典型水体沉积物与点源周边环境的全氟烷酸类化合物污染现状及趋势研究
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摘要
在过去半个世纪里,以全氟烷酸类化合物(PFAAs)为代表的全氟化合物(PFCs)凭借其独特的物理化学性质,已被广泛地应用于多种工业与民用产品的生产中。因为PFCs在环境中的持久性,近年来这类化合物已在全世界范围内的各类环境介质、生物体和人体内被检出,它们所具有的生物蓄积性和多种毒性,已对生态系统和人类造成了一定的威胁。2009年,全氟辛烷磺酸(PFOS)及其盐连同其前体化合物全氟辛烷磺酰氟(PFOSF),被正式增加至《斯德哥尔摩公约》的附件B中,旨在于全球范围内限制其生产与使用。
目前国内有关PFCs的研究主要集中于不同水体和湿沉降、以及生物和非职业暴露人群的PFCs污染水平,而有关我国典型流域沉积物中PFCs的污染现状和污染特征的研究仍缺乏。此外,有关我国生态环境和非职业暴露人群的PFCs污染水平研究,均未能明确生态环境或人群对PFCs的暴露源,因此有必要对国内已知的PFCs点源周边生态环境和非职业暴露人群的PFCs污染水平及其分布特征开展研究。
本论文通过研究我国辽河流域中浑河、太子河、辽河,长江三角洲中黄浦江、玄武湖、秦淮河,和珠江三角洲中珠江、深圳湾、布吉河的水体沉积物,以及阜新氟化工工业园区周边生态环境和当地非职业暴露人群,得出以下结论：
1)辽河流域沉积物中PFCs的总浓度介于0.19-1.0 ng/g dw之间,而该流域河水中PFCs的总浓度介于5.6-43 ng/L之间。PFOS为该流域沉积物中主要的PFCs污染物,而该流域河水中主要的PFCs污染物为PFBS和PFOA。沉积物中PFCs的总浓度不断增加的垂直变化趋势存在于辽河流域的三个主要支流中。
2)珠江三角洲的珠江广州段河流沉积物中PFCs的总浓度介于0.09-3.6 ng/g dw之间,而深圳湾和布吉河沉积物中PFCs的总浓度介于0.22-0.54 ng/g dw之间。PFOS为珠江广州段沉积物中主要的PFCs污染物,而深圳湾和布吉河则为PFOA。长江三角洲的黄浦江上海段沉积物中PFCs的总浓度介于0.25-1.1 ng/g dw之间,而南京玄武湖和秦淮河沉积物中PFCs的总浓度介于0.14-0.46 ng/g dw之间。PFOA为黄浦江上海段和南京水体沉积物中主要的PFCs污染物。沉积物中PFCs的总浓度不断增加的垂直变化趋势同样存在于长江和珠江三角洲的主要水体中。
3)通过连续监测沈阳凌空明渠排污口处污水与沉积物中PFCs在每日不同时间点的实时浓度,发现污水中多种PFCs的浓度水平在30%至1189%范围内波动,而沉积物中各种PFCs的浓度水平相对稳定,表明对同一水体在某一时间点的单次采样,有可能造成对该水体中PFCs浓度水平的高估或低估,而沉积物可以较好地反映水体中PFCs的长期污染状况。
4)阜新氟化学工业园区周边的环境中存在严重的PFOA污染,并呈逐渐增加的趋势。河水与沉积物中PFOA的最高浓度分别为668 ng/L和48 ng/g dw,地下水中PFOA浓度的最大值为524 ng/L。阜新自来水源水、出厂水和公共供水系统的自来水中PFOA的最大浓度分别为16、2.7和1.7 ng/mL。一室药物代谢动力学模型的计算结果显示,阜新居民通过饮用自来水对PFOA污染的摄入量占当地居民对PFOA暴露总量的13%。阜新人群血清中PFOA的浓度水平介于0.02-93 ng/mL之间,几何平均值为4.3 ng/mL。氟化工园区附近鸡鸭血清中PFOA浓度最大值分别为3.0和15 ng/mL,而鸡鸭肝脏中主要PFCs污染物PFOS和PFOA的浓度最大值分别为3.8和4.1 ng/g ww。
本论文的研究结果有助于我国相关部门掌握国内典型流域中PFCs的污染现状和趋势,从而为相关的环境风险评价和制订控制PFCs污染的法律法规提供科学依据；并为我国针对已知PFCs点源进行长期监测提供理论和数据支持,继而为降低PFCs污染对点源周边生态系统与人群健康所造成的潜在威胁做出贡献。
Research on Perfluoroalkyl Acid (PFAA) Contamination Status and Trend in the
In the past five decades, perfluorochemicals (PFCs),featured with perfluoroalkyl acids (PFAAs), have been employed universally in both industrial and domestic products, due to their special physicochemical characteristics.In recent years, these compounds have been detected in various environmental matrices, biota and human globally, resulting from their environmental persistence.Their existences have posed certain environmental risks to the ecosystems and human, in terms of their bioaccumulation and diverse toxicities.In 2009, perfluorooctane sulfonate (PFOS) and its salts together with its precursor, perfluorooctane sulfonyl fluoride (PFOSF), were consequently added to Annex B of the Stockholm Convention, calling for restricted production and use worldwide.
