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1.
Polybrominated diphenyl ethers (PBDE) are a class of brominated flame retardants with some congeners having the ability to accumulate in body lipids. The incorporation of PBDE in consumer products found primarily in the indoor environment suggests that routes of exposure include inhalation of indoor air and contact with indoor dust. The purpose of this study was to test the hypothesis that lifestyle factors, and in particular the proximity and use of products likely to contain PBDE in the indoor environment, are primarily responsible for levels of PBDE found in human milk. Human milk samples were taken from two populations of lactating women in the same geographic region of the United States: one “typical” of US suburban lifestyle, and the other practicing a traditional Amish lifestyle, which excludes many modern amenities containing PBDE, such as computers and televisions. For a subset of the cohort, persistent organic pesticides and polychlorinated biphenyls (PCB) were also measured in human milk samples. Despite the small number of participants, there is evidence suggestive of Amish women having lower PBDE concentrations in their milk. In addition, the nonsignificant differences in levels of PCBs and pesticides between the two groups of women as compared to the significant differences in levels of PBDE suggest an important route of exposure for PBDE other than diet. Information prepared for study participants is provided to initiate a dialogue on how to best communicate biomonitoring findings to study participants and to the public in general.  相似文献   

2.
Polybrominated diphenyl ethers (PBDEs) are brominated flame retardants (BFRs) which have recently been detected in human blood and milk in the USA, and presently these PBDE levels are found to be the highest globally. On a population basis, individual blood and individual milk analyses show similar congener patterns and levels. Until now, there has not been a study comparing PBDE levels in milk and blood of the same individuals. This study is the first to report these levels for PBDEs, though partitioning between blood and milk has been done previously for dioxins and polychlorinated biphenyls (PCBs). Twelve congeners in 11 nursing mothers’ blood and milk were found and the data describe partitioning ratios between blood and milk. The data suggest it may be easier for smaller, less brominated congeners to move from blood to milk.  相似文献   

3.
Levels of polybrominated diphenyl ether (PBDE) flame retardants have been increasing in humans and the environment for the past few decades. Human levels are markedly higher in the US than Europe. Although food appears to be a significant route of intake, food PBDE levels are not substantially higher in the US than Europe. House and office dust appear to be major routes of exposure with air believed to usually provide a lesser route of intake. Because there are very few measurements of airborne PBDE that have been performed in relevant microenvironments in the US, increased efforts to assess airborne PBDE in the US as sources of exposure are needed. This study reports, for the first time from a Southwestern US city in Texas, the results of measurements of airborne PBDE in multiple locations, two outdoor and six indoor (residential and office) from active air sampling with collection of a combination of both vapor- and particulate-phase PBDE. Higher PBDE levels were measured in indoor than outdoor air, which confirms previous findings. Of 11 measured congeners including BDE 209, total PBDE levels in two outdoor air samples were 112 and 125 pg m?3 and the indoor air levels ranged from 175 to 1232 pg m?3 with a median of 572 pg m?3. These findings suggest that sources of air contamination with PBDE may be similar in Texas as elsewhere in North America. However, more sampling is required to (1) better determine if this is the case and (2) attempt to characterize potential sources of PBDE contamination in both indoor and outdoor air by analysis of congener patterns.  相似文献   

4.
Contamination profiles of organochlorine pesticides (OCPs), polychlorinated biphenyls (PCBs), and polybrominated diphenyl ethers (PBDEs) were determined in six fish species from three selected regions along coastal waters off Savannah, GA, USA. Concentrations of PCBs were predominant (12–493 ng g?1 lw) followed by PBDEs (10–337 ng g?1 lw), OCPs such as DDTs (2.7–153 ng g?1 lw), chlordanes (3.8–34 ng g?1 lw), cyclodienes (<0.1–35 ng g?1 lw), mirex (<0.1–8.6 ng g?1 lw), γ-hexachlorocyclohexane (<0.1–1.4 ng g?1 lw), and hexachlorobenzene (<0.1–0.68 ng g?1 lw). The results indicated no region-specific difference in the contaminants however inter-species as well as intra-species differences were evident. Comparison of DDTs, PCBs, and PBDEs profiles in fish with those from other countries revealed that fish from coastal waters off Savannah contained relatively less concentrations of PCBs and chlorinated pesticides, while PBDE concentrations were comparable or even higher than fish samples from other regions. Polychlorinated biphenyl congeners and chlorinated pesticide tempoal trend data exhibited no increase of contamination levels. The levels of PCBs and chlorinated pesticides in fish from Savannah coastal waters were below the Food and Drug Administrations (FDA) established limits for human consumption.  相似文献   

