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The present study investigated contamination of polybrominated diphenyl ethers (PBDEs) in sediment and fish samples collected from rivers in Guiyu, China where electronic waste (e-waste) is recycled and disposed. PBDE congeners with mono-to hepta-brominated and deca-brominated substitutions were detected using (13)C(12) isotope dilution GC/MS/MS and GC/MS methods, respectively. The total PBDE concentrations ranged from 4434 to 16088 ng/g (dry weight) in Nanyang River bank sediment, from 55 to 445 ng/g in Nanyang River bottom sediment and 51.3 to 365 ng/g in Lianjiang River bottom sediment in Guiyu compared with those from 16.1 to 21.4 ng/g in wastewater discharged from a vehicle repairing workshop in Lo Uk Tsuen in Hong Kong. No PBDE congeners were detected in bottom sediment and fish from Mai Po Marshes in Hong Kong. The mean concentrations of total PBDEs in mixed muscles of tilapia (Oreochromis spp) from Lianjiang River were 115 ng/g wet weight (ww) and from wastewater in Hong Kong were 4.1 ng/g ww. Highest mean PBDE concentration was obtained in liver (2687 ng/g ww), followed by abdomen muscle (1088 ng/g ww) of bighead carp (Aristichthys nobilis) collected from Nanyang River. A significant correlation of concentration of each PBDE congener between sediment and muscle from Guiyu was observed. The present results of total PBDEs in sediment and fish were 10 and 1000 times higher than other studies. Open burning and dumping of e-waste are the major causes of PBDE contamination.

Background: Little is known about the rates of loss (depuration) of polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs) from mothers during lactation. Depuration rates affect infant exposure to chemicals during breast-feeding, and fetal and lactational transfers during subsequent pregnancies., Objective: Our objective in this study was to estimate depuration rates of PBDEs and PCBs using serial samples of breast milk., Method: Nine first-time mothers (primiparae) each collected samples at 4, 6, 8, 12, 16, 20, and 24 weeks after birth. Nine additional primiparae each collected two samples at varying time intervals (18 to > 85 weeks after birth). Analytical precision was assessed to evaluate the accuracy of measured monthly percentage declines in PBDEs and PCBs., Results: The four major PBDE congeners decreased 2 or 3% +/- 1% per month over the 6-month period. These decreases were consistent over a 50-fold range (21-1,330 ng/g lipid weight) of initial PBDE concentrations in breast milk. The change in PCB-153 ranged from + 0.3% to -0.6% per month, with heterogeneous slopes and greater intraindividual variability. PBDE and PCB concentrations declined 1% per month over longer periods (up to 136 weeks)., Conclusions: Our data indicate that PBDEs and PCBs are not substantially (4-18%) reduced in primiparae after 6 months of breast-feeding. Consequently, the fetal and lactational exposures for a second child may not be markedly lower than those for the first. Participants were volunteers from a larger study population (n = 82), and were typical in their PBDE/PCB levels and in many demographic and lifestyle factors. These similarities suggest that our results may have broader applicability.

Southern sea otters (Enhydra lutris nereis) from the California coast continue to exhibit a slower population regrowth rate than the population in Alaska. Infectious diseases have been identified as a frequent cause of death. Infectious diseases caused by varied pathogens including bacteria, fungi, and parasites were suggestive of compromised immunological health of mature animals in this population. To test the hypothesis that elevated exposure to immunotoxic contaminants such as polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs) contribute to disease susceptibility via immunosuppression, we determined concentrations of PBDEs and PCBs in livers of 80 adult female sea otters that died of infectious diseases, noninfectious causes, or emaciation. Concentrations of PBDEs and PCBs in sea otter livers varied widely (10-26,800 ng/g and 81-210,000 ng/g, lipid weight, respectively). Concentrations of PBDEs in sea otters were some of the highest values reported for marine mammals so far. Although PCB concentrations in sea otters have declined during 1992-2002, the mean concentration was at the threshold at which adverse health effects are elicited. Concentrations of PBDEs and PCBs were significantly correlated, suggesting co-exposure of these contaminants in sea otters. No significant association was found between the concentrations of PBDEs and the health status of sea otters. Concentrations of PCBs were significantly higher in otters in the infectious disease category than in the noninfectious category, suggesting an association between elevated PCB concentrations and infectious diseases in Southern sea otters.

