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1.
Polychlorinated biphenyls (PCBs) are among the most toxic environmental pollutants. Food, especially animal based, has been described as the major source for human exposure to PCBs. We investigated PCB levels (congeners 10, 28, 52, 153, 138, and 180) in cheese from 14 cities of Rio Grande do Sul, Brazil. The fat was extracted using sodium sulfate and petroleum ether, and PCBs purification was conducted using florisil and hexane. The identification and quantification were made in a gas chromatograph with microelectron capture detector (GC-microECD). PCB congeners were found (lower bound data as ngg(-1) fat) in the following rank: 52 (15.75)>180 (4.91)>28 (3.43)>153 (3.00)>10 (2.38)>138 (1.37). Summation operatorPCB contamination ranged from 0 to 78.32 ngg(-1) fat. Differences in PCB levels between industrialized (33.32 ngg(-1) fat) and homemade (26.58 ngg(-1) fat) cheese and between two different regions (36.19 vs. 26.95 ngg(-1) fat) were not statistically significant. For university students, the estimated daily intake (EDI) of PCBs from cheese ranged from 0 to 3.13 pgkg(-1) b.w. EDI was significantly higher for industrialized than homemade cheese, and for cheese from Mountain/Porto Alegre region than from Santa Maria/South/Western region. No sample exceeded maximum level of PCBs allowed in dairy products in the European Community.  相似文献   

2.
Patterns of contamination by polychlorinated biphenyls (PCBs) were investigated in fourteen samples of coastal sediments from Hong Kong. Congener-specific analyses revealed nine sediment samples from Junk Bay to contain PCBs at concentrations ranging from 31 to 2200 ng g(-1) dry weight, concentrations generally increasing with distance north in the Bay. By contrast, five sediments from the Tolo area to the north-east of Hong Kong exhibited total PCB levels of only 6.6 to 45 ng g(-) dry weight. The patterns of relative abundance of PCB congeners in the northern Junk Bay sediments suggested the existence of ongoing source(s) of PCBs in this area; biphenyls of lower chlorination were present at high concentration in these samples. Three coplanar PCBs (3', 4, 4'-tetrachlorobiphenyl; 3,3',4,4',5-pentachlorobiphenyl; and 3,3',4,4',5,5'-hexachlorobiphenyl) were found to be present in Junk Bay sediments; these are highly toxic and are cause for concern in aquatic environments. The abundance of the three coplanar PCBs in the sediments studied was similar to that in commercial PCB mixtures, suggesting that these congeners are not enriched over other PCBs by the sediments of coastal ecosystems. It is concluded that the preferential enrichment of coplanar PCBs occurs in the biosphere, rather than in sediments.  相似文献   

3.
Persistent organochlorines, such as polychlorinated biphenyls including coplanar congeners and DDT compounds were measured in the liver of different species of mollusc cephalopods: broadtail squid (Illex coindetii), horned octopus (Eledone moschata) and spider octopus (Octopus salutii) collected in two different areas of the Adriatic Sea (central and southern Adriatic Sea). The concentration of PCBs exceeded DDT ones in horned octopus (PCBs: 617.0 ngg(-1) lipid weight, DDTs: 188.0 ngg(-1) lipid weight) and in spider octopus (PCBs: 590.0 ngg(-1) lipid weight, DDTs: 293.0 ngg(-1) lipid weight), while in broadtail squid PCB load (748.0 ngg(-1) lipid weight) was similar to those of DDTs (514.5 ngg(-1) lipid weight). No significant difference in PCB levels was observed among species, while DDT concentrations were higher in broadtail squid than in horned octopus and spider octopus. DDTs composition showed slight differences in relation to species, thought p,p'-DDE was the predominant compound in all cephalopod species (broadtail squid: 88.1%, horned octopus 94.1%, spider octopus: 97.5%). PCB isomer profiles were similar among species being hexachlorinated isomers the most abundant, followed by penta- and heptachlorobiphenyls, while tri- and tetrachlorobiphenyls made up a small percentage of the total PCB residues. Regarding coplanar congeners, non-ortho PCBs were below the detection limit in all samples and the 2,3,7,8-TCDD toxic equivalent (TEQ) concentrations were very low. The influence of biological and ecological factors (size/weight and location) on the bioaccumulation of organochlorine compounds has been discussed.  相似文献   

