多溴联苯醚及十溴二苯乙烷在上海市典型环境介质中的分布及生态风险评估
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摘要
随着经济社会的不断发展以及区域城市化和工业化的进一步加剧，包括多溴联苯醚（PBDEs）和多溴二苯乙烷（DBDPE）在内的多种阻燃剂产品不断向环境中扩散，污染日益严重。上海作为国际化大都市，其产业结构一直偏重，资源消耗与污染排放一直处于高位。微型电子计算机、汽车等工业产业的增长，使环境中的阻燃剂等持久性有机污染物（POPs）的污染负荷加重。同时，人口增长速度过快，生活垃圾及汽车尾气等污染物的排放总量持续不断增加，使得上海市区域内POPs的污染源不断增长，令上海面临严重的环境污染问题。
本研究主要以上海市三大水体（包括黄浦江、苏州河以及蕴藻浜）中的沉积物、上海市特定校园环境内室内灰尘以及校园环境内非职业暴露者等典型环境介质为目标对象，对八种PBDEs同系物（包括BDE-28，-47，-99，-100，-153，-154，-183和-209）和DBDPE等溴系阻燃剂在目标介质中的分布特征及潜在的生态风险进行深入研究；对上海市典型环境介质所受到的PBDEs和DBDPE污染现状、潜在污染源进行科学的评估；为研究以PBDEs和DBDPE为代表的溴系阻燃剂在上海市不同环境介质间的相互关联性提供数据基础，同时也为制定各种区域性或全球性的策略提供前提条件。通过研究，本文得到以下主要结果与结论：
(1)文章首次对上海地区表层沉积物中PBDEs的污染水平、时空分布特征和潜在污染来源进行系统研究，并进一步探讨该污染物对区域内水体底息生物可能产生的生态风险，为控制PBDEs的环境排放，保护当地水生生态环境提供重要的科学依据。
研究结果表明PBDEs在上海市水体沉积物中广泛存在。对比国内外其他相关研究可以发现，本研究区域内BDE-209的浓度处于相对较高的水平，而其余七种PBDEs同系物的总浓度之和则相对较低。
BDE-209在沉积物样品中占PBDEs总量的97%以上。除BDE-209外，所检测的其余七种PBDEs同系物中，BDE-47和BDE-99所占比例较大，接下来是BDE-28。通过Spearman相关性分析可以发现，沉积物中的BDE-209与∑8PBDEs存在显著性相关。说明BDE-209在上海地区对沉积物中∑8PBDE有最主要贡献。上海市水体沉积物中的PBDEs主要来源于商业用多溴联苯醚阻燃剂产品。同时，沉积物中的高溴代PBDEs同系物可能通过不同途径转化为低溴代PBDEs同系物。
对沉积物中的PBDEs进行生态风险评估发现，PBDEs对研究地区沉积物中的底息生物目前没有表现出明显的生态风险。不过，鉴于本地区高浓度的十溴联苯醚可能通过食物链转化为高毒性的五溴联苯醚，而进一步提高生态风险。因此，PBDEs对本研究区域内水生生态系统可能造成的生态风险还需进一步持续研究。
(2)文章首次研究了校园环境中室内灰尘PBDEs含量分布以及校园环境中非职业暴露者头发样品中的PBDEs含量分布情况。对头发样品和灰尘样品中PBDEs的潜在污染来源进行分析，并对二者之间的相关性进行初步研究。
研究结果表明，所有室内灰尘和人体头发样品中都能检测到PBDEs的存在，证实该物质在非职业暴露场所的校园室内环境中分布比较广泛。所有PBDEs目标同系物在灰尘中的检出率为100%；而在头发样品中，除BDE-100和BDE-154的检出率较低以外，其余六种PBDEs同系物均有较高检出率（>50%）。
BDE-209是室内灰尘和人体头发样品中占主导地位的PBDEs同系物。除BDE-209以外，BDE-47和BDE-99两种同系物在灰尘和头发样品中所占的比例较高。同时，通过Spearman相关性分析和主成分分析的结果可以发现，灰尘和头发样品中的PBDEs主要来源于商业用多溴联苯醚物质，且主要以商业用十溴联苯醚为主。相关性研究还发现，人体头发样品中的BDE-47与同一采样区域室内灰尘中的BDE-47存在显性相关（r=0.44, p=0.048）。同时，另一种PBDEs同系物BDE-99在头发样品和灰尘样品中也存在类似的显性相关性（r=0.68, p=0.025）。
(3)文章首次报道了本地区非生物样品（沉积物）和生物样品（人体头发）中新型溴系阻燃剂DBDPE的浓度含量水平及分布特征。
研究结果表明，所有沉积物样品和头发样品中均能检测出DBDPE。这说明该种新型溴系阻燃剂已在上海市不同类型的环境介质中有广泛分布。DBDPE在沉积物中的浓度与BDE-209的浓度显性相关；而在头发样品中，这两种物质没有表现出明显的相关性。这说明，沉积物中的DBDPE和BDE-209有相同的潜在污染来源，而头发样品中两种物质的来源则较为随机。此外，DBDPE与TOC在夏季沉积物样品中的相关性较好，而在冬季样品中的相关性较差。
DBDPE在不同流域沉积物中的平均浓度呈现：苏州河>黄浦江>蕴藻浜的趋势。而DBDPE在不同性别上的浓度分布与包括PBDEs，PCBs，OCPs等在内的POPs类似，污染物在女性头发样品中的浓度高于男性样品。本研究中，女生头发样品中DBDPE的平均浓度是男生头发中的3.4倍。
