浙江省二恶英、多氯联苯污染水平及其对人体健康危害的风险评价研究
摘要
二恶英、多氯联苯是斯德哥尔摩公约中提出需要控制的十二中持久性有机污染物,两者虽然来源不同,但由于其相同的毒性和对环境和人类的危害,早就引起了各国政府的重视,这也是国际学者研究的热点和难点。中国于2001年5月参加公约,在2004年11月正式生效。但由于二恶英、多氯联苯检测难度极大却费用昂贵,再者本底不清,使得我国的履约困难重重。为防治血吸虫病杀灭钉螺而使用大量的五氯酚钠、城市发展需要的垃圾焚烧、大量的化工、农药和造纸企业的废液排放等,都对浙江省的环境和居民健康造成了潜在的危害。为摸清浙江省二恶英、多氯联苯污染的本底,也为政府决策部门制定治理环境措施提供科学的依据,有必要对浙江省的二恶英、多氯联苯污染水平进行监测,并对其来源和可能造成的健康危害作一定的评价,为建设“绿色浙江”作出应有的贡献。
本文以美国EPA1613和EPA1668A的分析方法为基础,系统地建立了土壤(底泥)和生物样品(鱼肉、血液和母乳)中二恶英、多氯联苯的检测方法。同时对浙江省钱塘江流域中的鱼类(鲫鱼和鲤鱼),以及浙江省五个地区的土壤、底泥和鲫鱼中的二恶英、多氯联苯进行定性和定量分析,获得了监测地区的二恶英、多氯联苯污染水平和特征,为该地区此类污染物的有效控制提供了理论和实验依据。此外,还分析了浙江省部分人群的母乳、血液和脂肪中二恶英、多氯联苯种类和含量,探讨该地区部分人群中的二恶英、多氯联苯污染水平和特征,并初步开展了风险评价。全文分为五个部分：
1、对二恶英、多氯联苯的性质、来源、毒性作用进行了阐述,对二恶英和多氯联苯的国内外分析方法进展、污染状况、风险评估等进行了综述。
2、参考美国EPA1613B、1668A(环境样品和生物样品中二恶英及多氯联苯的检测方法)和加拿大海洋渔业研究所的方法,对土壤和生物材料(鱼肉和母乳)中二恶英、多氯联苯进行方法学试验,包括样品制备、提取和纯化、分离及仪器检测等条件的优化,系统地建立了土壤、鱼肉和母乳中二恶英、多氯联苯的检测方法。对标准参考物质CRM：WMF-01检测结果所示(n=6),PCDD/F同位素内标的平均回收率范围在59.6%-122.14%之间,RSD在1.60%～-12.71%之间；PCB同位素内标的平均回收率范围在55.6%-101.2%之间,RSD在4.63%～-11.55%之间；此外,该方法经参加国际盲样比对和标准参考物质的检验,符合美国EPA1613B、1668A方法规定的各项指标。该方法的正确性和可行性也为下一步研究的开展打下了基础。
3、该部分研究了钱塘江流域采集的鲫鱼和鲤鱼中多氯代二苯并-对-二恶英和多氯代二苯并呋喃(PCDD/Fs)和多氯联苯(PCBs)的污染水平和特征。结果表明,在鲫鱼和鲤鱼肉中总PCDD/Fs浓度平均值分别为4.29 pg/g ww(湿重)和5.39 pg/g ww；总PCBs(共23个同系物)浓度平均值分别为4.70 ng/g ww和2.36 ng/gww；总毒性当量(TEQ)平均值分别为1.24 pg/g和1.11 pg/g。在PCDD/F同系物中,含量较多的为2,3,7,8-TCDF,1,2,3,7,8-PeCDF和2,3,4,7,8-PeCDF。同时,低氯代的CB31/28物质在两种鱼中含量较多。本次实验中鲫鱼和鲤鱼肉中的PCDD/Fs,PCBs和总TEQ的测定值与国内其它水域中鱼肉中的含量相当。可见,钱塘江水域中鱼肉的TEQ水平相对较低,位于允许的安全水平。
4、该部分测定了浙江省五个地区的土壤、底泥和鲫鱼中的二恶英和多氯联苯的含量和毒性当量。结果表明,土壤、底泥和鲫鱼中的平均总二恶英浓度分别为1993.5 pg/g(以重计)、2550.7pg/g(以干重计)和5.25 pg/g(以湿重计)；平均总多氯联苯的浓度分别为97000pg/g(以重计)、306332 pg/g(以干重计)和12678 pg/g(以湿重计)；平均总毒性当量分别为27.6 pg g-1 pg/g(以重计)、468.6 pg/g(以干重计)8.2 pg/g(以湿重计)。研究表明,在研究的五个地区中,路桥地区的二恶英和多氯联苯污染严重,含量已接近曾报道的广东电子垃圾回收地和越南两个污染最严重的地区,应引起当地政府及相关部门的重视；金华和永嘉地区土壤和底泥中多氯联苯含量较高,但具体的污染来源尚未确定,有待于进一步研究；五个地区的居民每人每日的暴露量进行评估显示,路桥地区居民食用鲫鱼的每人每日的暴露量较高,建议少量或不食用。
5、该部分别对浙江省普通人群人体脂肪、母乳、血液中的二恶英和多氯联苯的污染水平和污染特征图谱进行了调查研究。结果表明,人体脂肪、母乳、儿童血液中17种二恶英平均总浓度分别为108 pg/g lipid、55.0±39.5 pg/g lipid和208±172 pg/g lipid;12种类二恶英PCB平均总浓度分别为32.8 ng/g lipid、8.0±0.4 ng/g lipid和9.8±5.3 ng/g lipid;指示性PCB平均总浓度分别为154 ng/g lipid、15.8±9.3 ng/g lipid和28.3±11.9ng/g lipid。人体脂肪、母乳、血液中二恶英和多氯联苯的毒性当量分别为9.22 pg/g lipid、3.09±2.36 pg/g lipid、11.7±7.9 pg/g lipid和16.2 pg/g lipid、3.56 pg/g lipid、11.9±6.6 pg/g lipid。几种主要食品如鱼类和鸡蛋中二恶英和多氯联苯的污染指纹图谱与人体组织中检测到的该类污染物污染指纹图谱非常相近,证明膳食摄入是普通人群暴露二恶英类物质的主要途径。由于东西方饮食习惯的差异,东方人对脂肪含量高的动物源性食品的摄入要远远低于欧美人,这可能是造成东西方人群脂肪中二恶英类化合物污染水平差异的一个重要原因。