4.
Yang H  Xue B  Jin L  Zhou S  Liu W 《Chemosphere》2011,83(2):137-143
The spatial distribution and source of polychlorinated biphenyls (PCBs) in 30 surface sediments of Yueqing Bay, Xiangshan Bay, and Sanmen Bay in Eastern China were analysed. Total concentrations of PCBs ranged from 9.33 to 19.60 ng g−1 dry weight for all the sampling stations. The observed PCB levels were lower than those in areas of high urbanisation or contamination in the bay. Low-chlorinated PCBs, dominated by tri-PCB, were identified as the prevalent contaminate of surface sediments, and the top three PCB congeners were lighter chlorinated congeners (PCB 8, PCB 18 and PCB 28). These results were in agreement with the fact that tri-PCB compounds are the dominant contaminants in China. The result of the principal component analysis revealed that all samples were similar in composition to Aroclor 1242, suggesting they might originate from electrical capacitors and transformers. The levels of PCBs were significantly correlated with the total organic carbon in the sediments.  相似文献   

5.
Polychlorinated biphenyls (PCBs) contamination in tropical and sub-tropical areas and the associated risks have attracted great concern. A total of 69 samples representing five distinct land types were collected to assess PCB concentrations in the Pearl River Delta (PRD), South China, including spatial distributions in soils of the area, the probable anthropogenic sources, and related potential risks. PCBs concentrations in soils of the PRD ranged from 0.3 to 202 ng?g?1. More severe PCBs contamination was presented in the western part than in the eastern part of the PRD region. The PCBs were dominated by low-chlorinated biphenyls; however, the proportion of higher-chlorinated biphenyls was elevated with the influence of industrial activities. Principal component analysis indicated that PCBs contamination in soils of the PRD region was mainly associated with 1#PCBs, while 2#PCB and e-waste emission in South China also accounted for it partly, especially to the industrial activity severely impacted areas. Toxic equivalent (TEQ) of the dioxin-like PCBs in the soils indicated that higher risk of PCB contamination was presented in the Dongjiang River Valley (55 ng?TEQ?kg?1, on average) than in the Xijiang River Valley, and were mostly contributed by the congener of PCB126.  相似文献   

6.
Tan J  Cheng SM  Loganath A  Chong YS  Obbard JP 《Chemosphere》2007,68(9):1675-1682
Although the use of organochlorine pesticides (OCPs) and polychlorinated biphenyls (PCBs) has been prohibited in Singapore since 1980, OCPs and PCBs still can be detected in the environment and represent a potential threat to public health. In this study, OCPs and PCBs were measured in house dust samples collected from 31 homes across the island-state of Singapore. Organochlorine pesticides, such as hexachlorocyclohexanes (HCHs), chlordanes and dichlorodiphenyltrichloroethanes (DDTs) were tested, with a range of 相似文献   

7.
Monitoring of immission of persistent organic pollutants in the industrialized area of Volta Redonda (V.R.) and in the National Park of Itatiaia (PNI) in southeast Brazil was performed using an endemic bromeliad species as biomonitor and measuring bulk deposition rates of polychlorinated biphenyls (PCB) and polycyclic aromatic hydrocarbons (PAH). For the sum of PCB, overall deposition rates were between 17 and 314 ng/(m2 day) in winter and between 43 and 81 ng/(m2 day) in summer, respectively. Deposition rates of dioxin-like PCBs ranged from 0.14 to 2.8 pg WHO-TEQ/(m2 day) in winter and from 0.90 to 4.3 pg WHO-TEQ/(m2 day) in summer. PCB deposition rates (total PCB and WHO-TEQ) were in the same range in winter in V.R. and PNI. In summer, contamination levels in V.R. were 6-10-folds higher than in PNI. PCB concentrations in biomonitor samples from V.R. and PNI were in the same range in summer and in winter. Concentrations of total PCB ranged from 14 to 95 microg/kg dry matter (d.m.) in winter and from 18 to 27 microg/kg d.m. in summer, respectively. The TEQ values were between 1.7 and 4.1 ng WHO-TEQ/kg d.m. in winter and between 1.9 and 2.9 ng WHO-TEQ/kg d.m. in summer. PCB concentrations of di-ortho PCB but not of non-ortho PCB were a factor of 2-4 lower in summer in both areas. PCB congener profiles resembled those from technical formulations. The profiles shifted to the higher chlorinated congeners in summer, probable due to revolatilisation of the lighter components at higher temperatures. PCB profiles in biomonitor resembled those from deposition samples and the shift to the heavier congeners in summer was even more pronounced. PAH deposition rates were in a similar range in both areas (131-2415 ng/(m2 day)). PAH levels in biomonitor samples from V.R. were about one order of magnitude higher than in samples from PNI indicating the impact of local sources. PAH profiles revealed stationary thermal processes as main source of contamination in V.R. whereas in PNI, biomass burning seems to be the main contamination source.  相似文献   