5.
为调查电子垃圾回收活动对当地水生生物造成的多溴联苯醚(PBDEs)污染,测定了广东某电子垃圾回收地附近水库中水生生物样品(水蛇、鱼类、草虾和田螺)和对照区样品(鲮鱼)中18种PBDEs含量,通过对样品氮同位素的测定,探讨了PBDEs在该地淡水食物链上的生物富集特征.研究结果显示,∑PBDEs(总PBDEs含量)在水蛇、鱼类、草虾和田螺中分别为39.6~186、1.82~75.7、4.60~17.1和7.26~17.0μg·g-1(脂重),比华南地区鱼体中∑PBDEs的平均含量高3个数量级,表明电子垃圾回收活动已对当地水生生物造成了PBDEs的严重污染.除BDE66、BDE99、BDE153、BDE183和BDE209外,其他13种PBDE单体在食物链上均存在着生物放大效应,但生物放大能力(B值)与正辛醇-水分配系数logKOW相关性不明显,可能是由于某些PBDE单体在生物体内存在代谢作用.以上结果表明,由电子垃圾回收活动导致的PBDEs污染存在较大的生态风险,应该引起高度关注.  相似文献   

6.
电子废弃物拆解地水体多溴联苯醚分布特征   总被引:2,自引:0,他引:2  
为了解和比较广东贵屿电子废弃物拆解地和珠三角城市地区水体中多溴联苯醚的种类、含量及分布特征,于2011年9月在广东贵屿周边地区和广州采集了20个地下水、7个地表水和4个珠江水,用反相C18萃取小柱提取净化后,利用气相色谱-质谱法测定了样品中的8种多溴联苯醚(PBDEs)。研究结果表明:贵屿地区地下水中PBDEs浓度总体上较高,总质量浓度范围为2.54~71.74 ng·L-1,平均为22.97 ng·L-1,各类PBDEs的检出率为25%~95%。三溴联苯醚(BDE28)、四溴联苯醚(BDE47)、五溴联苯醚(BDE99和BDE100之和)、六溴联苯醚(BDE153和BDE154之和)、七溴联苯醚(BDE183)和十溴联苯醚(BDE209)的质量浓度分布分别为nd~0.64、nd~18.43、nd~25.26、nd~13.92、nd~9.06和nd~15.60 ng·L-1。从物种上来看,分别源于四溴、五溴和十溴联苯醚产品的BDE47、BDE99和BDE209是贵屿地区地下水样中的优势同系物。通过比率P=(BDE47+BDE99)/BDE209研究发现:低溴代联苯醚比高溴代联苯醚更易被地表径流迁移转换进入到地下水中。贵屿地区地表水中PBDEs的质量浓度范围为3.41~63.83 ng·L-1,平均总质量浓度为19.38 ng·L-1,稍低于当地地下水中PBDEs的平均总质量浓度,PBDEs的组成以高溴代的BDE209为特征,与世界其他水体研究结果相比,可以发现贵屿地区的地表水中PBDEs的平均总质量浓度明显偏高,说明该地区的地表水受到较严重的PBDEs污染,必须引起足够的重视。珠江水中PBDEs的总质量浓度范围为3.48~20.84 ng·L-1,平均为10.39 ng·L-1,表明近年来珠江水体中PBDEs污染有逐渐恶化的趋势。  相似文献   