Research on the occurrences and distributions of PFCs in China so far have been mainly focused on diverse water bodies, wet precipitation, biota, and non-occupationally PFCs-exposed populations, yet little is known about the current contamination status and features of sediment PFCs in typical water bodies within Chinese regions.In addition, sources of PFCs contaminations have not been identified in the previous research on the PFCs contaminations in ecosystem, environment, and non-occupationally exposed populations, it is thus necessary to carry on studies on the PFCs contaminations and distribution features in ecosystem, environment, and non-occupationally exposed populations around known PFCs point sources in China.
The present study aimed to investigate the sediments from the Hun River, Taizi River, and Daliao River in the Liao River system, the Huangpu River in the Yangtze River Delta, the Zhujiang River in the Pearl River Delta of China, and the ecosystem, environment, and non-occupationally exposed populations around Fuxin fluorochemical industrial park. As a result, four conclusions could be drawn as follows.
1)The total concentrations of PFCs were determined in the range of 0.19 to 1.0 ng/g dry weight (dw) in sediments from the Liao River system, and those in river water there were between 5.6 and 43 ng/L.PFOS was the dominant PFC contaminant in the sediments, while PFBS and PFOA were the dominant ones in the river water. An overall decreasing trend of PFCs contaminations with depth was observed in all the sediment cores from the three main streams of the Liao River system.
2) The total concentrations of PFCs were determined between 0.09 and 3.6 ng/g dw in sediments from the Zhujiang River of Guangzhou, and those in sediments from the Shenzhen Bay and the Buji River of Shenzhen were between 0.22 and 0.54 ng/g dw. PFOS was the dominant PFC contaminant in the sediments from Guangzhou, while PFOA was the dominant one in the sediments from Shenzhen. The total concentrations of PFCs were determined between 0.25 and 1.1 ng/g dw in sediments from the Huangpu River of Shanghai, and those in sediments from the Lake Xuanwu and Qinhuai River of Nanjing were between 0.14 and 0.46 ng/g dw. PFOA was the dominant PFC contaminant in both the sediments from Shanghai and Nanjing.An overall decreasing trend of PFCs contaminations with depth was observed in all the sediment cores from the main water bodies of the Yangtze and Pearl River Deltas.
3)Based upon the continuous monitoring on the PFCs contaminations in the wastewater and sediments from Shenyang Lingkong Canal at various time points, the levels of several PFCs in the wastewater fluctuated in the range of 30% to 1189%, while those in the sediments were relatively stable, indicating that the single sampling in the same water body at any time point might lead to over-or under-estimation of the PFCs levels in that water body, however, sediment might reflect the long-term PFCs contamination levels in a water body.
4) Severe PFOA contamination with an increasing trend existed in the environment around Fuxin fluorochemical industrial park. The maximum concentration of PFOA in river and sediment were 668 ng/L and 48 ng/g dw, respectively;the highest PFOA concentration in groundwater beneath the park was 524 ng/L;the highest PFOA concentrations in the raw, finished, and drinking water of Fuxin were 16,2.7, and 1.7 ng/mL, respectively. One-compartment pharmacokinetic model indicated that, drinking water contributed 13% of the daily PFOA exposure in Fuxin. In human serum, PFOA had the geometric mean at 4.3 ng/mL,ranging from 0.02 to 93 ng/mL.The maximum concentrations of serum PFOA in chicken and ducks around the park were 3.0 and 15 ng/mL, respectively.As the dominant PFCs contaminations, the maximum concentrations of liver PFOS and PFOA in chicken and ducks there were 3.8 and 4.1 ng/g wet weight (ww),respectively.