根据研究结果和二恶英、多氯联苯的污染来源及途径,提出了二恶英、多氯联苯的防治和控制措施。
Polychlorinated dibenzo-p-dioxins/furans (PCDD/Fs) and polychlorinated biphenyls (PCBs) are two of the twelve persistent organic pollutants (POPs) recognized by Stockholm Convention. They are highly persistent compounds and have been detected in air, water, soil, sediment, animals and foods. In the past 2 decades, a great concern has been raised worldwidely on these pollutants due to their potential threats to human health. However, the determination of PCDD/Fs and PCBs is a complicated and expensive procedure, on the other hand, data that reflecting their background is not enough. Zhejiang is a fast-developing province in China; at the same time, its environment has been seriously influenced by side products of industry activity. The pollutants may orgin from municipal waste burning, waste water from paper making mills, and pesticide manufactory, etc. More badly, many of these contaminants contain toxical compounds like dioxin and PCBs with a certain extent. So it's absolutely necessary to monitor these kinds of pollutants and make corresponding evaluation on their risks to both environment and human health.
The methods for the determination of PCDD/Fs and PCBs with stable isotope dilution technique and gas chromatography-mass spectrometry were established based on US EPA method 1613B and 1668A respectively. The methods were applied for the determination of dioxins and PCBs in fish (from Qiantang River), soil-sludge-fish (from five districts of Zhejiang) and human samples as well (breast milk, serum and human adipose tissue from Zhejiang general population) with the aim of monitoring PCDD/Fs-PCBs level and their corresponding congener profile in both environmental samples and bio-bodies. Furthermore, risk assessment was also carried out. The work is consisted of five parts:
(1) A review of dioxin and PCBs, including their chemical and physical property, contamination source, toxicity and risk assessment, as well as the progress of analytical method.