7.
Polychlorinated biphenyl (PCB) congeners were analyzed by high resolution gas chromatography/high resolution mass spectrometry (HRGC/HRMS) of whole blood samples taken from 24 healthy adult Japanese volunteers (12 males and 12 females; age range 25–46 years). On average, 95 PCB congeners were detected in whole blood samples. The mean of total PCB concentration in whole blood was 771.9 pg g–1 whole blood (139.6 ng per g-lipid). Congener-specific analysis identified the predominant PCB congeners as #153 (22.2), #180 (11.6), #138 (8.4), #182/187 (6.6), #118 (5.6), #163/164 (5.0), #99 (3.9), #74 (3.6), #146 (3.3), #170 (3.0) and #156 (2.2), representing 75.6 of all PCBs detected in the human blood samples. Among the predominant PCB congeners, #153, #180, #138, #187 #118, #99 and #74 had chlorine as the substituent at the 2-, 4- and 5- positions of the phenyl-ring. In human blood in Japanese individuals, it is assumed that these congeners would be characteristic of the entire population, based on the relation between PCB ingestion and metabolism. Measuring 209 PCB congeners has the advantage of providing detailed information regarding the congener distribution within the blood samples, which can be compared to congener patterns in other matrices. Congener-specific analysis of 209 PCB congeners is especially useful in evaluating human exposure to PCBs.  相似文献   

8.
We investigated the occurrence of halogenated flame retardants (HFRs) including polybrominated diphenyl ethers (PBDEs), six novel brominated flame retardants (NBFRs) and dechlorane plus in air and soils on the eastern slope of Mt. Gongga on the eastern Tibetan Plateau. We detected all of the NBFR except bis(2-ethylhexyl)-tetrabromophthalate and pentabromoethyl benzene. NBFRs constituted the most prevalent group. BDE-28 and BDE-47 dominated among the PBDE congeners. Decabromodiphenyl ethane was detected at relatively high levels up to 171 pg/m3 and 1450 pg/g dry weight in air and soils, respectively; however, it appeared to be easily degraded in the environment. A general decreasing trend was observed among the HFR concentrations with increasing altitude, and this was due to the prominent contribution of source emissions over possible influence of environmental conditions. This study also suggests that HFRs are supplied to forest soils mainly in the form of precipitation and retained in the O horizon layers.  相似文献   

9.
分析了水生(鲶鱼)和陆生(家鸽)生物体中卤系阻燃剂(HFRs)的组成和浓度。鲶鱼中短链氯化石蜡(SCCPs)浓度均值为30 800 ng·g~(-1)lw(脂肪归一化浓度),是最主要的HFRs,然后依次是多溴联苯醚(PBDEs)(2 300 ng·g~(-1)lw)、四溴双酚A(TBBPA)(37 ng·g~(-1)lw)、六溴环十二烷(HBCD)(21 ng·g~(-1)lw)、德克隆(DP)(14 ng·g~(-1)lw)、十溴二苯乙烷(DBDPE)(7.1 ng·g~(-1)lw)和六溴苯(HBB)(6.2 ng·g~(-1)lw);而家鸽中PBDEs含量最高(17 000 ng·g~(-1)lw),其次是SCCPs(7 600 ng·g~(-1)lw)DP(1 600 ng·g~(-1)lw)DBDPE(14 ng·g~(-1)lw)HBB、TBBPA和HBCDs(未检出)。鲶鱼和家鸽HFRs组成比较发现,鲶鱼中具有较高百分含量的低溴代PBDE单体和较低的fanti值,而家鸽中具有较高百分含量的高溴代PBDE单体和较高的fanti值。实验结果初步表明,水生生物较多地富集水溶性较大的化合物,陆生生物则较多地富集疏水性较强的化合物。研究认为以上水生和陆生生物体中污染物的差异性富集现象可能与化合物因不同物理化学性质导致的不同环境迁移行为有关。  相似文献   

10.
Intake of many persistent organic pollutants (POPs) including dioxins, dibenzofurans and PCBs is almost exclusively from gastrointestinal ingestion of animal fats in the diet. With polybrominated diphenyl ether (PBDE) brominated flame retardants (BFRs), no consensus exists at present as to the extent of intake from food, from indoor dust or other routes of intake. Vegans, or pure vegetarians, were previously found to have low body burden of dioxins and dibenzofurans in blood. Data reported here for the first time show a trend towards lower PBDE levels with longer time periods without ingestion of food of animal origin in 8 adult residents of the United States. A stronger relationship between lower PBDE levels and time without meat, specifically, is consistent with substantial PBDE intake from meat relative to fish or dairy products in Americans. These vegans had somewhat lower PBDE levels with a range 12.4–127 and a median 23.9?ppb than published reports of US general population samples which had a range of 4–366 and median of 26?ppb. Our findings suggest that food of animal origin may be a major but not the sole contributor to human body burden of PBDEs.  相似文献   