8.
The purpose of this study was to investigate polychlorinated biphenyls (PCBs) contamination in tilapia (Oreochromis mossambicus) collected from the Manoa stream and Ala Wai Canal of O'ahu, an island of the geographically isolated Hawaiian archipelago. Our results show that the average concentrations of PCBs varied from 51.90 to 89.42 ng g(-1) lipid weight for the sampling sites. Relative toxic potencies (RTPs) and toxic equivalencies (TEQs) were determined to be 20.38-40.60 ng TCDDg(-1) lipid weight and 2.89-4.17 ng TEQ g(-1) lipid weight by 7-ethoxy-resorufin-O-deethylase (EROD) activity analysis and calculation of PCB concentrations based on toxic equivalency factors (TEFs), respectively. Penta-chlorinated congeners were found to be predominant, which revealed that Aroclor 1254 was a possible major source of PCBs in our fish samples. PCB 118, an indicator PCBs, constituted more than 55% and 30% of the total PCBs and TEQs, respectively. In addition, PCB 118 was found to have a linear correlation to the total PCBs (R=0.975) and TEQs (R=0.782). Detection of concentrated PCBs in Hawaiian waters suggests a potentially adverse impact of this pollutant on human health, as well as ecological systems, and suggests the necessity of environmental monitoring and hazard assessment of PCBs within the Hawaiian Islands.  相似文献   

9.
Zhang L  Shi S  Dong L  Zhang T  Zhou L  Huang Y 《Chemosphere》2011,85(3):399-405
In this study, polychlorinated biphenyls (PCBs) pollution in the surface water of the Yangtze River Delta (YRD) was investigated. A total of 26 samples were collected from water bodies in three cities within the YRD during the dry season from October to November of 2009. The total PCBs (dissolved plus particulate) ranged from 1.23 to 16.6 ng L(-1) and were dominated by tri-, tetra-, and penta-chlorinated biphenyls. The mean PCBs in the Beijing-Hangzhou Grand Canal and the Yangtze River were 8.84 and 3.36 ng L(-1), respectively. A t-test showed that there were no significant differences in the concentration of samples from the metropolitan area and the development zone. According to the Chinese national environmental quality standards for surface water (GB 3838-2002), the concentrations of PCBs observed in this study do not pose a hazard to aquatic or human health. Overall, this study described the PCB concentration and homolog distribution patterns in one of the most rapidly developing areas in China, and the results can be used as reference levels for future PCB monitoring programs.  相似文献   

10.
Tonghui River, a typical river in Beijing, People's Republic of China, was studied for its water and sediment quality, by determining the levels of 16 polycyclic aromatic hydrocarbons (PAHs), 12 polychlorinated biphenyls (PCBs) and 18 organochlorine pesticides in water and sediment samples. Total PAHs, PCBs and organochlorine pesticides concentrations in water varied from 192.5 to 2651 ng/l, 31.58-344.9 ng/l and 134.9-3788 ng/l, respectively. The total PAHs, PCBs and organochlorine pesticides concentrations in surficial sediments were 127-928 ng/g, 0.78-8.47 ng/g and 1.79-13.98 ng/g dry weight, respectively. The results showed that the concentration of these selected organic pollutants in sediment was higher than those in surface water. It may be due to the fact that organic hydrophobic pollutants tend to stay in the sediments. The PAHs were dominated by 2-, 3-ring components in water samples and by 3- and 4-ring compounds in sediment. For organochlorines, alpha-HCH, delta-HCH, Heptachlor, Endosulfan II, DDT are the major organochlorine pesticides in water while Heptachlor, Dieldrin and DDE composed of 95% of total organochlorine pesticides in sediment. For HCHs (HCHs=alpha-HCH+beta-HCH+gamma-HCH+delta-HCH), the predominance of alpha-HCH of total HCHs were clearly observed in water and sediment. PCB18, PCB31 and PCB52 were predominant in water, on average these compounds collectively accounted for 67% of total PCBs. But in sediment, the predominant compounds were PCB28, PCB31 and PCB153, which accounted for 71% of total PCBs in sediment. The levels of micro pollutants in our study areas were compared with other studies.  相似文献   

