【作者】 笪春年；

【导师】 刘桂建；

【作者基本信息】 中国科学技术大学 ， 环境科学， 2014， 博士

【摘要】 有机氯农药(OCPs)是一类典型的持久性有机污染物,在环境中难氧化、降解周期长、毒性大,对生态环境和人类健康造成的污染和危害已经引起了普遍关注。OCPs在海岸带中的分布、迁移转化及生态毒理效应是探索全球分配、迁移行为和污染水平的一个重要组成部分。本论文以黄河入海口水体、土壤、沉积物、沉积柱中OCPs为研究对象,利用固相萃取法、索式抽提、气相色谱---质谱联用分析(GC-MS)、主成分分析法、同位素定年、数学模型等多种直接和间接测试分析方法,研究了OCPs在不同介质中的赋存规律、潜在生态风险、人类健康风险、历史沉降记录和来源,探索了有机氯农药的行为归宿和交换规律。通过研究主要取得了以下几个方面的研究成果：(1)系统地建立了多介质体系中有机氯农药的分析方法,水样和固体样品的方法检测限分别为0.001-0.01ng/L和0.001-0.004ng/g,优于同类文献报道；回收率范围为75%-102%,相对标准偏差在0.2%-10%,回收率和标准偏差符合USEPA的要求,本研究建立的方法可以推广应用于多介质环境中有机氯农药的分析。(2)通过对有机氯农药在不同介质相中的分配规律研究,揭示了本研究区域环境介质中的有机氯农药来源于历史使用的有机氯农药在不同介质中重新分配的结果。HCHs倾向于由水相向沉积相沉积,DDTs倾向于由沉积相向水相释放的规律。(3)利用210Pb同位素定年法进行OCPs的沉降记录研究,揭示了OCPs从1925年-2005年期间的沉降记录变化与历史使用量和土壤残留量相关。(4)首次系统地对OCPs在黄河入海口多介质环境中的分布特征、来源、归宿、风险、相关性及行为研究,发现了HCHs和DDTs在环境介质中分别是以β-HCH和DDE形式存在,这是由于二者在环境中难降解所致；通过源分析表明了OCPs主要来自于历史残留所致,近期也有少量的工业林丹被使用过；有机氯农药之间的相关性分析揭示了有机氯农药化合物在不同介质中有类似的迁移规律；风险评价表明了γ-HCH和p’p-DDE将引起更多的生态风险,β-HCH的致癌风险应该引起重视,区域内有OCPs致癌风险较低。更多还原

【Abstract】 Organochlorine pesticides (OCPs) as an important class of typical persistent organic pollutants in the environment, it is difficult to oxidation, degradation of long cycle and high toxicity, the pollution and harm to ecological environment and human health has caused widespread concern around the world. The distribution, migration, transformation and ecotoxicological effects of OCPs in the coastal region is to explore its global distribution, migration behavior and the pollution level,In this thesis, organochlorine pesticides in water, soil, sediments and sedimentary column from the Yellow River estuary is as the research object, Solid phase extraction, Soxhlet extraction, gas chromatography-mass spectrometry, principal component analysis, isotopic dating, mathematical models and other direct and indirect test and analysis method are used. Study on the occurrence regularity, potential ecological risk, human health risk, the historical settlement record and input source of OCPs in different medium is to explore the behavior and fate of organochlorine pesticides and exchange rules in different medium.The main results are obtained in the following aspects through the study:(1) The method for analysis of organochlorine pesticides was established in multi media system, Methods of the detection limits for water samples and solid samples are0.001-0.01ng/L and0.001-0.004ng/g, respectively. They are superior to the similar reports in the literature; the recovery rate is in the range of75%-102%, the relative standard deviation is in the0.2%-10%, The detection limit was superior to similar reports in the literature, the recovery rate and standard deviation was in accordance with the requirements of USEPA, the method can be applied to the analysis of organic chlorine pesticide in the environment of multi media.(2) According to the distribution rules research of the organic chlorine pesticide in different medium phase,It was revealed the organic chlorine pesticide in regional environmental medium source from the redistribution of organochlorine pesticides in the environment in this study. HCHs tend from to the water to sedimentary facies deposition, DDTs tend to release by sedimentary to water phase.(3) The settlement dating recording of organic chlorine pesticides was studied by using210Pb isotope. It was revealed the settlement record changes of organochlorine pesticides during the years1925-2005was related with the past history use and soil residue.(4) The characteristics of the content, distribution, source, destination, risk, and their environmental behaviors of organic chlorine were studied systematically for the first time in multimedia environment from the the Yellow River estuary. It was found HCHs and DDTs in environmental media are existed in the form of β-HCH and DDE, which was mainly due to degrading difficultly in environment; The source analysis showed that the pesticide in the study area was mainly from the historical residue. Recently there are a large number of Lin Dan used in industrial. Correlation analysis between organochlorine pesticides compounds have revealed the migration of similar in different media. Risk assessment showed that the γ-HCH and p’p-DDE will cause more ecological risk. The carcinogenic risk of β-HCH should cause height to take seriously, the cancer risk of organochlorine pesticide in the region was low.更多还原