11.
The purpose of this study was to evaluate polychlorinated biphenyls (PCBs) contamination levels in roe and red deer from north-western Poland and to assess environmental pollution in this area. A quantitative analysis was conducted using a capillary gas chromatography/mass spectrometry method. The mean concentrations of ΣPCBs (sum of PCBs: 28, 52, 101, 138, 153, 180) in liver samples were 30.24±12.35 ng·g?1 of lipid weight (l.w.) in roe deer and 60.13±14.23 ng·g?1 l.w. in red deer, compared with 24.21±10.02 and 45.22±9.77 ng·g?1 in the lungs of roe and red deer, respectively. PCBs 138, 153 and 180 were the dominant congeners in the liver samples of the analysed animals, whereas PCB 138 and 153 in the lungs. TEQs levels calculated for only dioxin-like PCBs were low: 0.32 and 0.29 pg WHO-PCB-TEQ·g?1 fat in liver of red deer and roe deer, respectively. The mean PCB concentrations obtained in our study for organs of roe deer and red deer were several times lower than those reported elsewhere. These findings show that the investigated roe and red deer originated from an area with low levels of PCB contamination.  相似文献   

12.
珠江入海口水体中多溴联苯醚及其来源分析   总被引:3,自引:0,他引:3  
2005年3月至2006年2月,选取珠江8个入海口,进行每月1次为期1周年的水样采集。检测了96个水样的多溴联苯醚(PBDEs,包括BDE 28、47、66、85、99、100、138、153、154、183、196、197、203、206、207、208和209)的残留状况。水体中PBDEs的质量浓度为0.344~68.0 ng·L-1。PBDEs的组成分析结果表明:珠江水体PBDEs的来源以土壤和沉积物源为主,而目前珠三角陆地环境中PBDEs仍不断蓄积,其通过珠江地表径流迁移转换的PBDEs将逐年增多,给珠三角水生态环境带来的压力逐日增加,所造成的生态环境及公众健康影响将是深远的。  相似文献   

13.
Herein, we studied the occurrence and profiles of thirteen PBDE congeners in 30 river sediment samples from Shanghai, China. The concentrations of Σ13PBDEs ranged from 110 to 13,071 pg g ?1 dw, with an average value of 2,841 pg g ?1 dw. BDE-209 was the predominant congener accounting for more than 65 % of total PBDEs, demonstrating that the major source of PBDEs in sediment samples was associated with the prevalent use of technical deca-BDE products. Moreover, low brominated BDEs in sediments also came from the degradation of higher brominated BDEs. In addition, taking into consideration of dietary exposure, PBDEs in serum samples collected from the locals were also detected with range of 419–26,744 pg g?1 (average 5,561 pg g ?1), which suggested a relatively low burden of PBDEs contamination to human body compared with the condition in other place. And in serum, low brominated compounds constituted the majority of total PBDE congeners.  相似文献   

14.
Human breast milk samples, collected during April 2007 in Tabriz, Iran, were analyzed for organochlorine (OC) pesticides, such as dichlorodiphenyltrichloroethane (DDT) and its metabolites, hexachlorobenzene (HCB), α, β, and γ-hexachlorocycloexane (HCH) isomers and six polychlorinated biphenyls (PCB) congeners (IUPAC Nos. 28, 52, 101, 138, 153, and 180). Organochlorine pesticides and OCB were both prevalent in the samples of human breast milk. Average concentrations of HCB, DDT, HCH, and PCB were 1020, 1930, 1660, and 690 ng g?1 lipid weight, respectively. A positive correlation was observed between concentration of OC in human breast milk and mothers age with primiparae. Women having higher OC concentrations than multiparae women suggests that these parameters influence the OC burden in lactating women. The estimated tolerable daily intakes (TDIs) of HCH, HCB and PCB solely from human breast milk were 100, 46, and 43% of samples, respectively, exceeding guideline thresholds given as TDI proposed by Health Canada. Although high daily intakes may raise concerns for possible adverse effects of OC, women in Tabriz are recommended to breastfeed due to the numerous advantages for mother and child.  相似文献   