11.
Levels of polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs) were measured in paired human adipose tissue and liver samples (n=25) from Belgium. Average concentrations and standard deviation of sum PBDEs (congeners 28, 47, 99, 100, 153, 154 and 183) were 5.3+/-3.0 (range 1.4-13.2) and 3.6+/-2.1 (range 1.0-10.0)ngg(-1) lipid weight (lw) in adipose tissue and liver, respectively. These concentrations were similar to reported PBDE data from Belgium and were at the lower end of the concentration range reported elsewhere in the world. In both tissues under study, BDE 153 and BDE 47 were the most abundant PBDE congeners, contributing approximately 35% and 25% to the total PBDE content. Average concentrations and range of PCBs (sum of 23 congeners) were 490 (range 70-1130) and 380 (range 90-1140)ngg(-1)lw in adipose tissue and liver, respectively. No correlation between age and concentrations of PBDEs could be found (r=0.04), while PCB concentrations correlated significantly with age (r=0.62, p<0.01, for the sum PCBs; r=0.64, p<0.01 for PCB 153 alone). Factors, such as exposure pathways (food, dust and air), rates of bioaccumulation, metabolism and elimination, influence the concentrations of PBDEs differently than those of PCBs in humans.  相似文献   

12.
Hydrophobic organic contaminants (HOC) (i.e. PAHs and PCBs) were measured in the water column and in Eurytemora affinis samples from the Seine Estuary collected from November 2002 to February 2005. Results showed seasonal variations of both total PCB and PAH levels in the suspended particulate matter (SPM) and in the copepods with maximum levels during winter times. PAH and PCB concentrations in the SPM ranged from 499 to 5819ngg(-1) and from 58 to 463ngg(-1), respectively. Phenanthrene, pyrene and benzo[b+j+k]fluoranthene (B[b+j+k]F) were the predominant PAH compounds in the water column, while CB 101, 118, 153 and 138 were the most abundant PCB congeners. PCBs and PAHs bioaccumulated by E. affinis (EA) varied between 383 and 1785ngg(-1) and 165-3866ngg(-1). CB101, 153, 138 and B[b+j+k] were, respectively, the major compounds of PCB and PAH fingerprints in EA. Thereby, the copepods could reach high accumulation factor (ACF) (91000 for PCBs and 17000 for PAHs). The principal component analyses of contaminant concentrations and environmental parameter datasets distinguished two groups of copepods. The winter time cluster, with high percentage of adult copepods, which bioaccumulated the highest PCB and PAH body-burdens, and the second cluster with juveniles showing the lowest HOC concentrations. Thus, PAH and PCB concentrations in EA exhibited significant correlations with the percentage of adults making up the samples.  相似文献   

13.
Hong SH  Yim UH  Shim WJ  Li DH  Oh JR 《Chemosphere》2006,64(9):1479-1488
To assess the organochlorine contamination in the Korean marine environment, a nationwide monitoring study was conducted. A total of 138 surface sediments, covering the whole Korean coast, were collected and analyzed. Organochlorine compounds (OCs) were widely distributed in the Korean coastal environment, with PCB and DDT contamination being particularly prevalent. The overall concentrations of PCBs, DDTs, HCHs, CHLs, and HCB in surface sediments were in the range of 0.088-199ngg(-1) (median value: 1.56ngg(-1)), 0.006-135ngg(-1) (0.68ngg(-1)), not detected (ND)-5.46ngg(-1) (0.32ngg(-1)), ND-3.26ngg(-1) (0.14ngg(-1)), and ND-2.59ngg(-1) (0.05ngg(-1)), respectively. The southeastern coast was found to be highly contaminated. Overall contamination status of Korean coastal sediments with regard to OCs is lower than that of USA. With the exception of highly industrialized sites, Korean coastal areas in general showed similar OC concentrations to those of other Asian countries. There was a significant correlation between distributions of most organochlorine contaminants with each other. OC contamination is closely related to shipping and industrial activities. Of the 7 sites categorized as highly polluted, 4 are in a harbor zone. Adverse effects to benthic communities are expected at the levels of OC contamination observed from harbor and industrial areas.  相似文献   

