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题名: 辽河流域高风险有机污染物的污染特征与筛查研究
作者: 滕曼
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: 魏复盛
关键词: 辽河 ; Liao River ; 有机氯类污染物 ; organic chlorine pollutants ; 新型POPs ; new POPs ; 优控污染物 ; priority pollutants ; 环境监测 ; environmental monitoring
其他题名: Pollution characterization and screening for the high-risk organic pollutants in Liaohe Basin, Northeast China
中文摘要:       辽河流域是我国东北部重要的工业基地,为我国的城市化和工业化进程做出了历史性的重大贡献,随着经济的快速发展,辽河流域水环境形势日益严峻,尤其是有机污染问题凸显,而目前对高风险有机污染物的环境残留、污染特征和迁移转化规律的认识还不够。 本文从环境管理的角度出发,立足污染物控制的不同阶段,围绕环境监管控制范围中已纳入、将要纳入和未来可能纳入的高风险有机污染物(毒性高或污染水平高),开展污染存量分析与污染物筛查研究。具体如下: 针对传统POPs中的有机氯农药(OCPs)和多氯联苯(PCBs),研究其在稻田生态系统中的河流、沉积物、稻田土壤和生物体中的分布特征、迁移特点和生物累积效应。结果显示:稻田土壤与相邻地沉积物样品中的总PCBs含量呈显著相关,具有类似的指纹,表明长期的河流灌溉对辽河下游流域稻田土壤的PCBs污染具有显著贡献。通过研究中华绒螯蟹、泥鳅和青蛙体内的有机氯类污染物的水平和分布,发现了PCBs和OCPs的生物累积作用具有种间差异和地点特异性,中华绒螯蟹对PCBs和OCPs具有较强的生物累积能力,计算得出其对六六六(ΣHCH)、滴滴涕(ΣDDT)、灭蚁灵、六氯苯(HCB)和多氯联苯(ΣPCB)的生物土壤累积因子分别为24.5、15.3、122.2、28.1和54.6。 针对新型POPs六溴环十二烷(HBCDs)、四溴双酚A(TBBPA)和多氯萘(PCNs),建立了复杂基质中三类新型POPs的选择性分离方法。以去活化硅胶为吸附剂,分别采用正己烷、正己烷/二氯甲烷(1:1)和正己烷/二氯甲烷(1:3)可将PCNs、HBCDs和TBBPA顺序洗脱,实现了三者的选择性分离。应用所建立的方法对加标的土壤样品提取液进行了测定。结果表明,该方法可以实现复杂基质中三类新型POPs的有效分离。 针对优控有机污染物的筛选,研究采用C18/HLB串联的固相萃取法进行水样富集,对水样进行全扫描分析,通过保留时间锁定(RTL)-解卷积技术(DRS)识别水样中痕量有机污染物,实现辽河流域水体中特征污染物的初步筛选与确定;对初步筛选出的污染物进行半定量分析,并计算污染物的风险商,确定最终的辽河流域优控污染物候选者清单,主要为多环芳烃等。此研究工作可为下一步污染物的监管提供参考和依据。 通过本论文的研究,证实了长期河流灌溉对稻田土壤PCBs污染的显著贡献,揭示了PCBs和OCPs的生物累积特征,发现了中华绒螯蟹的较强的生物累积能力。实现了复杂基质中PCNs、HBCDs和TBBPA的同时分离,方法有效、可靠。建立了基于风险分析的优控有机污染物筛选方法,并初步确定辽河流域优控污染物清单。研究揭示了传统POPs的污染规律,建立了新型POPs的监测技术方法,并初步确立优控污染物的筛选程序,为认识和防控各控制阶段的污染物提供了重要的理论基础和必要的技术支撑。
英文摘要:
      Liao River basin is an important industrial base in northeast China. With the rapid economic development, the pollution of aquatic environment becomes more serious, especially the prevalence of organic pollutants. In this study, from the perspective of environmental management and on the objectives of pollution control at different stages, the pollution characterization and screening for high-risk organic pollutants(with high toxicities and high accumulation levels)in the Liao River Basin were carried out. These organic pollutants included the chemicals that have been in the list of monitored pollutants, will be as the priority pollutants, and may be listed as candidate contaminants in the future. The detailed results and main conclusion are as followed. As for the traditional POPs, the occurrence and distribution of organic chlorine pesticide (OCPs) and polychlorinated biphenyls (PCBs) in river sediments and paddy soils from the downstream of Liao River Basin were analyzed, and their biological accumulations in the organisms of rice fields were characterized simultaneously. The “fingerprints” of PCBs in sediment samples and their adjacent paddy soils were similar and there was a significant correlation between the total PCB contents in sediment samples and their adjacent paddy soils, which suggested that the long-term river irrigation caused the significant pollution of PCBs in the rice fields. By comparing the levels and distribution of OCPs and PCBs in mitten crab, loach and frog, it was found that the bioaccumulations of these pollutants were species-specific and site-specific. The mitten crab had the strong abilities for the bioaccumulation of OCPs and PCBs. The biota-soil accumulation factors (BSAF) of ΣHCH, ΣDDT, Mirex, HCB and ΣPCBs in mitten crab were calculated to be 24.5, 15.3, 122.2, 28.1 and 54.6, respectively. As for the analysis of new POPs, hexabromocyclododecanes (HBCDs), tetraromobisphenol A (TBBPA) and polychlorinated naphthalenes (PCNs), a separation method of high-efficiency for the determination in complex matrices was established by choosing appropriate adsorbent and optimizing the elution conditions. Under the optimized separation conditions, the recoveries of analytical standards, measured by LC-MS/MS and GC-MS, were near to 100%. The optimized separation methods were applied to the determination of HBCDs, TBBPA and PCNs in the soils. The results showed that PCNs, HBCDs and TBBPA could be eluted subsequently with high recoveries by hexane, hexane/dichloromethane (v/v, 1: 1) and hexane/dichloromethane (v/v, 1: 3), respectively. As for the screening of priority pollutants, C18 solid extraction column coupled with HLB solid extraction column was used to extract the organic pollutants in water samples. The trace pollutants were identified based on the total scanning mode and the Deconvolution Reporting Software (DRS). The semi-quantitative analysis was carried out for the identified pollutants, and then the risk quotients of these pollutants were calculated. Thereby, preliminary screening method for priority pollutants in aquatic environment was established. Meanwhile a list of preliminary priority pollutants of Liao River was suggested, which was dominated by polycyclic aromatic hydrocarbons (PAHs). This study indicated a significant contribution of long-term irrigation of river water to the pollution of PCBs in paddy soils from the lower reach of Liao River Basin. The large capacity to accumulate PCBs, DDT, HCH, HCB and Mirex by Mitten-handed crabs was discovered. An efficient and reliable method for the selective separation of PCNs, HBCD and TBBPA was developed. Also, a method of screening priority pollutants based on risk assessment was established, and the priority pollutants of Liao River were initially identified.
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/35121
Appears in Collections:水污染控制技术研究室_学位论文

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Recommended Citation:
滕曼. 辽河流域高风险有机污染物的污染特征与筛查研究[D]. 北京. 中国科学院研究生院. 2012.
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