15.
研究了6种多氯联苯(PCBs)3,3′,4,4′-四氯联苯(PCB77)、2,3,3′,4,4′-五氯联苯(PCB105)、2,3′,4,4′,5-五氯联苯(PCB118)、3,3′,4,4′,5-五氯联苯(PCB126)、2,3,3',4,4',5-六氯联苯(PCB156)和商业型混合多氯联苯Aroclor1254,两种多溴联苯醚(PBDEs)2,2′,4,4′-四溴二苯醚(PBDE47)、十溴二苯醚(PBDE209)对人类癌细胞生长和斑马鱼脱膜与不脱膜胚胎发育的影响.8种化合物均使用0.01、0.1、1.0、10μmol·L-14个浓度进行1~6d的暴露实验.结果表明,PBDE209在最高浓度10μmol·L-1下对结肠癌细胞HCT116(暴露3d后)和RKO(暴露5d后)具有显著的生长抑制作用,所有化合物均对乳腺癌细胞没有显著影响.相比之下,化合物对受精后5~6h(5~6hpf)的斑马鱼胚胎的毒性效应显得比较明显,而各化合物对胚胎的致畸和致死效应又不相同,其毒性强弱依次为PCB126≈PCB156>PCB1254(Aroclor1254)>PBDE47>PCB77>PCB105≈PCB118≈PBDE209.其中PBDE209在未脱膜暴毒后均无致畸与致死现象,脱膜暴毒后最高浓度才表现出显著意义的致畸作用,而PBDE47在最高浓度下可产生高达80%的致畸率,这说明胚胎绒毛膜具有有效阻挡大分子物质如PBDE209进入的作用.PCBs的毒性效应与其空间结构密切相关.如PCB126和PCB105具有相同的分子式,前者在1μmol·L-1下就引起了显著的致死和致畸效应,而后者即使在10μmol·L-1下也没有显著的效应.实验结果也说明不同类型的实验对象所展示的毒性效应并不相同,化合物对体外培养的细胞和发育中的胚胎具有不同的影响.  相似文献   

16.
Samples of groundwater, river water, river sediment, paddy soil, rice seeds, hen eggs, fish, umbilical cord blood, and newborn meconium were collected from October 2002 to October 2003 near a large site in China used for the disassembly of obsolete transformers and other electronic or electrical waste. Six indicator PCB congeners, three non-ortho dioxin-like PCB congeners, and six organochlorine pesticides were determined in the samples by GC with electron capture detector. The results demonstrated that the local environment and edible foods had been seriously polluted by toxic PCBs and organochlorine pesticides. The actual daily intakes (ADIs) of these pollutants were estimated for local residents living in the area. The intake data showed that the contents of PCBs in these local residents were substantial, as the ADI estimates greatly exceed the reference doses set by the World Health Organization and the United States Agency for Toxic Substances and Disease Registry. The presence of the indicator PCB congeners in the cord blood and the meconium samples, as well as significant correlations (r 2 > 0.80, p < 0.05) between these levels, suggests a potential biotransfer of these indicators from mothers to their newborns. This preliminary study showed that obsolete transformers and other electronic or electrical waste can be an important source for the emission of persistent organic pollutants into the local environment, such as through leakage, evaporation, runoff, and leaching. Contamination from this source appears to have reached the level considered to be a serious threat to environmental and human health around the disassembly site.  相似文献   

17.

Background

Since 1990, every 5 years, moss sampling is conducted within the European moss monitoring programme to assess the atmospheric deposition of airborne pollutants. Besides many other countries, Germany takes regularly part at these evaluations. Within the European moss monitoring 2015, more than 400 moss samples across Germany were taken according to a harmonized methodology for the assessment heavy metal and nitrogen input. In a pilot programme, eight of these sites were chosen for additional investigations on a broad range of organic contaminants to evaluate their accumulation in moss and thereby their presence in atmospheric deposition in Germany. Target compound classes comprised polycyclic aromatic hydrocarbons (PAH), polychlorinated dibenzodioxins and –furans (PCDD/F), dioxin-like and non-dioxin-like polychlorinated biphenyls (dl-PCB, ndl-PCB), polyfluorinated alkyl substances, classical flame retardants as well as emerging chlorinated and brominated flame retardants. In total, 120 target compounds were analysed. For some analytes, comparisons of accumulation in moss and tree leave samples were possible.