Polychlorinated biphenyls (PCBs) and the structurally related polybrominated diphenyl ethers (PBDEs) have been associated with chronic neurotoxicity involving reduced motor activity and impaired attentiveness. Such neurobehavioral effects indicate that the central nervous system may represent an important target organ for the action of these persistent contaminants in wildlife. As a consequence, the brain of different terrestrial and aquatic birds collected in Switzerland was analysed for PCBs and PBDEs. In parallel, the same contaminants were examined in the accompanying adipose tissue. After clean-up by means of glass columns containing acidified silica, deactivated alumina and anhydrous sodium sulphate, the samples were analysed by high resolution gas chromatography/tandem mass spectrometry (HRGC-MS/MS). Median PCB concentrations in the brain (sum of PCB 28, PCB 52, PCB 101, PCB 118, PCB 138, PCB 153 and PCB 180) ranged between 13 ng g(-1) wet weight (ww) in blackbirds (Turdus merula) and 428 ng g(-1) ww in sparrow hawks (Accipiter nisus). Median PBDE concentrations in the brain (sum of BDE 28, BDE 47, BDE 99, BDE 100, BDE 153, BDE 154 and BDE 183) ranged from below the decision limit in buzzards (Buteo buteo) and blackbirds, to 14 ng g(-1) ww in sparrow hawks. After correction for the respective lipid content, higher PCB or PBDE concentrations in brain compared to adipose tissue, were found in three sparrow hawks, four buzzards and in all investigated blackbirds. These results suggest that a deficit in the neuroprotective function of the blood-brain barrier may cause unexpected levels of PCBs and PBDEs in the central nervous system.

Polybrominated diphenyl ethers (PBDEs) are persistent, bioaccumulative, organohalogen compounds that are increasing exponentially in the Great Lakes (Canada/USA) biota. The present study was undertaken to examine the immunological effects of a commercial PBDE mixture in ranch mink (Mustela vison). Twenty-week-old mink (n = 10 mink/group) were exposed to 0, 1, 5, or 10 ppm of DE-71 through their diet for eight weeks. The phytohemagglutinin-induced cutaneous reaction, and antibodies specific to keyhole limpet hemocyanin conjugated to dinitrophenol were measured. Liver microsomal ethoxyresorufin-O-deethylase (EROD) activity also was measured. Organs were weighed and spleens were examined histologically. No differences were found in the PHA-induced skin response in exposed mink; mink in the two highest treatments exhibited significant increases in antibody production over control mink. Systemic toxicity was apparent; significant body weight reductions were found in mink exposed to 5 and 10 ppm of DE-71. Exposed mink had significantly larger relative spleen, adrenal, and liver masses than control mink. Spleens of mink exposed to 10 ppm of DE-71 had significantly increased germinal center development and incidence of B-cell hyperplasia. The activity of EROD was induced in all treated mink relative to controls and was positively associated with the liver somatic index. Hematocrit in mink from the two highest exposure groups was significantly lower than control mink. Percentage neutrophils increased and percentage lymphocytes decreased significantly in mink from the higher two dosage groups. Our findings have direct relevance to wild mink in the Great Lakes ecosystem, because mink are top predators of the aquatic food web, providing evidence for the vulnerability of this species to the effects of environmental PBDE mixtures.

The levels of selected polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs) were measured in human milk samples from the areas of Venice and Rome, primarily in order to characterize the current levels of infant exposure to PCBs and PBDEs due to breast feeding in Italy. Sixteen non-dioxin-like PCBs, including the traditional indicator congeners, and 11 PBDEs, comprising the relevant PBDE-47, PBDE-99, and PBDE-153, were determined. Congeners were selected for analysis according to their relative abundance in human tissues, toxicological relevance, and diffusion in the environment. Dietary habits of the milk donors were recorded by questionnaires; mothers of the Venice area were classified into three groups according to their consumption of local fish, molluscs, and other fishery products. Sigma(16)(PCBs) and Sigma(11)(PBDEs) (ng g(-1) fat) for the areas of Venice and Rome were respectively, 250-390 and 240, and 1.6-2.8 and 4.1. An increase of fish and fishery product consumption could not be associated with an increase of PCB and PBDE levels in milk.