With the continuous development of social economics and further growing regionalurbanization and industrialization, numerous categories of flame retardants, includingpolybrominated diphenyl ethers (PBDEs) and polybromodiphyl ethane (DBDPE), continuouslyspread to the environment and cause increasingly serious pollution. As an international metropolis,industrial structure of Shanghai mainly consists of heavy industries, which makes the resourceconsumption and pollution discharge at a high level. What is more, with the increasing ofindustries of computer and automobile, the pollution of flame retardants in the environment havebeen aggravating. Meanwhile, with the rapid growing of population, the total amount of garbage,automobile exhaust and emission of other pollutants continuously increase, which makes Shanghaiface serious problems of environmental pollution.
The research objects of the present study aimed to understanding the pollution levels, spatialdistribution, isomeric composition, possible sources and potential ecological risk of8PBDEs(including BDE-28,-47,-99,-100,-153,154,-183and-209) and DBDPE in variousenvironmental mediums of Shanghai, and supplying data of the pollution relations between thoseenvironmental mediums, and precondition for formulating strategies of regional or globalcontrolling as well. The major findings and conclusions are as follows:
(1) This study unveiled the pollution levels, spatial and seasonal distributions and potentialpollution sources of PBDEs in the sediment from principal watersheds of Shanghai (includingHuangpu River, Suzhou Creek and Yunzao Creek) for the first time. Furthermore, the potentialecological risk caused by PBDEs was also studied in this study, which supplied importantscientific basis for controlling the discharge of PBDEs and protecting the local ecologicalenvironment.
The results showed that PBDEs were detected in all the sediment samples, indicating thatthese contaminants were ubiquitous in riverine environment of Shanghai. Compared to otherglobal studies, it could be found that the levels of BDE-209in sediment were relativly high, whilethose of the total concentrations of the other PBDE congeners (except for BDE-209) wererelatively low.
BDE-209accounted for more than97%of the total PBDEs in each of the sediment samples.Of the other individual PBDE congeners measured exclusion of BDE-209, BDE-47and BDE-99were the most abundant, followed by BDE-28. The results of Spearman correlation coefficient testshowed that BDE-209significantly correlated with total concentration of PBDEs in sediments,which indicated BDE-209mostly contributed to PBDE contaminants in sediments. PBDEs insediments of Shanghai mainly derived from the commercial flame retardants of PBDEs. Thehigher brominated PBDE homologues in sediment may transform into the lowers through differentpaths.