Results of the present study provide the current contamination status and trend of PFCs in typical water systems of China for the relative Chinese administrative sections, as the scientific bases for the environmental risk assessments and legislative controls for PFCs contaminations.In addition, it could provide supporting method and data for the long-term monitoring of PFCs point sources, contributing to minimize the potential risks of PFCs contaminations posed on the surrounding ecosystems and human health.
目前国内有关PFCs的研究主要集中于不同水体和湿沉降、以及生物和非职业暴露人群的PFCs污染水平,而有关我国典型流域沉积物中PFCs的污染现状和污染特征的研究仍缺乏。此外,有关我国生态环境和非职业暴露人群的PFCs污染水平研究,均未能明确生态环境或人群对PFCs的暴露源,因此有必要对国内已知的PFCs点源周边生态环境和非职业暴露人群的PFCs污染水平及其分布特征开展研究。
本论文通过研究我国辽河流域中浑河、太子河、辽河,长江三角洲中黄浦江、玄武湖、秦淮河,和珠江三角洲中珠江、深圳湾、布吉河的水体沉积物,以及阜新氟化工工业园区周边生态环境和当地非职业暴露人群,得出以下结论：
1)辽河流域沉积物中PFCs的总浓度介于0.19-1.0 ng/g dw之间,而该流域河水中PFCs的总浓度介于5.6-43 ng/L之间。PFOS为该流域沉积物中主要的PFCs污染物,而该流域河水中主要的PFCs污染物为PFBS和PFOA。沉积物中PFCs的总浓度不断增加的垂直变化趋势存在于辽河流域的三个主要支流中。
2)珠江三角洲的珠江广州段河流沉积物中PFCs的总浓度介于0.09-3.6 ng/g dw之间,而深圳湾和布吉河沉积物中PFCs的总浓度介于0.22-0.54 ng/g dw之间。PFOS为珠江广州段沉积物中主要的PFCs污染物,而深圳湾和布吉河则为PFOA。长江三角洲的黄浦江上海段沉积物中PFCs的总浓度介于0.25-1.1 ng/g dw之间,而南京玄武湖和秦淮河沉积物中PFCs的总浓度介于0.14-0.46 ng/g dw之间。PFOA为黄浦江上海段和南京水体沉积物中主要的PFCs污染物。沉积物中PFCs的总浓度不断增加的垂直变化趋势同样存在于长江和珠江三角洲的主要水体中。
3)通过连续监测沈阳凌空明渠排污口处污水与沉积物中PFCs在每日不同时间点的实时浓度,发现污水中多种PFCs的浓度水平在30%至1189%范围内波动,而沉积物中各种PFCs的浓度水平相对稳定,表明对同一水体在某一时间点的单次采样,有可能造成对该水体中PFCs浓度水平的高估或低估,而沉积物可以较好地反映水体中PFCs的长期污染状况。
4)阜新氟化学工业园区周边的环境中存在严重的PFOA污染,并呈逐渐增加的趋势。河水与沉积物中PFOA的最高浓度分别为668 ng/L和48 ng/g dw,地下水中PFOA浓度的最大值为524 ng/L。阜新自来水源水、出厂水和公共供水系统的自来水中PFOA的最大浓度分别为16、2.7和1.7 ng/mL。一室药物代谢动力学模型的计算结果显示,阜新居民通过饮用自来水对PFOA污染的摄入量占当地居民对PFOA暴露总量的13%。阜新人群血清中PFOA的浓度水平介于0.02-93 ng/mL之间,几何平均值为4.3 ng/mL。氟化工园区附近鸡鸭血清中PFOA浓度最大值分别为3.0和15 ng/mL,而鸡鸭肝脏中主要PFCs污染物PFOS和PFOA的浓度最大值分别为3.8和4.1 ng/g ww。
本论文的研究结果有助于我国相关部门掌握国内典型流域中PFCs的污染现状和趋势,从而为相关的环境风险评价和制订控制PFCs污染的法律法规提供科学依据；并为我国针对已知PFCs点源进行长期监测提供理论和数据支持,继而为降低PFCs污染对点源周边生态系统与人群健康所造成的潜在威胁做出贡献。
Research on Perfluoroalkyl Acid (PFAA) Contamination Status and Trend in the
In the past five decades, perfluorochemicals (PFCs),featured with perfluoroalkyl acids (PFAAs), have been employed universally in both industrial and domestic products, due to their special physicochemical characteristics.In recent years, these compounds have been detected in various environmental matrices, biota and human globally, resulting from their environmental persistence.Their existences have posed certain environmental risks to the ecosystems and human, in terms of their bioaccumulation and diverse toxicities.In 2009, perfluorooctane sulfonate (PFOS) and its salts together with its precursor, perfluorooctane sulfonyl fluoride (PFOSF), were consequently added to Annex B of the Stockholm Convention, calling for restricted production and use worldwide.