In this study, the concentrations of polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs) in milk from women living in the vicinity of a new hazardous waste incinerator (HWI) in Catalonia, Spain, were determined. The study was performed after 4 years of regular operations in the facility and the present PCB levels were compared with baseline concentrations obtained in a pre-operational program. PCBs and PBDEs levels were determined by HRGC/HRMS in 15 samples. In the present study planar PCBs ranged from 1.3 to 6.3 pg WHO-TEQ/g fat with a mean value of 3.8 pg WHO-TEQ/g fat. After adding dioxin-like mono-ortho-PCBs the total PCB-TEQ concentrations ranged from 3.8 to 13.3 pg WHO-TEQ/g fat (mean value: 8.7 pg WHO-TEQ/g fat). A comparison of the current data with those obtained in the baseline study showed significant decreases for both planar and total WHO-TEQ of PCBs: 47.9% and 44.6%, respectively. PCB concentrations in milk of women living in urban zones were higher than those living near industrial areas (10.1 and 7.4 pg WHO-TEQ/g fat, respectively). Mean PBDE concentrations were 2.2 and 2.5 ng/g fat for women living in urban and industrial zones, respectively. Dietary intake of PCBs and PBDEs for a standard adult woman samples were 898 and 843 ng/day for PCBs, and 72 and 63 ng/day for PBDEs, for residents in urban and industrials areas, respectively. This study suggests that dietary intake is more relevant for human exposure to PCBs and PBDEs than living near the HWI.

Bioaccumulation factors (BAFs) were determined for (14)C-PCB 101 and (14)C-PBDE 99 in the pelagic copepod Calanus finmarchicus after exposure to either contaminated water or after being fed contaminated phytoplankton (the dinoflagellate Prorocentrum minimum or the diatom Thalassiosira weissflogii). BAFs in algae range from 7.6 to 8.0 for PCB 101 and from 8.5 to 8.6 for PBDE 99. BAFs in copepods were significantly lower, 6.3-6.8 for PCB 101 and 7.6 for PBDE 99. For each compound, the BAFs in copepods were independent of what algal species they had consumed, even though the bioaccumulation of both compounds were higher in P. minimum than in T. weissflogii. The ratios between BAF and the K(ow) for PCB 101 and PBDE 99 were similar within each of the three species, but varied between species. For copepods the ratios were 2-4, for T. weissfloggii 15-22 and for P. minimum 32-40. The data strongly suggest that the two compounds bioaccumulate in a similar manner and that there is no biomagnification in the transfer between phytoplankton and herbivorous copepods.

The concentrations of polybrominated diphenyl ethers (PBDEs) 17, 28, 47, 49, 66, 85, 99, 100, 153, 154, and 183 were determined in ringed seal blubber from central East Greenland collected in 1986, 1994, 1999 and during the period 2001 to 2004. The trend of PBDEs was compared with the trends of polychlorinated biphenyls (PCBs) 28, 31, 52, 101, 105, 118, 138, 153, 156, and 180 during the same period. The levels of sigmaPBDE in East Greenland ringed seals ranged from 21.8 ng g(-1) lipid weight (1w) in 1986 to 39.3 ng g(-1) lw in 2001 and are among the highest observed in ringed seal from the Arctic. The dominating congeners were BDE-47 (75.4%) and BDE-99 (9.7%). The concentrations of PBDEs and PCBs increased with the age of the seals, and therefore only young seals < or =4 years old) were included in the temporal trend analyses. No significant trend (p > 0.14) was observed in sigmaPBDE or the congeners BDE 28, 47 and, 99 during the period while sigmaPCB decreased significantly (p = 0.004) over the period from 1986 to 2004 with an estimated annual rate of 4.3%.

