Congener-specific accumulation and environmental risk assessment of polybrominated diphenyl ethers in diverse Korean sewage sludge types

Industrial, domestic wastewater, and livestock sludge samples were collected from 23 wastewater treatment plants in Korea and analyzed for polybrominated diphenyl ethers (PBDEs). The concentrations of Σ₁₉PBDE ranged from 4.01 to 10,400 ng/g dry weight. The average Σ₁₉PBDE concentrations in industrial, domestic wastewater, and livestock sludge were 1,560?±?3,610, 402?±?148, and 27.6?±?50.4 ng/g dry weight, respectively. The composition of PBDEs differed according to the type of sludge. Among the PBDE congeners, BDE 209 was dominant in all sludge samples. After BDE 209, relatively high levels were found for BDE 28 and 47 from industrial sludge, BDE 47 and 99 from domestic wastewater sludge, and BDE 206, 207, and 208 from livestock sludge. Using hierarchical cluster analysis, sludges were divided into three groups according to PBDE congener composition. A risk assessment of PBDEs in sludge used for soil amendment was carried out. Preliminary results indicated that the potential risk of soil exposed to PBDEs in sludge was relatively low.     

An exposure study with polybrominated diphenyl ethers (PBDEs) in female European starlings (Sturnus vulgaris): toxicokinetics and reproductive effects

We exposed female European starlings to a pentabromodiphenyl ether (Penta-BDE) mixture through subcutaneous implants, and examined levels and profiles of polybrominated diphenyl ethers (PBDEs) together with reproductive effects. Sum PBDE levels increased significantly in the serum of the exposed females from 218 ± 43 to 23,400 ± 2035 pg/ml. Sum PBDE concentrations in the eggs of the exposed group ranged from 130 ± 12 to 220 ± 37 ng/g wet weight (ww). The profile in serum after egg laying was very similar to that in eggs. There were no detectable levels of HO-PBDEs in both serum and eggs. Fewer females of the exposed group initiated egg laying compared to the control group, although the difference was not significant. In addition, egg weight and volume were significantly higher in the exposed group. These results suggest that, at the investigated exposure levels (150 μg sum PBDEs/bird), PBDEs may have a negative effect on reproductive performance.     

State of polybrominated diphenyl ethers in China: an overview

Polybrominated diphenyl ethers (PBDEs), extensively used as flame retardants, are ubiquitous environmental contaminants that are found in both abiotic and biotic environmental samples. Sufficient evidence shows that PBDEs have been rapidly accumulating in the environment of China, especially in the Southeast regions. This paper summarizes and critically reviews the published scientific data on PBDEs in China, including the levels of PBDEs in the air, soil, water, sediment, the terrestrial and marine organisms, and human samples in China. The data preliminarily reveal the state of PBDEs in China.     

House dust as a source of human exposure to polybrominated diphenyl ethers in Kuwait

This study reports concentrations of polybrominated diphenyl ethers (PBDEs) in dust samples collected from 17 homes in Kuwait. PBDEs were measured in all homes investigated with mean summation operatorPBDEs concentration ranging from 1 to 393 ng g(-1), with a geometric mean of 76 ng g(-1). The dominant congener in all samples was BDE 209 constituting ca. 85% of the summationPBDEs followed by BDE 99 (5%), BDE 47 (4.5%), and BDE 183 (2%). The congener mixture in dust is dominated by those in deca and penta formulations. Using the measured concentrations and estimates of dust ingestion rates for children and adults, estimated human non-dietary exposure based on mean PBDE levels were 14.8 and 1.5 ng day(-1) for children and adults, respectively. The 10-fold difference in exposure estimates between children and adults in this study supports previous reports that children are at greater risk from pollutants that accumulate indoors. The ubiquitous distribution of these chemicals as noted in this study highlights the fact that we are continuously exposed to low doses of chemicals in the indoor environment.     

Distribution of polybrominated diphenyl ethers in breast milk from North China: Implication of exposure pathways