With the hazard quotient approach, PBDEs were estimated to pose no hazard to benthicorganisms in riverine sediments in Shanghai at present. However, due to high concentration ofdeca-BDE and the high toxicity of penta-BDE, potential risk of PBDEs to organisms inecosystems of Shanghai watersheds may be still an issue of concern.
(2) This study unveiled the pollution levles, distributions and potential sources of PBDEs inindoor dust and human hair samples from campus environment as well. The sources of PBDEs indust and hair samples were analyzed, and correlation analysis of PBDE homologues in both dustand hair samples were conducted.
The results showed that PBDEs could be found in all the indoor dust and human hair samples,implying these pollutants had been widely spreaded in the non-occupational exposureenvironment. All the detection frequencies of PBDE congeners were found to be100%, whilemost PBDE congeners showed good detection frequencies (>50%) in hair samples except forBDE-100and BDE-154.
BDE-209was the predominant congener among all the PBDEs in both dust and hair samples.BDE-47and BDE-99were the second dominant congeners in detected samples. Spearmancorrelation coefficient test and pricipal component analysis showed that PBDEs in dust and hairsamples mainly derived from the commercial PBDEs, especially commercial decabrominateddiphenyl ethers. Through the correlation coefficient test, significant positive correlations wereobserved between human hair and indoor dust for BDE-47(r=0.44, p=0.048) and BDE-99(r=0.68, p=0.025).
(3) This study reported the contamination levels and distribution characteristics of DBDPEin non-biological samples (sediment) and biological samples (human hair) from Shanghai area for the first time.
The results showed that DBDPE was detectable in all the sediment and hair samples, whichimplied this emerging brominated flame retardant had been widely distributed in differentenvironmental mediums in Shanghai. Significant correlations were found between DBDPE andPBDEs in sediment, however there was no correlation between the two substances in hair samples.Such phenomena demonstrated DBDPE and BDE-209in sediment shared common pollutionsources, and sources of the two substances might be more random. In addition, the correlationsbetween DBDPE and TOC in the summer sediment samples were better, but less in the wintersamples.
Average concentrations of DBDPE detected in the sediments of different rivers were infollowing descending order: Suzhou Creek> Huangpu River> Yunzao Creek. The genderdifference of DBDPE concentrations in hair was similar to other pollutants, such as PBDEs, PCBs,OCPs and so on; pollutant concentrations in female hair samples are always higher than those inmales, namely. The average concentration of DBDPE in female hair was3.4times higher than thatin males in the present study.