Research on the occurrences and distributions of PFCs in China so far have been mainly focused on diverse water bodies, wet precipitation, biota, and non-occupationally PFCs-exposed populations, yet little is known about the current contamination status and features of sediment PFCs in typical water bodies within Chinese regions.In addition, sources of PFCs contaminations have not been identified in the previous research on the PFCs contaminations in ecosystem, environment, and non-occupationally exposed populations, it is thus necessary to carry on studies on the PFCs contaminations and distribution features in ecosystem, environment, and non-occupationally exposed populations around known PFCs point sources in China.
The present study aimed to investigate the sediments from the Hun River, Taizi River, and Daliao River in the Liao River system, the Huangpu River in the Yangtze River Delta, the Zhujiang River in the Pearl River Delta of China, and the ecosystem, environment, and non-occupationally exposed populations around Fuxin fluorochemical industrial park. As a result, four conclusions could be drawn as follows.
1)The total concentrations of PFCs were determined in the range of 0.19 to 1.0 ng/g dry weight (dw) in sediments from the Liao River system, and those in river water there were between 5.6 and 43 ng/L.PFOS was the dominant PFC contaminant in the sediments, while PFBS and PFOA were the dominant ones in the river water. An overall decreasing trend of PFCs contaminations with depth was observed in all the sediment cores from the three main streams of the Liao River system.
2) The total concentrations of PFCs were determined between 0.09 and 3.6 ng/g dw in sediments from the Zhujiang River of Guangzhou, and those in sediments from the Shenzhen Bay and the Buji River of Shenzhen were between 0.22 and 0.54 ng/g dw. PFOS was the dominant PFC contaminant in the sediments from Guangzhou, while PFOA was the dominant one in the sediments from Shenzhen. The total concentrations of PFCs were determined between 0.25 and 1.1 ng/g dw in sediments from the Huangpu River of Shanghai, and those in sediments from the Lake Xuanwu and Qinhuai River of Nanjing were between 0.14 and 0.46 ng/g dw. PFOA was the dominant PFC contaminant in both the sediments from Shanghai and Nanjing.An overall decreasing trend of PFCs contaminations with depth was observed in all the sediment cores from the main water bodies of the Yangtze and Pearl River Deltas.
3)Based upon the continuous monitoring on the PFCs contaminations in the wastewater and sediments from Shenyang Lingkong Canal at various time points, the levels of several PFCs in the wastewater fluctuated in the range of 30% to 1189%, while those in the sediments were relatively stable, indicating that the single sampling in the same water body at any time point might lead to over-or under-estimation of the PFCs levels in that water body, however, sediment might reflect the long-term PFCs contamination levels in a water body.
4) Severe PFOA contamination with an increasing trend existed in the environment around Fuxin fluorochemical industrial park. The maximum concentration of PFOA in river and sediment were 668 ng/L and 48 ng/g dw, respectively;the highest PFOA concentration in groundwater beneath the park was 524 ng/L;the highest PFOA concentrations in the raw, finished, and drinking water of Fuxin were 16,2.7, and 1.7 ng/mL, respectively. One-compartment pharmacokinetic model indicated that, drinking water contributed 13% of the daily PFOA exposure in Fuxin. In human serum, PFOA had the geometric mean at 4.3 ng/mL,ranging from 0.02 to 93 ng/mL.The maximum concentrations of serum PFOA in chicken and ducks around the park were 3.0 and 15 ng/mL, respectively.As the dominant PFCs contaminations, the maximum concentrations of liver PFOS and PFOA in chicken and ducks there were 3.8 and 4.1 ng/g wet weight (ww),respectively.
Results of the present study provide the current contamination status and trend of PFCs in typical water systems of China for the relative Chinese administrative sections, as the scientific bases for the environmental risk assessments and legislative controls for PFCs contaminations.In addition, it could provide supporting method and data for the long-term monitoring of PFCs point sources, contributing to minimize the potential risks of PFCs contaminations posed on the surrounding ecosystems and human health.
引文
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