The breast milk concentrations of polybrominated diphenyl ethers (PBDEs; sum of eight congeners: BDE-28, 47, 99, 100, 153, 154, 183 and 209) were determined (by high resolution gas chromatographic high resolution mass spectrometry) in samples from primiparous women collected in 2006 in Tianjin, China. Dietary and lifestyle habits of the participants were obtained by questionnaires. The median total PBDE concentration (including BDE-28, 47, 99, 100, 153, 154, 183) was 2500 pg g⁻¹ lipid weight, ranging from 1700 to 4500 pg g⁻¹ lipid weight. These levels were in the same range as those from Europe and Japan but much lower than those from North America. The congener profile in China was also different from other countries. The contribution of BDE-28 was around 15%, much higher than any other country, implying that a different Penta-BDE formulation might be used in the Chinese market. The lower ratio of the sum of BDE-47, 99, and 100 to the sum of BDE-153 and 154 suggested that Octa-products were in more demand in China. A significant correlation was found between a woman’s PBDE concentration and the time she used electronic appliances (h/d). This implies that electronics are a potential source of PBDEs to people. Inhalation or ingestion of particulate matter (such as dust) may also be an important exposure pathway. There was no significant correlation between the PBDE concentration and the consumption of meat, fish, and milk. Further research is needed to determine the specific contribution of each exposure route and their health effects.     

Occurrence and concentrations of polybrominated diphenyl ethers in sewage sludge from three wastewater treatment plants in Kuwait

Polybrominated diphenyl ether (PBDE) concentrations were measured in sewage sludge samples collected from three wastewater treatment plants in Kuwait over a six month period. PBDEs were detected in all samples analyzed and there were significant differences between the three wastewater treatment plants. The mean (and range) of summation PBDEs concentrations measured are as follows: Jahra 52.5 ng g(-1) (5.7-169.5 ng g(-1)); Reqqa, 144 ng g(-1) (32-296 ng g(-1)); Umm Haylaman, 377 ng g(-1) (23-1599 ng g(-1)). The differences in concentrations of the sum of penta congeners were consistently different at the three treatment plants with values increasing in the order: Jahra相似文献   

A contemporary assessment of polybrominated diphenyl ethers (PBDE) in the ambient air and soil of Azerbaijan

PBDEs were measured in air and soil across Azerbaijan to establish contemporary concentrations at 13 urban and rural sites. Polyurethane foam passive air samplers (PUF-PAS) were deployed for a period of a month with surface soil samples collected at the same sites. Unlike organochlorine pesticides previously surveyed by our group, PBDE concentrations in both contemporary air and soil were low in comparison to recent European and Asian studies. For example, mean ∑₉PBDE concentrations in air and soil were 7.13 ± 1.66 pg m^?3 and 168 ± 57 pg g^?1, respectively. The fully brominated BDE-209 was the most abundant congener observed in soil (174.8 ± 58.5 pg g^?1), comprising ~ 96% of ∑₁₀PBDE. However, the PAS-derived air concentrations for highly brominated congeners must be viewed with caution as there is uncertainty over the uptake rates of particle-bound chemicals using these devices. Some of the highest concentrations in air were observed at sites with the highest wind speeds and at several remote locations in the north of the country and this requires further research. Levels of BDE-47 and 99 (the two most abundant congeners in the widely used penta-formulation) were lower than levels reported elsewhere suggesting limited use/import of the penta-BDE formulation in Azerbaijan.     

Spatial distribution of polybrominated diphenyl ethers and polybrominated biphenyls in lake trout from the Laurentian Great Lakes

Concentrations of two types of brominated flame-retardants (BFRs); polybrominated diphenyl ethers (PBDEs) and polybrominated biphenyls (PBBs) were determined in a single age class of lake trout (Salvelinus namaycush) collected from the Laurentian Great Lakes in 1997. Mean concentrations of total PBDE were highest in samples from Lake Ontario at 95+/-22 ng/g wet weight (ww) or 434+/-100 ng/g lipid weight (lw) while the lowest concentrations were observed in Lake Erie lake trout (27+/-8.6 ng/g ww, 117+/-37 ng/g lw). In all samples, the predominant PBDE congeners were 2,2',4,4'-tetrabromodiphenyl ether (BDE-47), 2,2',4,4',5-pentabromodiphenyl ether (BDE-99), and 2,2',4,4', 6-pentabromodiphenyl ether (BDE-100), which are the primary components of the commonly used penta-BDE formulation flame retardant. Lake trout collected from Lake Huron had the highest concentrations of PBBs (3.1+/-1.7 ng/g ww, 15+/-8.5 ng/g lw), while the lowest levels were detected in fish from Lake Superior (0.25+/-0.13 ng/g ww, 1.7+/-0.89 ng/g lw). In all lake trout samples, 2,2',4,4',5,5'-hexabromobiphenyl (BB-153), a major constituent of the flame-retardant FireMaster BP-6, was the predominant PBB congener.     