(2) In this part, the method for the determination of PCDD/Fs and PCBs in soil and bio-samples (fish and breast milk) was established based on US EPA method 1613B, 1668A and the method of Canada EPS 1/RM/31 for environmental samples. The extraction, purification, separation procedure and instrumental detection parameters were optimized. The method was validated using Certificated Reference Materials (CRM:WMF-01, Fortified fish samples). The recovery of 13C labeled PCDD/Fs in WMF-01 was in the range of 59.6%-122.1%, RSD was in the range of 1.60%-12.7% (n=6), The recovery of 13C labeled PCBs in WMF-01 was in the range of 55.6%-101.2%, RSD was in the range of 4.63%-11.6% (n=6). These results were within the range recommended by EPA 1613B and 1668A. We also participated in 2006 international comparsion on dioxin in food and our results were acceptable. The accuracy of the established method may provide an analyze basis for our later studies
(3) In this part, the concentrations and congener patterns of polychlorinated dibenzo-p-dioxins, dibenzofurans (PCDD/Fs) and polychlorinated biphenyls (PCBs) were determined in the muscles of nineteen crucian carp and eleven White Amur bream collected from Qiantangjiang River. The means of total PCDD/Fs were 4.29 pg g"1 wet weight (ww) in crucial carp and 5.39 pg g-1 ww in White Amur bream. The means of total PCBs (sum of 23 congeners) were 4.70 ng g-1 ww in crucial carp and 2.36 ng g-1 ww in White Amur bream. The means of total TEQ were 1.24 pg g-1 ww in crucial carp and 1.11 pg g-1 ww in White Amur bream. The predominating PCDD/F congeners were 2,3,7,8-TCDF,1,2,3,7,8-PeCDF and 2,3,4,7,8-PeCDF. The level of lower chlorinated CB31/28 was high in two fish species. The levels of PCDD/Fs, PCBs and total TEQ in fish caught from Qiantangjiang River were similar to those in similar fish species caught from some rivers and lakes in China. The lower levels of total TEQ levels measured in fish muscles allow local residents consuming fish caught from Qiantangjiang River at an acceptable safety level.
(4) In this chapter, we determined the concentrations and toxicity equivalences (TEQs) of PCDD/Fs and PCBs in fishes, soils and sediments from five districts to investigate the levels of these two pollutants in Zhejiang Province, China. The means of total PCDD/Fs in soils, sediments and fishes were 1993.5 pg g-1 dry weight (dw),2550.7 pg g-1dw and 5.25 pg g-1 wet weight (ww) respectively. The averages of total PCBs in soils, sediments and fishes were 97000 pg g-1 dw,306332 pg g-1dw and 12678 pg g-1 ww respectively. The means of total TEQs in soils, sediments and fishes were 27.6 pg g-1 dw,468.6 pg g-1dw and 8.2 pg g-1 ww respectively. Present research showed that Luqiao, one of selected five districts was seriously contaminated by PCDD/Fs and PCBs which presented the similar level to Guangdong (China) and Veitnam heavily polluted by chemical defoliants and electronic waste. High PCB level was also found in soil/sludge collected from Jinhua and Yongjia, but their possible sources were still unclear. We estimated daily exposure to these pollutants through dietary intake, the data showed the intake of Crucian Carp had a health risk. Accordingly,we suggest loacal residents eat little or no Crucian Carp from Luqiao.
(5) In this part, concentration and congener profile (finger print) of dioxin and PCBs in human samples (blood, adipose tissue, breast milk) from genernal population of Zhejiang province were investigated. The data showed that the concentration of PCDD/Fs in human adipose tissue, breast milk and children blood were 108 pg/g lipid, 55.0±39.5 pg/g lipid and 208±172 pg/g lipid respectively, concentrations of 12 dioxin like PCB were 32.8 ng/g lipid,8.0±0.4 ng/g lipid and 9.8±5.3 ng/g lipid respectively, concentrations of indicator PCBs were 154 ng/g lipid,15.8±9.3 ng/g lipid and 28.3±11.9 ng/g lipid respectively. The corresponding TEQ of PCDD/Fs and PCBs in adipose tissue, breast milk and children blood were 9.22 pg/g lipid,3.09±2.36 pg/g lipid,11.7±7.9 pg/g lipid and 16.2 pg/g lipid,3.56 pg/g lipid,11.9±6.6 pg/g lipid respectively. The finger prints of PCDD/Fs and PCBs from major food category (egg, fish for example) were very similar to each other. Food intake represents the main route of human exposure to PCDD/Fs and PCBs. People in East Asia have similar diets, and their food intake of animal origin is generally lower than that of Europeans. This may partly explain why WHO PCDD/F TEQs for East Asia are generally lower than those for Europe. Prevention and control regulations for PCDD/Fs and PCBs are suggested in this paper according to contaminants sources and their transferring routes in the environment.
