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题名: 短链氯化石蜡分析方法及环境化学行为研究
作者: 袁博
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: 江桂斌
关键词: 短链氯化石蜡 ; Short-Chain Chlorinated Paraffins(SCCPs) ; 定量 ; Quantification ; 污染现状 ; Environmental Level ; 生物富集 ; Bioaccumulation ; 工业产品 ; Industrial Product
其他题名: Analytical Method and Environmental Behavior of Short-Chain Chlorinated Paraffins
中文摘要:    
    本论文针对新型持久性有机污染物—短链氯化石蜡在环境样品中的分析检测方法进行了系统的研究,建立并比较了气相色谱与电子俘获检测器/电子轰击串接质谱/负化学源质谱等三种检测器联用测定短链氯化石蜡的仪器方法。结合文献并通过实验建立了利用气相色谱—负化学源质谱的数据处理和定量分析的方法,并通过程序参数设定和逻辑公式实现整个过程的自动化。同时,针对土壤和生物样品等不同环境介质,建立了测定环境样品中短链氯化石蜡的前处理技术,结果表明,所建立的定量分析方法回收率和重现性良好。 应用所建方法,对我国环渤海地区的双壳类和螺类软体动物样品中的短链氯化石蜡进行了研究,发现该地区普遍存在短链氯化石蜡的污染,且在人口最密集的天津地区平均浓度最高。软体动物中短链氯化石蜡总浓度在64.9-5510 ng/g(干重)之间,平均氯含量61.1%,主要以链长C10和C11的同族体为主,六氯和七氯是最主要的氯原子取代形式。不同物种间短链氯化石蜡的富集浓度和单体组成存在差异。在采集的十一个物种中,砂海螂、白蛤和牡蛎表现出较高的富集能力。双壳类软体动物短链氯化石蜡的浓度普遍高于作为捕食者的螺类。短链氯化石蜡的含量和软体动物体内的脂肪含量呈显著线性正相关关系,而和生物营养级则显著负相关,说明短链氯化石蜡在这一区域内的软体动物中没有营养级放大的现象。 采集了浙江台州电子垃圾拆解中心及周边区域内土壤、水稻(包括稻壳和糙米)以及福寿螺等多种环境及生物样品,对其所含有的短链氯化石蜡在该区域的空间分布及在不同环境介质中的累积特征进行了研究。结果表明,各种介质中的短链氯化石蜡在电子垃圾拆解中心区域的浓度显著高于周边区域,说明拆解活动会造成电子垃圾中的短链氯化石蜡释放到周围环境中。随着样品和拆解中心距离的增加,链长较短、氯原子取代个数较少的单体比例呈上升趋势。说明挥发性强的同族体具有更强的迁移能力。稻壳和福寿螺中短链氯化石蜡的浓度高于土壤样品,稻壳中的浓度比糙米中高一个数量级。和土壤相比,水稻倾向于富集挥发性强的同族体,而福寿螺对脂溶性强的同族体有良好的富集能力。 对我国八家主要的氯化石蜡工厂的九种工业产品进行了仪器定量分析。通过与标准品的色谱图比对和质谱结果研究,在其中八种产品中发现了不同含量的短链氯化石蜡。通过对工业产品中混有的短链氯化石蜡的单体组成分析表明,原料中含有的短链烷烃氯化是氯化石蜡工业产品中短链氯化石蜡的主要来源。
英文摘要:     Comprehensive studies were carried out on the analytical method of short-chain chlorinated paraffins (SCCPs), a group of new persistent organic pollutants, in environmental matrix. Three quantitative methods for analyzing CPs were compared using gas chromatograph-electron capture detector (GC-ECD), gas chromatograph-electron capture negative ion low resolution mass spectrometry (GC-ECNI-LRMS) and gas chromatograph-electron ionization tandem mass spectrometry (GC-EI-MS2). The instrumental analysis and quantitative method using ECNI-MS were built up to reduce the deviation and errors during the usage of low resolution mass spectrometry. The entire quantitative process was automatic by setting integral program parameters and the adoption of logical formula, which can dramatically reduce the consuming of time on quantification. Different pretreatment processes for the analysis of SCCPs in soil and biota samples were established. The results indicated the recovery of internal standard and reproducibility of the method were satisfactory. The established methods were applied to investigate the distributions, bioaccumulations of SCCPs in bivalves and gastropods collected from nine coastal cities of Chinese Bohai Sea. The mollusks in Tianjin showed the highest average concentrations of SCCPs, which were also the most densely populated city in the sampling area. The concentrations of total SCCPs in the mollusks were in the range 64.9 – 5510 ng/g (dry weight), with an average chlorine content of 61.1%. C10 and C11 were the predominant homologue groups of SCCPs, and six/seven chlorinated compounds were the main congener groups. Concentrations of SCCPs were generally higher in bivalves samples than that of gastropods, although the latter were the predator in this food chain. Mya arenaria, Mactra veneriformis and Crassostrea talienwhanensis (Oyster) had higher concentrations of SCCPs than other species, implying that these bivalves can be used as sentinels to indicate SCCPs contamination in the coastal regions. A significant positive linear relationship was found between SCCP concentrations and lipid contents, whereas the lipid-normalized SCCP concentrations were negatively linear-related to the trophic levels, which implied that SCCPs showed trophic dilution for mollusks in this region. The distributions, transport, and environmental fate of SCCPs in multi environmental matrices were studied in Taizhou, Zhejiang Province, which is a notorious e-waste dismantling area. The environmental matrices include soils, paddy (Oryza sativa, including husk and rice unpolished) and Apple snails (Ampullariidae). The concentrations in all samples collected from dismantling area were significantly higher than those from the outskirt areas 5-60 km away from the contaminated center, indicating that dismantling activities would cause the releasing and pollution of SCCPs to the ambient environment. With the increasing of migration distance of SCCPs from the contamination source, the percentage of congeners of shorter carbon chain length and less number of chlorides substituted were also increasing. SCCP congener with higher volatility possessed longer range transport potential. Both the concentrations and congener patterns were different among various kinds of samples. SCCPs in snails and husks were generally higher than that in soil samples. The concentrations of SCCPs in husks were one order of magnitude higher than that in corresponding rice samples. Compared with the congener pattern in soil, paddy samples tended to accumulate SCCP congeners with high volatility, and snail samples had a good potential in accumulating congeners with high lipophilicity. SCCPs in nine technical chlorinate paraffins (CPs) products were analyzed from eight domestic CPs manufactories by comparing the chromatography and mass spectrometry results between the technical products and CPs standards. Various degrees of SCCPs were found in eight technical products. The concentrations of SCCPs were below the limit of detection in the products of long-chain paraffins. The SCCPs in most of the products had a high proportion of C13 congeners. All these results indicate that chlorination of short-chain alkane in the material lead to the generation of SCCPs in the CPs produc
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/35106
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:
袁博. 短链氯化石蜡分析方法及环境化学行为研究[D]. 北京. 中国科学院研究生院. 2012.
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