Distribution of polybrominated diphenyl ethers in Japanese autopsy tissue and body fluid samples

Brominated flame retardants are components of many plastics and are used in products such as cars, textiles, televisions, and personal computers. Human exposure to polybrominated diphenyl ether (PBDE) flame retardants has increased exponentially during the last three decades. Our objective was to measure the body burden and distribution of PBDEs and to determine the concentrations of the predominant PBDE congeners in samples of liver, bile, adipose tissue, and blood obtained from Japanese autopsy cases. Tissues and body fluids obtained from 20 autopsy cases were analyzed. The levels of 25 PBDE congeners, ranging from tri- to hexa-BDEs, were assessed. The geometric means of the sum of the concentrations of PBDE congeners having detection frequencies >50 % (ΣPBDE) in the blood, liver, bile, and adipose tissue were 2.4, 2.6, 1.4, and 4.3 ng/g lipid, respectively. The most abundant congeners were BDE-47 and BDE-153, followed by BDE-100, BDE-99, and BDE-28+33. These concentrations of PBDE congeners were similar to other reports of human exposure in Japan but were notably lower than concentrations than those reported in the USA. Significant positive correlations were observed between the concentrations of predominant congeners and ΣPBDE among the samples analyzed. The ΣPBDE concentration was highest in the adipose tissue, but PBDEs were distributed widely among the tissues and body fluids analyzed. The PBDE levels observed in the present study are similar to those reported in previous studies in Japan and significantly lower than those reported in the USA.     

Bioaccumulation, maternal transfer and elimination of polybrominated diphenyl ethers in wild frogs

To investigate bioaccumulation, maternal transfer and elimination of polybrominated diphenyl ethers (PBDEs) in amphibians, we collected adult frogs (Rana limnocharis) from a rice field in an e-waste recycling site in China. We found that ∑PBDEs in the whole frogs and various tissues (brain, liver, testis and egg) ranged from 17.10 to 141.11 ng g⁻¹ wet weight. Various tissues exhibited a similar PBDE congener profile, which was characterized by intermediate brominated congeners (BDE-99 and BDE-153) as the largest contributors, with less lower brominated congeners (BDE-28 and BDE-47) and higher brominated congeners (BDE-209). The maternal transfer capacity of PBDEs declined with the increase in bromine numbers of PBDE congeners. We suggest that the bromine atom number (the molecular size, to some degree) might be a determining factor for the maternal transport of a PBDE congener rather than K_ow (Octanol-Water partition coefficient), which expresses a compound’s lipophilicity. ∑PBDEs concentrations in frogs decreased over time during a depuration period of 54 days when these wild frogs were brought to the lab from the e-waste recycling site. The half-life of ∑PBDEs was 35 days, with about 14 days for BDE-47, and 36 and 81 days for BDE-99 and BDE-153, respectively. The data shows that the elimination of PBDEs has no essential difference from aquatic and terrestrial species.     

Validation of a flow-through sampler for pesticides and polybrominated diphenyl ethers in air

At locations without access to the electrical grid, a flow-through sampler (FTS) collects large volumes of air for the analysis of semi-volatile organic compounds (SVOCs). To test its performance under field conditions, an FTS and a traditional pumped high volume air sampler, both using polyurethane foam (PUF) as sampling medium, were co-deployed at the campus of the University of Toronto Scarborough from August 2006 to June 2007. Polybrominated diphenyl ethers (PBDEs) and various pesticides were quantified in the samples taken by both samplers to test the FTS's applicability to relatively non-volatile and slightly polar SVOCs. Air concentrations in samples taken with the FTS over five 2-week periods compare favourably with the average of the concentrations in several 24-h active high volume samples taken during the same period. In particular, time trends, temperature dependence relationships, and isomer ratios show a reasonable agreement between the two sampling techniques. An empirical linear solvation energy relationship for predicting the apparent theoretical plate number of the PUF assembly used in the FTS illustrates the effect of chemical properties, as well as temperature and wind speed, on sampling efficiency. In the absence of electrical power, the FTS can collect SVOCs from large air volumes as reliably and quantitatively as traditional HiVol samplers, although without separating gas and particle phase.     

The occurrence of polybrominated diphenyl ethers in river and coastal biota from Portugal

Throughout this work PBDEs level determination in biota was developed for the first time in Portugal. The data obtained was important to provide a global perspective of Portugal contamination by PBDEs and allows the comparison with studies made in other countries. Environmental levels of fourteen polybrominated diphenyl ethers (PBDEs) were analysed in a number of biota samples (Barbus sp. and Mytilus galloprovincialis) taken over a large geographic range covering five rivers and coastal areas of Portugal. Tetrabromodiphenyl ether (BDE 47) was found in almost all samples ranging from not detected (nd) to 30ngg(-1) dry weight (dw). BDE 47 concentration is correlated with mussels weight indicating the bioaccumulation of this compound. Pentabromodiphenyl ethers (BDE 99 and BDE 100) were detected in several samples, but in lower concentrations.     