Results

Except for certain flame retardants, PFAS, and ndl-PCB, substances of all other compound classes could be quantified in moss samples of all sites. Concentrations were highest for PAH (40–268 ng g?1) followed by emerging flame retardants (0.5–7.7 ng g?1), polybrominated diphenyl ethers (PBDE; 0.3–3.7 ng g?1), hexabromocyclododecane (HBCD; 0.3–1.2 ng g?1), dl-PCB (0.04–0.4 ng g?1) and PCDD/F (0.008–0.06 ng g?1).

Conclusions

Results show the widespread atmospheric distribution and deposition of organic contaminants across Germany as well as the suitability of moss as bioaccumulation monitor for most of these compound classes. Compared to nearby tree leaf samples, accumulation potential of moss appeared to be higher for pollutants of high octanol–air partition coefficient (KOA) and octanol–water partition coefficient (KOW).
  相似文献   

18.
As one of China’s great metropolises, Shanghai is suffering from the impact of manufacture and the use of chemical industrial products, and it faces serious pollution from polychlorinated biphenyls (PCBs). Therefore, in this study, in order to assess the seasonal and spatial character of contamination from chemical industrial zones, the concentrations of PCBs have been measured in various environmental media, including soil, leaves, and atmospheric particulate samples collected in a chemical industrial zone of Shanghai and compared with samples from presumably unpolluted sites of rural areas. In soils, the PCB concentrations ranged from 0.5 ng g−1 (unpolluted site) to 586.85 ng g−1 (chlor-alkali industry site). The concentrations of PCBs in evergreen leaves ranged from 0.3 ng g−1 to 32.46 ng g−1, and more chlorinated biphenyls congeners, such as penta-biphenyls and hexa-biphenyls, were the dominant contributors in winter and spring. Seasonal differences and the constitution patterns of congeners might be affected by the temperature and industrial activities. The PCB concentrations in the leaves of deciduous trees increase over time as the leaves grow. The PCB concentration in atmospheric particulates was in the range of 9.22–14.15 × 103 pg m−3, which might be the result of influence from climate and industrial activities. The relativity of PCB contents among the environmental media was discussed. The results in this paper provide an important profile of the current contamination status of a key chemical industrial zone in China.  相似文献   

19.
Polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) were analysed in surface soil samples collected in 2001–2002 at an open urban area of Madrid. In order to obtain representative samples, three collection points at the site were chosen. The most abundant PAHs and PCBs were phenanthrene, fluorene, pyrene, chrysene and benzo[a]pyrene and hexa- and heptachlorinated PCBs, respectively. The sum of selected PAHs (13 compounds) and PCBs (15 congeners) averaged 1 and 0.1?µg?g?1, respectively. PCB levels in winter were 2–10 times higher than summer ones, while seasonal variation for most of PAHs were not observed. Good correlations among all PCBs were found. Five PAHs were also well correlated.  相似文献   

20.
Xu  Jing  Qian  Wangyang  Li  Juying  Zhang  Xiaofei  He  Jian  Kong  Deyang 《Environmental geochemistry and health》2019,41(5):2315-2327

Polybrominated diphenyl ethers (PBDEs) are a class of organic pollutants. They are used as flame retardants that caused worldwide environmental concern. This study investigated the occurrence of PBDEs in soils and dusts from three plastic manufacture plants and surrounding areas in Eastern China. A total of 13 PBDE congeners were detected using gas chromatography-mass spectrometer (electron impact ionization). The total concentrations of PBDEs range from 2.21 to 558, 19.7–4916, and 8.70–18,451 ng/g dry weight in the soils of three sampling areas, with mean of 1004 ng/g d w; in dusts, the concentrations range from 7240 to 10,469, 684–4482, and 193–3989 ng/g d w, with an overall mean of 3619 ng/g d w. The most abundant congener is the BDE-209, followed by BDE-153 and BDE-85. This indicates that the brominated flame retardant added in the plastic manufacture is mainly the commodity decabromodiphenyl ether. In comparison with other polluted areas around the world, the PBDE concentrations in the soils of the plastic manufacture plants are similar to those in soils of waste plastic disposal areas and PBDEs production sites, but orders of magnitude higher than those in agricultural soils, mountain soils and rural soils. Daily exposure was estimated using the average concentrations of the pollution sites. The hazard quotient shows that the PBDEs pose considerable human health risks, especially to children, to which attention should be paid.

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