.65 ng/g dw, respectively. As a predominant congener, PCB 11 were detected in all the samples, and the contribution to ∑20PCBs could reach up to 80% in some places. The distributions of PCBs and PCB 11 in soil of same province were discrepant. Besides, there were no significant difference for PCB 11 in soils of three provinces, which might indicate that similar emission source was existed in three provinces. Subsequently, the contamination level and distribution of PCBs and PCB 11 were investigated in the sediments from seven main river basins in China.The concentrations of PCBs and PCB 11 were 0.29-21.7 ng/g dw, and 0.036-2.57 ng/g dw, respectively. PCB 11 was found with high concentraions in all samples, which had a proportion up to 47% in ∑20PCBs. The PCBs levels were much higher in southern and eastern of China, especially in Pearl River Basin and the downstream of Yangtze River. For PCB 11, no significant difference was observed among the sediment of all rivers except Pearl River. At last, we studied the bioaccumution of 20 PCB congeners in earthworm, including PCB 11. A total of 60 paired samples including earthworm, corresponding soil and wormcast were collected from a typical E-waste dismantling area in east China. ∑20PCBs concentrations in earthworm, soil and wormcast were 0.74-30.94, 0.57-21.6,and 1.30-78.8 ng/g dw, respectively. PCB 11 were detected in all samples with concentrations of 0.05-0.42, 0.14-0.76, and 0.19-1.67 ng/g dw, which contributed 3.97%,17.4%,and 20.3% to ∑20PCBs, respcetively. The maximum BSAF of PCBs was presented with logKOW around 6.5, and the BSAF of PCB 11 was in the range of 0.03-0.60 in this study, which indicated that the PCB 11 in earthworm might not be bioaccumulated by earthworm.
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/35173
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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Recommended Citation:
商红涛. PCB 11在国产有机颜料中的来源及其在我国部分地区土壤及河流沉积物中的分布特征研究[D]. 北京. 中国科学院研究生院. 2013.
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