14.
The concentrations of gas-phase polychlorinated biphenyls (PCBs) in the atmosphere of the Camden, NJ, USA are elevated by as much as 20 times over regional background. These high PCB levels are a concern because they lead to atmospheric deposition loadings of PCBs to the tidal Delaware River that exceed the entire total maximum daily load (TMDL). Two models were applied to the atmospheric PCB concentration data from Camden in an attempt to identify the PCB source types and regions. Positive matrix factorization (PMF) was used to identify the source types. Four factors were identified which are thought to represent sources such as volatilized Aroclors and particle-phase PCBs. The potential source contribution function (PSCF) model was then used to identify the geographic source regions by examining the origination points for air parcels that result in high PCB concentrations at the Camden receptor site. The PSCF model for ΣPCBs indicates PCB source regions throughout the Philadelphia–Camden metro area, including portions of both Pennsylvania and New Jersey. The PSCF plots for the resolved PMF factors suggest that factors 1–4 show fewer distinct source regions, indicating that their sources are diffuse and/or lie very close to the receptor site. The PSCF plots for factors 2 and 3 reveal very different source regions. Factor 2 primarily arises from the city of Philadelphia, whereas factor 3 originates in southern New Jersey and south of Philadelphia. This study demonstrates the utility of the combined PMF/PSCF approach in identifying atmospheric PCB source types and regions.  相似文献   

15.
Jiang Y  Wang X  Zhu K  Wu M  Sheng G  Fu J 《Chemosphere》2011,83(6):767-773
Surface soil samples taken from 55 sampling sites at the urban areas of Shanghai were collected and analyzed for the occurrence of 144 polychlorinated biphenyls (PCBs) by GC-μECD. The results showed that totally 74 PCB congeners were identified and the mean concentration of total PCBs was 3057 ng kg−1 with a range of 232 to 11325 ng kg−1. Compared with the related reports, the level of PCBs contamination in this study was approximately equal to the global background value in soils, but higher than Chinese background for rural and urban soils. According to the compositional profiles of PCBs homologues, a higher proportion of low chlorinated (from tri-CBs to hexa-CBs) was observed. The results indicated that PCB15 + 13, PCB18, PCB28, PCB104 + 47 and PCB153 were the most dominant congeners among the identified PCBs. Through homologues analysis, cluster analysis and principal component analysis (PCA), it was found that PCBs were stretched from mixed local sources, and appeared to be mostly originated by Aroclor 1260- and 1254-like mixtures as well as some samples influenced by Aroclor 1232 and 1242. The correlation analysis showed the relatively good correlation among the PCB homologues and soil total organic carbon (TOC), suggesting important influence of soil TOC on PCBs contamination in soil matrix in Shanghai region. The toxic equivalency (TEQ) concentrations of these six dioxin-like PCBs detected in urban soil samples range from 2.71 to 24.9 pg kg−1-PCDDeq with a mean 8.18 pg kg−1-PCDDeq.  相似文献   

16.
This study investigated the contamination levels, homologue, and congener profiles and evaluated the residue inventory of polychlorinated biphenyls (PCBs) in sediment of the Songhua River in the vicinity of cement plant. The total concentration of detected 35 PCB congeners ranged from 1.12 to 2.19 ng/g dry weight (dw) in sediment, with a mean value of 1.56 ng/g dw, and the concentration of PCBs decreased in the following order: the downstream?>?cement plant?>?upstream. The results of total organic carbon (TOC)-normalized PCB concentrations indicate that the sediments have low potential ecological risk in this area. The study results on homologue and congener of PCBs show that the emissions from cement production could be the major sources of PCBs in sediment, and the low-chlorinated PCBs will be exchanged among air, water, and sediment with increasing temperature during summer and flow to downstream with water during the wet season. The spatial density and total burden of PCBs in the surface sediments were 17.2 ng/cm2 and 1.2 kg, respectively. To our knowledge, this study is the first to explore the pollution characteristics of unintentionally produced PCB emissions from cement industry by means of monitoring sediment samples.  相似文献   