本文以美国EPA1613和EPA1668A的分析方法为基础,系统地建立了土壤(底泥)和生物样品(鱼肉、血液和母乳)中二恶英、多氯联苯的检测方法。同时对浙江省钱塘江流域中的鱼类(鲫鱼和鲤鱼),以及浙江省五个地区的土壤、底泥和鲫鱼中的二恶英、多氯联苯进行定性和定量分析,获得了监测地区的二恶英、多氯联苯污染水平和特征,为该地区此类污染物的有效控制提供了理论和实验依据。此外,还分析了浙江省部分人群的母乳、血液和脂肪中二恶英、多氯联苯种类和含量,探讨该地区部分人群中的二恶英、多氯联苯污染水平和特征,并初步开展了风险评价。全文分为五个部分：
1、对二恶英、多氯联苯的性质、来源、毒性作用进行了阐述,对二恶英和多氯联苯的国内外分析方法进展、污染状况、风险评估等进行了综述。
2、参考美国EPA1613B、1668A(环境样品和生物样品中二恶英及多氯联苯的检测方法)和加拿大海洋渔业研究所的方法,对土壤和生物材料(鱼肉和母乳)中二恶英、多氯联苯进行方法学试验,包括样品制备、提取和纯化、分离及仪器检测等条件的优化,系统地建立了土壤、鱼肉和母乳中二恶英、多氯联苯的检测方法。对标准参考物质CRM：WMF-01检测结果所示(n=6),PCDD/F同位素内标的平均回收率范围在59.6%-122.14%之间,RSD在1.60%～-12.71%之间；PCB同位素内标的平均回收率范围在55.6%-101.2%之间,RSD在4.63%～-11.55%之间；此外,该方法经参加国际盲样比对和标准参考物质的检验,符合美国EPA1613B、1668A方法规定的各项指标。该方法的正确性和可行性也为下一步研究的开展打下了基础。
3、该部分研究了钱塘江流域采集的鲫鱼和鲤鱼中多氯代二苯并-对-二恶英和多氯代二苯并呋喃(PCDD/Fs)和多氯联苯(PCBs)的污染水平和特征。结果表明,在鲫鱼和鲤鱼肉中总PCDD/Fs浓度平均值分别为4.29 pg/g ww(湿重)和5.39 pg/g ww；总PCBs(共23个同系物)浓度平均值分别为4.70 ng/g ww和2.36 ng/gww；总毒性当量(TEQ)平均值分别为1.24 pg/g和1.11 pg/g。在PCDD/F同系物中,含量较多的为2,3,7,8-TCDF,1,2,3,7,8-PeCDF和2,3,4,7,8-PeCDF。同时,低氯代的CB31/28物质在两种鱼中含量较多。本次实验中鲫鱼和鲤鱼肉中的PCDD/Fs,PCBs和总TEQ的测定值与国内其它水域中鱼肉中的含量相当。可见,钱塘江水域中鱼肉的TEQ水平相对较低,位于允许的安全水平。
4、该部分测定了浙江省五个地区的土壤、底泥和鲫鱼中的二恶英和多氯联苯的含量和毒性当量。结果表明,土壤、底泥和鲫鱼中的平均总二恶英浓度分别为1993.5 pg/g(以重计)、2550.7pg/g(以干重计)和5.25 pg/g(以湿重计)；平均总多氯联苯的浓度分别为97000pg/g(以重计)、306332 pg/g(以干重计)和12678 pg/g(以湿重计)；平均总毒性当量分别为27.6 pg g-1 pg/g(以重计)、468.6 pg/g(以干重计)8.2 pg/g(以湿重计)。研究表明,在研究的五个地区中,路桥地区的二恶英和多氯联苯污染严重,含量已接近曾报道的广东电子垃圾回收地和越南两个污染最严重的地区,应引起当地政府及相关部门的重视；金华和永嘉地区土壤和底泥中多氯联苯含量较高,但具体的污染来源尚未确定,有待于进一步研究；五个地区的居民每人每日的暴露量进行评估显示,路桥地区居民食用鲫鱼的每人每日的暴露量较高,建议少量或不食用。
5、该部分别对浙江省普通人群人体脂肪、母乳、血液中的二恶英和多氯联苯的污染水平和污染特征图谱进行了调查研究。结果表明,人体脂肪、母乳、儿童血液中17种二恶英平均总浓度分别为108 pg/g lipid、55.0±39.5 pg/g lipid和208±172 pg/g lipid;12种类二恶英PCB平均总浓度分别为32.8 ng/g lipid、8.0±0.4 ng/g lipid和9.8±5.3 ng/g lipid;指示性PCB平均总浓度分别为154 ng/g lipid、15.8±9.3 ng/g lipid和28.3±11.9ng/g lipid。人体脂肪、母乳、血液中二恶英和多氯联苯的毒性当量分别为9.22 pg/g lipid、3.09±2.36 pg/g lipid、11.7±7.9 pg/g lipid和16.2 pg/g lipid、3.56 pg/g lipid、11.9±6.6 pg/g lipid。几种主要食品如鱼类和鸡蛋中二恶英和多氯联苯的污染指纹图谱与人体组织中检测到的该类污染物污染指纹图谱非常相近,证明膳食摄入是普通人群暴露二恶英类物质的主要途径。由于东西方饮食习惯的差异,东方人对脂肪含量高的动物源性食品的摄入要远远低于欧美人,这可能是造成东西方人群脂肪中二恶英类化合物污染水平差异的一个重要原因。
