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Alternative TitleRelease, Distribution, and Health Risk of Typical Persistent Organic Pollutants (POPs) from Thermal Metallurgical Processes in Some Area
Thesis Advisor徐盈
Degree Grantor中国科学院水生生物研究所
Place of Conferral水生生物研究所
Keyword金属热处理 持久性有机污染物 二噁英 多氯联苯 多溴联苯醚 高分辨气质联用 来源 指纹特征 电子垃圾 健康风险 8-羟基脱氧鸟苷 长江口 烧结 路桥
Abstract持久性有机污染物(POPs)的释放,环境分布及其对人体健康的影响是当前国内外关注的一个热点。二噁英(PCDD/Fs),多氯联苯(PCBs) 和多溴联苯醚(PBDEs)由于具有高度的环境持久性、生物蓄积性、半挥发性和高毒性等特点,更是成为POPs研究中的焦点。最新研究表明,金属热处理过程(包括烧结,无序焚烧,铜熔解炉,电子熔解炉和线圈熔解炉等)均能导致大量污染物的释放,是POPs释放的重要污染源。本文选择典型的金属热处理工厂-武汉钢铁集团的烧结厂为试验点,研究了铁矿石烧结过程二噁英的释放;选择长江口宝钢排污口附近地区以及浙江路桥电子废物拆解地区为试验点,研究了二噁英在环境中的分布与指纹特征;选择路桥电子垃圾拆解从业人员为对象,评价了高浓度典型POPs暴露对人体健康的风险。所获得的主要研究结果如下: 1.建立了同时分析二噁英、多氯联苯和多溴联苯醚的同位素稀释-高分辨气质联用(HRGC/HRMS)-多离子检测(MID)方法和分析质量保证和质量控制体系(QA/QC)。样品的分离纯化效果,方法的回收率和检测限等都达到美国环保署相关标准分析方法的要求。利用标准参考物和实际样品的分析证明了该实验方法的可靠性和分析结果的准确性。 2.采用同位素稀释-HRGC/HRMS-MID方法分析了烧结厂不同除尘系统中排放的烟尘和静电除尘器灰尘中的二噁英。结果显示,烧结过程中产生的二噁英主要来自台车的机头部分,是台车机头部分冷却区中从头合成(de novo synthesis)的结果。样品中的二噁英以PCDFs占优势为主要指纹特征:浓度最高的同系物依次为TCDFs和PeCDFs。并且,2,3,4,7,8–PeCDF对 WHO-TEQs的贡献最大,占总TEQ值的45%左右。 3.以长江口为试验点,采用同位素稀释--HRGC/HRMS-MID方法分析长江口表层底泥和双壳类生物中的二噁英。结果显示,在宝钢集团烧结厂排污口下游的生物样品中2,3,4,7,8-PeCDF对总毒性当量起主要的贡献。说明烧结厂产生的二噁英是一个重要的污染源。研究发现,二噁英在生物体内有很明显的累积。尤其是石洞口双壳类生物中的二噁英浓度,已经超过了国际相关规定的最高限值,会对周围环境和人体健康造成一定的影响。 4.以浙江路桥电子垃圾拆解现场为试验点,采用同位素稀释-HRGC/HRMS- MID同时分析方法检测了典型环境样品中二噁英、多氯联苯和多溴联苯醚。研究发现,该地区环境样品中的二噁英、多氯联苯和多溴联苯醚浓度水平已超过世界上其他同类研究所报道的数值。样品的指纹特征表明:二噁英和多溴联苯醚主要来源于电子垃圾的无序焚烧,废旧变压器拆解过程中释放的变压器油是当地多氯联苯的主要来源。拆解工人周围环境中的样品和头发中污染物的浓度表明,工人处于高浓度的二噁英、多氯联苯和多溴联苯醚暴露的环境之中。 5.以8-OHdG为氧化损伤的生物标志物,采用HPLC-ECD方法检测了路桥地区电子垃圾拆解工人上班前和下班后尿液中8-OHdG的浓度水平。结果显示,下班后工人尿液中8-OHdG浓度是上班前的4倍。这说明工人在高浓度的二噁英、多氯联苯和多溴联苯醚暴露环境中,人体受到了严重的氧化损伤。下班后尿液中8-OHdG的浓度甚至和一些前列腺和膀胱癌症患者的水平相当,表明这些在高浓度POPs暴露下从业的工人正面临较大癌症风险。 上述研究结果为我国POPs污染控制及其环境健康风险评价提供了重要科学依据和技术支持。
Other AbstractRelease, distribution, and health risk of persistent organic pollutants (POPs), especial of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), polychlorinated biphenyls (PCBs), and polybrominated diphenyl ethers (PBDEs), are becoming a major environmental concern in the world. Theses compounds are highly persistent, semi-volatile, bioaccumulative, and have the adverse effects including immune, endocrine, nervous and reproductive toxicities to humans and animals. According to the latest inventory of PCDD/Fs emissions, thermal metallurgical processes, such as sintering, open burning of E-waste, and secondary smelters of different metal, are the other major pollution sources. Therefore, the samples collected from sinter plant were analyzed to discuss the emission and profile of PCDD/Fs. Human or environmental samples collected from Luqiao area in Zhejiang province or Changjiang Estuary to evaluate the contamination status. The potential sources of these contaminants in those areas and their potential influence to the environment and human beings were also discussed. The major content and the results are as follows. 1. The method for simultaneous determination of PCDD/Fs, PCBs, and PBDEs by isotope dilution-HRGC/HRMS-MID was established based on method US EPA 1613B, 1668A, and 1614. It was validated using the reference materials, and applied for the analysis of environmental samples. All the recoveries are within the acceptable ranges specified in the US EPA standard methods. 