17.
Katsoyiannis A 《Chemosphere》2006,65(9):1551-1561
The occurrence of polychlorinated biphenyls (PCBs) was investigated in the Soulou stream in the area of Eordea, northwestern Greece, receiving the effluents of two lignite burning power plants. The study was carried out after an accidental fire in one of the power plants during which losses of an amount of Aroclor 1232 were recorded. PCBs were determined in water and sediment samples collected from the wastewater treatment unit of the power plant and various points across the stream. Concentrations of PCBs were in the same order of magnitude as in other surface waters and sediments previously found in the Greek territory. The sum concentrations of seven PCBs (#28, #52, #101, #118, #138, #153, #180) varied between 94 and 206 ngl(-1) in waters, and between 67 and 500 ngg(-1) in sediments. Profile analysis of PCB congeners revealed large differences between waters and sediments, showing also significant dissimilarity with the profile of Aroclor 1232.  相似文献   

18.
Although atmospheric deposition is generally the dominant pathway of PCBs into agricultural food chains, soil ingestion by livestock can be important in some cases. The relationship between PCB levels in cow's milk and in pasture soil was studied in the Irkutsk region in Siberia where an historical atmospheric source(s) of PCBs has led to widespread contamination of soil. Milk samples were collected in spring and again in autumn from 18 different farms and analyzed for PCBs. Pasture soil samples were also collected and analyzed. The PCB concentrations in both milk and soil ranged over more than an order of magnitude between the farms. A good correlation was obtained between PCB levels in autumn milk and in soil. This together with a range of other evidence suggested that ingestion of pasture soil was the dominant source of the PCB contamination in the milk. The average soil ingestion rate was estimated to be 1700 g/d, which is at the upper end of values reported in the literature. This may be due to the arid summer climate or the animal husbandry practices in Siberia.  相似文献   

19.
Abstract

The development of high-resolution mass spectrometry methods for the measurement of polychlorinated biphenyls (PCBs) in environmental samples has dramatically reduced detection limits, leading to problems obtaining clean blanks. When PCBs are detected in samples at concentrations similar to the blanks, blank contamination must be addressed before fingerprinting and source apportionment through positive matrix factorization (PMF) can be successful. We tested a variety of blank correction methods using data from a study of water column concentrations of PCBs in the Spokane River, where concentrations of Σ209PCBs in whole water samples averaged 171?pg/L without blank correction and Σ209PCBs in the blanks averaged 88?pg/L. The results suggest that subtracting blank masses from sample masses can lead to erroneous results. Instead, censoring at one times the batch-specific blank level is a better approach. The sources of PCBs in field and method blanks were investigated by examining their congener profiles via PMF. The results suggest that commercial PCB formulations (in the US, Aroclors) continue to be the primary source of PCBs in blanks forty years after PCB production and use were banned in the United States. Other sources of PCBs to blanks include PCB 11 from pigments; PCBs 44?+?47?+?65, 45?+?51, and 68 arising from polymers cured using bis(2,4-dichlorobenzoyl) peroxide; and PCBs 1, 2, 3, 4, 8, 15 and others arising from silicone products derived from phenylsiloxanes, such as silicone-based adhesives.  相似文献   

20.
Sediments from Niagara River, an important waterway connecting two of the Great Lakes (Lake Erie to Lake Ontario), were analyzed for 14 congeners of polychlorinated biphenyls (PCBs) and 9 congeners of polybrominated diphenyl ethers (PBDEs) using accelerated solvent extraction and gas chromatography/mass spectrometry. Total concentrations of PCBs ranged from 1.7 to 124.6 ng/g were PCBs 138 and 153 were found in all samples. All sites but one showed PBDE in sediments with total concentrations as high as 148 ng/g, suggesting that PBDE is becoming an important class of POP. A land-use and coverage map was used to trace potential localized sources of PCB and PBDE contamination. Results indicate that the highest levels of PCBs and PBDEs were found in sediments collected from areas closest to the discharge locations of municipal wastewater treatment plants (WWTP) and local industries. This is the first study that suggests the importance of WWTP discharges as a potential source of PBDE contamination in the Great Lakes.  相似文献   

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