本研究主要以上海市三大水体（包括黄浦江、苏州河以及蕴藻浜）中的沉积物、上海市特定校园环境内室内灰尘以及校园环境内非职业暴露者等典型环境介质为目标对象，对八种PBDEs同系物（包括BDE-28，-47，-99，-100，-153，-154，-183和-209）和DBDPE等溴系阻燃剂在目标介质中的分布特征及潜在的生态风险进行深入研究；对上海市典型环境介质所受到的PBDEs和DBDPE污染现状、潜在污染源进行科学的评估；为研究以PBDEs和DBDPE为代表的溴系阻燃剂在上海市不同环境介质间的相互关联性提供数据基础，同时也为制定各种区域性或全球性的策略提供前提条件。通过研究，本文得到以下主要结果与结论：
(1)文章首次对上海地区表层沉积物中PBDEs的污染水平、时空分布特征和潜在污染来源进行系统研究，并进一步探讨该污染物对区域内水体底息生物可能产生的生态风险，为控制PBDEs的环境排放，保护当地水生生态环境提供重要的科学依据。
研究结果表明PBDEs在上海市水体沉积物中广泛存在。对比国内外其他相关研究可以发现，本研究区域内BDE-209的浓度处于相对较高的水平，而其余七种PBDEs同系物的总浓度之和则相对较低。
BDE-209在沉积物样品中占PBDEs总量的97%以上。除BDE-209外，所检测的其余七种PBDEs同系物中，BDE-47和BDE-99所占比例较大，接下来是BDE-28。通过Spearman相关性分析可以发现，沉积物中的BDE-209与∑8PBDEs存在显著性相关。说明BDE-209在上海地区对沉积物中∑8PBDE有最主要贡献。上海市水体沉积物中的PBDEs主要来源于商业用多溴联苯醚阻燃剂产品。同时，沉积物中的高溴代PBDEs同系物可能通过不同途径转化为低溴代PBDEs同系物。
对沉积物中的PBDEs进行生态风险评估发现，PBDEs对研究地区沉积物中的底息生物目前没有表现出明显的生态风险。不过，鉴于本地区高浓度的十溴联苯醚可能通过食物链转化为高毒性的五溴联苯醚，而进一步提高生态风险。因此，PBDEs对本研究区域内水生生态系统可能造成的生态风险还需进一步持续研究。
(2)文章首次研究了校园环境中室内灰尘PBDEs含量分布以及校园环境中非职业暴露者头发样品中的PBDEs含量分布情况。对头发样品和灰尘样品中PBDEs的潜在污染来源进行分析，并对二者之间的相关性进行初步研究。
研究结果表明，所有室内灰尘和人体头发样品中都能检测到PBDEs的存在，证实该物质在非职业暴露场所的校园室内环境中分布比较广泛。所有PBDEs目标同系物在灰尘中的检出率为100%；而在头发样品中，除BDE-100和BDE-154的检出率较低以外，其余六种PBDEs同系物均有较高检出率（>50%）。
BDE-209是室内灰尘和人体头发样品中占主导地位的PBDEs同系物。除BDE-209以外，BDE-47和BDE-99两种同系物在灰尘和头发样品中所占的比例较高。同时，通过Spearman相关性分析和主成分分析的结果可以发现，灰尘和头发样品中的PBDEs主要来源于商业用多溴联苯醚物质，且主要以商业用十溴联苯醚为主。相关性研究还发现，人体头发样品中的BDE-47与同一采样区域室内灰尘中的BDE-47存在显性相关（r=0.44, p=0.048）。同时，另一种PBDEs同系物BDE-99在头发样品和灰尘样品中也存在类似的显性相关性（r=0.68, p=0.025）。
(3)文章首次报道了本地区非生物样品（沉积物）和生物样品（人体头发）中新型溴系阻燃剂DBDPE的浓度含量水平及分布特征。
研究结果表明，所有沉积物样品和头发样品中均能检测出DBDPE。这说明该种新型溴系阻燃剂已在上海市不同类型的环境介质中有广泛分布。DBDPE在沉积物中的浓度与BDE-209的浓度显性相关；而在头发样品中，这两种物质没有表现出明显的相关性。这说明，沉积物中的DBDPE和BDE-209有相同的潜在污染来源，而头发样品中两种物质的来源则较为随机。此外，DBDPE与TOC在夏季沉积物样品中的相关性较好，而在冬季样品中的相关性较差。
DBDPE在不同流域沉积物中的平均浓度呈现：苏州河>黄浦江>蕴藻浜的趋势。而DBDPE在不同性别上的浓度分布与包括PBDEs，PCBs，OCPs等在内的POPs类似，污染物在女性头发样品中的浓度高于男性样品。本研究中，女生头发样品中DBDPE的平均浓度是男生头发中的3.4倍。
With the continuous development of social economics and further growing regionalurbanization and industrialization, numerous categories of flame retardants, includingpolybrominated diphenyl ethers (PBDEs) and polybromodiphyl ethane (DBDPE), continuouslyspread to the environment and cause increasingly serious pollution. As an international metropolis,industrial structure of Shanghai mainly consists of heavy industries, which makes the resourceconsumption and pollution discharge at a high level. What is more, with the increasing ofindustries of computer and automobile, the pollution of flame retardants in the environment havebeen aggravating. Meanwhile, with the rapid growing of population, the total amount of garbage,automobile exhaust and emission of other pollutants continuously increase, which makes Shanghaiface serious problems of environmental pollution.