Biomagnification of polychlorinated biphenyls (PCBs) and polybrominated diphenylethers (PBDEs) in food webs from the Baltic Sea and the northern Atlantic Sea was investigated. For this, we used PCB and PBDE concentration data, together with data on fish body weight and delta15N of fish and zooplankton as a measure of trophic position. In the Baltic Sea material, consisting of zooplankton, sprat, herring and salmon, we report biomagnification of all PCB congeners but PCB #209 and of PBDEs with 3-6 or 7 bromine atoms. Higher brominated PBDEs and PCB 209 did not biomagnify likely due to their high molecular weights or sizes and subsequent inefficient dietary uptake in fish. If salmon was excluded from the statistical analysis, strong biomagnification of PCB #209 was evident, indicating species differences in biomagnification. In the Baltic Sea material delta15N and body weight covaried. In the Atlantic Sea material, consisting of fish samples (herring and salmon) of larger body sizes, we show positive correlation between concentrations of most PCBs and PBDEs and body weight without increasing delta15N. This shows that biomagnification in some cases depends on body size and not trophic position. We conclude that there probably is trophic position dependence in biomagnification, which was manifested in a food chain from zooplankton to piscivores, but no further trophic position influence on biomagnification in fish at the highest trophic levels. In these fish, there was a body size effect leading to biomagnification, probably due to slower clearance in larger fish. PCB concentrations were generally between 2 and 6 times higher in Baltic Sea salmon than in Atlantic Sea salmon. Higher PBDE concentrations in the Baltic compared to the Atlantic Sea salmon were also found, but with a larger variation between congeners. Nona- to deca-BDEs were found in most investigated samples, which illustrates the bioavailability of these compounds. Unidentified penta-, hexa-, hepta-, and octa- BDEs were found in several samples.

The biotransformation of high bromosubstituted polybrominated diphenyl ethers (PBDEs) congeners contained in a commercial deca mixture (DeBDE) is of environmental concern because it might lead to the increase of toxic low brominated PBDEs in biota. A few studies have reported that freshwater fish dietary exposed to DeBDE or its main constituent, decabrominated PBDE congener (BDE-209), had their tissues enriched with PBDEs not initially present in fish or feed. In the present study, Atlantic tomcod (Microgadus tomcod) were intraperitoneally (IP) injected with DeBDE to assess hepatic concentration changes of PBDEs and methoxy polybrominated diphenyl ethers (MeO-PBDEs) in a marine fish species. Tomcod were also IP injected with polychlorinated biphenyl (PCB)-126 to evaluate the impact of cytochrome P4501A (CYP1A) induction on the biotransformation of injected PBDEs contained in DeBDE and PBDEs initially present in fish. Besides BDE-209, concentrations of BDE-203 and three other unidentified octabrominated PBDEs and the nonabrominated PBDEs (BDE-206, -207, and -208) were enriched in the liver of fish injected with DeBDE. All these PBDE congeners, essentially absent in control fish, were identified as impurities in DeBDE, and, thus, their presence could not be attributed exclusivelyto biotransformation. Despite a 4.3times increase of EROD activity in the liver of tomcod injected with both PCB-126 and DeBDE, compared to DeBDE alone, no further increases of PBDE hepatic concentrations were observed. However, depleted concentrations of BDE-17 (x 1.5) and 6-MeO-BDE-47 (x 1.4) were found in fish IP injected with DeBDE compared to control fish, likely due to activated hepatic metabolic enzymes other than CYP1A. Fish injected with PCB-126 showed an even more significant depletion of BDE-17 hepatic concentrations (x 3.5) than the one associated with the DeBDE treatment and a significantly lower proportion of fish with quantifiable concentrations of BDE-203. Thus, CYP1A inducers can promote the biotransformation of PBDEs in fish liver. This study shows that exposure of fish to DeBDE is expected to result in the enrichment of high brominated PBDEs in fish liver and that metabolic activities in fish can affect their PBDE bioaccumulation pattern and possibly the toxicity of PBDEs to fish.