2. The fly ash and electrostatic precipitator (ESP) dusts samples were collected from the sinter plant of Wuhan Iron & Still Group. The samples were analyzed for PCDD/Fs by HRGC/HRMS-MID according to US EPA 1613B method. The drying area in sinter belt was expected to be the main place to produce dioxins during sintering process by de novo synthesis. PCDFs congeners in the samples were dominant and it can be seen increasing with Cl atom (r2 = 0.98), the congeners of PCDFs were decreased. Among them, 2,3,4,7,8-PeCDF was found to constitute around 45% of the total WHO- toxic equivalent (TEQ) values in the samples. 3. Surface sediments and bivalves samples collected from the Changjiang Estuary were analyzed for PCDD/Fs by isotope dilution- HRGC/HRMS-MID. In the bivalves samples collected in the downstream near the sewage outlet of sinter plant in Baoshan Iron & Still Group, 2,3,4,7,8-PeCDF was found to be dominant congener and the main contributor to total WHO-TEQs. The waste from sinter plant was major source of PCDD/Fs in the Estuary. The biota-sediment accumulation factor (BSAF) values obtained showed that PCDD/Fs were apparently accumulated in the biota. European Community Authorities (ECA) has settled a maximum level of 4 pg WHO-TEQs/g fresh weight in fish muscle and fishery products. The PCDD/Fs in the bivalve samples in the estuary were higher than the ECA bench mark, and may have potential risk to the environment. 4. The environmental and human samples collected from Luqiao area, a typical E-waste dismantling area, were analyzed for PCDD/Fs, PCBs, and PBDEs by the simultaneous analysis using isotope dilution- HRGC/HRMS-MID technique. Comparing the results with those inform the other researches, the Luqiao area is considered as being highly polluted by PCDD/Fs, PCBs, and PBDEs. Their homologue and congener profiles in the samples demonstrated that high concentrations of PCDD/Fs and PBDEs were originated from open burning of E-waste, meanwhile dismantling of transformers and capacitors were main contributor for the contamination of PCBs. The results showed that the E-waste dismantling workers were exposed to high concentrations of PCDD/Fs, PCBs, and PBDEs. 5. Using 8-OHdG as a biomarker for DNA oxidative damage, the preworkshift and postworkshift urines samples were collected from male workers in the E-waste dismantling area. The results of 8-OHdG levels in preworkshift urines were 6.40 ± 1.64 µmol/mol creatinine, but the levels of 8-OHdG in postworkshift urines were found to be significantly higher up to 24.55 ± 5.96 µmol/mol creatinine (p < 0.05), that has even been close to the levels in the urine of cancer patients such as prostate cancer and bladder cancer. Therefore, it is expected that there is a high cancer risk from the DNA oxidative stress for those workers in the E-waste dismantling area, because they are exposed to the high concentrations of PCDD/Fs, PCBs, and PBDEs. The results from this study provide scientific bases and technological support for the control of POPs release, environmental and human health risk assessment.
Document Type学位论文
Recommended Citation
GB/T 7714
闻胜. 金属热处理过程中典型持久性有机污染物的释放、环境分布及其健康风险[D]. 水生生物研究所. 中国科学院水生生物研究所,2008.
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