The research objects of the present study aimed to understanding the pollution levels, spatialdistribution, isomeric composition, possible sources and potential ecological risk of8PBDEs(including BDE-28,-47,-99,-100,-153,154,-183and-209) and DBDPE in variousenvironmental mediums of Shanghai, and supplying data of the pollution relations between thoseenvironmental mediums, and precondition for formulating strategies of regional or globalcontrolling as well. The major findings and conclusions are as follows:
(1) This study unveiled the pollution levels, spatial and seasonal distributions and potentialpollution sources of PBDEs in the sediment from principal watersheds of Shanghai (includingHuangpu River, Suzhou Creek and Yunzao Creek) for the first time. Furthermore, the potentialecological risk caused by PBDEs was also studied in this study, which supplied importantscientific basis for controlling the discharge of PBDEs and protecting the local ecologicalenvironment.
The results showed that PBDEs were detected in all the sediment samples, indicating thatthese contaminants were ubiquitous in riverine environment of Shanghai. Compared to otherglobal studies, it could be found that the levels of BDE-209in sediment were relativly high, whilethose of the total concentrations of the other PBDE congeners (except for BDE-209) wererelatively low.
BDE-209accounted for more than97%of the total PBDEs in each of the sediment samples.Of the other individual PBDE congeners measured exclusion of BDE-209, BDE-47and BDE-99were the most abundant, followed by BDE-28. The results of Spearman correlation coefficient testshowed that BDE-209significantly correlated with total concentration of PBDEs in sediments,which indicated BDE-209mostly contributed to PBDE contaminants in sediments. PBDEs insediments of Shanghai mainly derived from the commercial flame retardants of PBDEs. Thehigher brominated PBDE homologues in sediment may transform into the lowers through differentpaths.
With the hazard quotient approach, PBDEs were estimated to pose no hazard to benthicorganisms in riverine sediments in Shanghai at present. However, due to high concentration ofdeca-BDE and the high toxicity of penta-BDE, potential risk of PBDEs to organisms inecosystems of Shanghai watersheds may be still an issue of concern.
(2) This study unveiled the pollution levles, distributions and potential sources of PBDEs inindoor dust and human hair samples from campus environment as well. The sources of PBDEs indust and hair samples were analyzed, and correlation analysis of PBDE homologues in both dustand hair samples were conducted.
The results showed that PBDEs could be found in all the indoor dust and human hair samples,implying these pollutants had been widely spreaded in the non-occupational exposureenvironment. All the detection frequencies of PBDE congeners were found to be100%, whilemost PBDE congeners showed good detection frequencies (>50%) in hair samples except forBDE-100and BDE-154.
BDE-209was the predominant congener among all the PBDEs in both dust and hair samples.BDE-47and BDE-99were the second dominant congeners in detected samples. Spearmancorrelation coefficient test and pricipal component analysis showed that PBDEs in dust and hairsamples mainly derived from the commercial PBDEs, especially commercial decabrominateddiphenyl ethers. Through the correlation coefficient test, significant positive correlations wereobserved between human hair and indoor dust for BDE-47(r=0.44, p=0.048) and BDE-99(r=0.68, p=0.025).
(3) This study reported the contamination levels and distribution characteristics of DBDPEin non-biological samples (sediment) and biological samples (human hair) from Shanghai area for the first time.
The results showed that DBDPE was detectable in all the sediment and hair samples, whichimplied this emerging brominated flame retardant had been widely distributed in differentenvironmental mediums in Shanghai. Significant correlations were found between DBDPE andPBDEs in sediment, however there was no correlation between the two substances in hair samples.Such phenomena demonstrated DBDPE and BDE-209in sediment shared common pollutionsources, and sources of the two substances might be more random. In addition, the correlationsbetween DBDPE and TOC in the summer sediment samples were better, but less in the wintersamples.
Average concentrations of DBDPE detected in the sediments of different rivers were infollowing descending order: Suzhou Creek> Huangpu River> Yunzao Creek. The genderdifference of DBDPE concentrations in hair was similar to other pollutants, such as PBDEs, PCBs,OCPs and so on; pollutant concentrations in female hair samples are always higher than those inmales, namely. The average concentration of DBDPE in female hair was3.4times higher than thatin males in the present study.
引文
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