根据研究结果和二恶英、多氯联苯的污染来源及途径,提出了二恶英、多氯联苯的防治和控制措施。
Polychlorinated dibenzo-p-dioxins/furans (PCDD/Fs) and polychlorinated biphenyls (PCBs) are two of the twelve persistent organic pollutants (POPs) recognized by Stockholm Convention. They are highly persistent compounds and have been detected in air, water, soil, sediment, animals and foods. In the past 2 decades, a great concern has been raised worldwidely on these pollutants due to their potential threats to human health. However, the determination of PCDD/Fs and PCBs is a complicated and expensive procedure, on the other hand, data that reflecting their background is not enough. Zhejiang is a fast-developing province in China; at the same time, its environment has been seriously influenced by side products of industry activity. The pollutants may orgin from municipal waste burning, waste water from paper making mills, and pesticide manufactory, etc. More badly, many of these contaminants contain toxical compounds like dioxin and PCBs with a certain extent. So it's absolutely necessary to monitor these kinds of pollutants and make corresponding evaluation on their risks to both environment and human health.
The methods for the determination of PCDD/Fs and PCBs with stable isotope dilution technique and gas chromatography-mass spectrometry were established based on US EPA method 1613B and 1668A respectively. The methods were applied for the determination of dioxins and PCBs in fish (from Qiantang River), soil-sludge-fish (from five districts of Zhejiang) and human samples as well (breast milk, serum and human adipose tissue from Zhejiang general population) with the aim of monitoring PCDD/Fs-PCBs level and their corresponding congener profile in both environmental samples and bio-bodies. Furthermore, risk assessment was also carried out. The work is consisted of five parts:
(1) A review of dioxin and PCBs, including their chemical and physical property, contamination source, toxicity and risk assessment, as well as the progress of analytical method.