Contaminants described as organochlorines (OCs; e.g., polychlorinated biphenyls [PCBs]) are present in tissues of marine mammals, including beluga whales (Delphinapterus leucas), but the complexity of contaminant exposure often is not fully known. The PCBs, OC pesticides, polybrominated diphenyl ether (PBDE) flame retardants, methylsulfonyl (MeSO2)- and hydroxy (OH)-PCB metabolites, and OH-PBDEs and methoxylated (MeO)-PBDEs were determined in the liver of beluga whales from two Canadian populations: the St. Lawrence Estuary (SLB; n=6), and western Hudson Bay in the Canadian Arctic (CAB; n=11). The sigmaPCB, sigmaDDT, and sigmaPBDE concentrations were higher (p < 0.05) in SLB versus CAB. Of 18 detectable OH-PCBs in SLB (mainly 4-OH-CB107, 4-OH-CB112, and 4'-OH-CB120), only 4'-OH-CB120 was found in CAB. The sigmaOH-PCB concentrations were less than 0.2% of the sigmaPCBs in both populations but were higher (p < 0.05) in SLB (65 +/- 22 ng/g lipid wt) than in CAB (3.1 +/- 0.5 ng/g lipid wt). The sigmaMeSO2-PCB concentrations were higher in SLB (3801 +/- 1322 ng/g lipid wt) relative to CAB (77 +/- 23 ng/g lipid wt) and were 11 and 4%, respectively, of the sigmaPCB concentrations. Of the 15 OH-PBDEs, only two congeners were detectable, but not quantifiable (notably 2'-OH-BDE 68 and 6-OH-BDE 47), in animals from both populations. Of the 15 MeO-PBDEs, 4'-MeO-BDE 17 and 6-MeO-BDE 47 in the SLB (n=2) and 2'-MeO-BDE 68 and 6-MeO-BDE 47 in the CAB (n=2) had concentrations from 20 to 100 ng/g lipid weight. The OH-PBDEs and MeO-PBDEs most likely are of natural origin and accumulated in beluga whales, whereas the OH-PCBs and MeSO2-PCBs are metabolites derived from accumulated PCBs. Canadian beluga whale liver contains previously unidentified organohalogen contaminants and metabolites and, thus, a complexity of contaminant exposure that may be impacting the health of Canadian beluga whale populations.

Background: Persistent organic pollutants (POPs) in wildlife and humans remain a cause of global concern, both in regard to traditional POPs, such as the polychlorinated biphenyls (PCBs), and emerging POPs, such as the polybrominated diphenyl ethers (PBDEs). To determine the time related concentrations, we analyzed human milk for these substances at three time points between 1987 and 1999. Polychlorobiphenylols (OH-PCBs), the dominating class of PCB metabolites, some of which are known to be strongly retained in human blood, were also included in the assessment., Methods: We obtained milk from the Faroe Islands, where the population is exposed to POPs from their traditional diet (which may include pilot whale blubber). In addition to three pools, nine individual samples from the last time point were also analyzed. After cleanup, partitioning of neutral and acidic compounds, and separation of chemical classes, the analyses were carried out by gas chromatography and/or gas chromatography/mass spectrometry., Results: Compared to other European populations, the human milk had high PCB concentrations, with pool concentrations of 2300 ng/g fat 1987, 1600 ng/g fat in 1994, and 1800 ng/g fat in 1999 (based on the sum of eleven major PCB congeners). The nine individual samples showed great variation in PCB concentrations. The OH-PCBs were present in trace amounts only, at levels of approximately 1% of the PCB concentrations. The PBDE concentrations showed a clear increase over time, and their concentrations in human milk from 1999 are among the highest reported so far from Europe, with results of individual samples ranging from 4.7 to 13 ng/g fat, Conclusion: Although remote from pollution sources, the Faroe Islands show high concentrations of POPs in human milk, particularly PCBs, but also PBDEs. The PBDEs show increasing concentrations over time. The OH-PCB metabolites are poorly transferred to human milk, which likely is related to their acidic character.