(2) In this part, the method for the determination of PCDD/Fs and PCBs in soil and bio-samples (fish and breast milk) was established based on US EPA method 1613B, 1668A and the method of Canada EPS 1/RM/31 for environmental samples. The extraction, purification, separation procedure and instrumental detection parameters were optimized. The method was validated using Certificated Reference Materials (CRM:WMF-01, Fortified fish samples). The recovery of 13C labeled PCDD/Fs in WMF-01 was in the range of 59.6%-122.1%, RSD was in the range of 1.60%-12.7% (n=6), The recovery of 13C labeled PCBs in WMF-01 was in the range of 55.6%-101.2%, RSD was in the range of 4.63%-11.6% (n=6). These results were within the range recommended by EPA 1613B and 1668A. We also participated in 2006 international comparsion on dioxin in food and our results were acceptable. The accuracy of the established method may provide an analyze basis for our later studies
(3) In this part, the concentrations and congener patterns of polychlorinated dibenzo-p-dioxins, dibenzofurans (PCDD/Fs) and polychlorinated biphenyls (PCBs) were determined in the muscles of nineteen crucian carp and eleven White Amur bream collected from Qiantangjiang River. The means of total PCDD/Fs were 4.29 pg g"1 wet weight (ww) in crucial carp and 5.39 pg g-1 ww in White Amur bream. The means of total PCBs (sum of 23 congeners) were 4.70 ng g-1 ww in crucial carp and 2.36 ng g-1 ww in White Amur bream. The means of total TEQ were 1.24 pg g-1 ww in crucial carp and 1.11 pg g-1 ww in White Amur bream. The predominating PCDD/F congeners were 2,3,7,8-TCDF,1,2,3,7,8-PeCDF and 2,3,4,7,8-PeCDF. The level of lower chlorinated CB31/28 was high in two fish species. The levels of PCDD/Fs, PCBs and total TEQ in fish caught from Qiantangjiang River were similar to those in similar fish species caught from some rivers and lakes in China. The lower levels of total TEQ levels measured in fish muscles allow local residents consuming fish caught from Qiantangjiang River at an acceptable safety level.
(4) In this chapter, we determined the concentrations and toxicity equivalences (TEQs) of PCDD/Fs and PCBs in fishes, soils and sediments from five districts to investigate the levels of these two pollutants in Zhejiang Province, China. The means of total PCDD/Fs in soils, sediments and fishes were 1993.5 pg g-1 dry weight (dw),2550.7 pg g-1dw and 5.25 pg g-1 wet weight (ww) respectively. The averages of total PCBs in soils, sediments and fishes were 97000 pg g-1 dw,306332 pg g-1dw and 12678 pg g-1 ww respectively. The means of total TEQs in soils, sediments and fishes were 27.6 pg g-1 dw,468.6 pg g-1dw and 8.2 pg g-1 ww respectively. Present research showed that Luqiao, one of selected five districts was seriously contaminated by PCDD/Fs and PCBs which presented the similar level to Guangdong (China) and Veitnam heavily polluted by chemical defoliants and electronic waste. High PCB level was also found in soil/sludge collected from Jinhua and Yongjia, but their possible sources were still unclear. We estimated daily exposure to these pollutants through dietary intake, the data showed the intake of Crucian Carp had a health risk. Accordingly,we suggest loacal residents eat little or no Crucian Carp from Luqiao.
(5) In this part, concentration and congener profile (finger print) of dioxin and PCBs in human samples (blood, adipose tissue, breast milk) from genernal population of Zhejiang province were investigated. The data showed that the concentration of PCDD/Fs in human adipose tissue, breast milk and children blood were 108 pg/g lipid, 55.0±39.5 pg/g lipid and 208±172 pg/g lipid respectively, concentrations of 12 dioxin like PCB were 32.8 ng/g lipid,8.0±0.4 ng/g lipid and 9.8±5.3 ng/g lipid respectively, concentrations of indicator PCBs were 154 ng/g lipid,15.8±9.3 ng/g lipid and 28.3±11.9 ng/g lipid respectively. The corresponding TEQ of PCDD/Fs and PCBs in adipose tissue, breast milk and children blood were 9.22 pg/g lipid,3.09±2.36 pg/g lipid,11.7±7.9 pg/g lipid and 16.2 pg/g lipid,3.56 pg/g lipid,11.9±6.6 pg/g lipid respectively. The finger prints of PCDD/Fs and PCBs from major food category (egg, fish for example) were very similar to each other. Food intake represents the main route of human exposure to PCDD/Fs and PCBs. People in East Asia have similar diets, and their food intake of animal origin is generally lower than that of Europeans. This may partly explain why WHO PCDD/F TEQs for East Asia are generally lower than those for Europe. Prevention and control regulations for PCDD/Fs and PCBs are suggested in this paper according to contaminants sources and their transferring routes in the environment.
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