Exposure to polybrominated diphenyl ethers associated with consumption of marine and freshwater fish in Hong Kong

Concentrations of polybrominated diphenyl ethers (PBDEs) in market fish have not previously been reported in Hong Kong. Axial and ventral muscles from 10 each common species of freshwater and marine fish purchased from markets in Hong Kong were analyzed for 22 PBDEs. Among the 10 freshwater fish species, spotted snakehead (Channa maculate) contained the highest level of PBDEs in ventral muscle (130 ng g(-1) wet wt.). For marine fish, bigeye (Priacanthus macracanthus) showed significantly higher levels of PBDEs (60.7 ng g(-1)wet wt. in ventral tissue) than all other marine species. The levels of PBDEs in fish samples ranged from 0.53 to 130 ng g(-1)wetwt. The tetrabrominated congener BDE-47 and pentabrominated BDE-99 were the predominant congeners, which accounted for 27% and 30%, respectively, of the total PBDEs. Daily PBDE intake was calculated according to the different fish consumption rate for Hong Kong consumers, and the results ranged from 222 to 1198 ng day(-1) for marine fish and 403-2170 ng day(-1) for freshwater fish. The daily PBDE intake from fish reported here were higher than those reported from the United States (8.94-15.7 ng day(-1)) and Europe (14-23.1 ng day(-1)).     

Levels and distribution of polybrominated diphenyl ethers in various tissues of birds of prey

In the present study, concentrations and tissue distribution of polybrominated diphenyl ethers (PBDEs; IUPAC # 28, 47, 99, 100, 153, 154, 183, and 209) were examined in brain, adipose tissue, liver, muscle, and serum of birds of prey. Median SigmaPBDE levels (BDE 28-183) in the tissues of sparrowhawks ranged from 360 to 1900 ng/g lipid weight (lw), which was in general one order of magnitude higher than in the tissues of common buzzards (26-130 ng/g lw). There were no differences in PBDE congener patterns between the various tissues within individuals of a certain species. Inter-species differences in PBDE patterns and in particular the percentage of BDE 99, 100 and 153 were, however, pronounced between sparrowhawk and common buzzard. BDE 209 was detected in nearly all serum and in some liver samples, but not in any other tissues. This observation suggests that exposure to BDE 209 is low or that this congener is poorly accumulated. Passive (lipid content related) diffusion could not completely describe the PBDE tissue distribution, e.g. the lowest PBDE-load was measured in brain, a fairly lipid rich tissue.     

Distribution of polychlorinated biphenyls and polybrominated diphenyl ethers in birds of prey from Switzerland

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.     

Absorption, disposition and excretion of polybrominated diphenyl ethers (PBDEs) in chicken

Except for fish, no toxicokinetic data on polybrominated diphenyl ethers (PBDEs) is available on relevant animals for the human food chain. In the present work, absorption, elimination through eggs and disposition of PBDEs in laying chickens were studied and compared to dioxin behaviour. Hens were fed with diet containing 3.4 mg/kg feed of PBDEs and 0.95 ng TEQ/kg feed of polychlorodibenzo-p-dioxins (PCDDs) and polychlorodibenzofurans (PCDFs). PBDEs have been demonstrated to show drastically different behaviours from PCDD/Fs and dioxin-like compounds. Excretion of PBDEs increased for two weeks and then decreased to nearly 0%. Sixty-two percent of ingested 2,2',4,4'-tetraBDE (BDE-47) were found in excreta after two weeks, suggesting a reductive debromination of PBDEs in the digestive tract. PBDE level in eggs increased during five weeks and reached 24 microg/g fat. After then, levels decreased to 3 microg/g fat at the end of the trial. PBDE bioconcentration factors estimated for abdominal fat varied from 0.7 for BDE-47 to 2 for BDE-183.     

Levels and pattern of polybrominated diphenyl ethers in eggs of Antarctic seabirds: Endemic versus migratory species

Chinstrap and gentoo penguins are endemic species that live year round south of the Antarctic Convergence. South polar skua is a migratory seabird that can be observed in Antarctica during the breeding season (i.e., austral summer). This study compares concentration and pattern of polybrominated diphenyl ethers (PBDEs) in eggs of seabirds breeding at King George Island, Antarctic Peninsula. PBDEs in south polar skua eggs are approximately 20 times higher than in penguin eggs suggesting that skuas are more exposed to contaminants during the non-breeding season when they migrate to waters of the northern hemisphere. The pattern of PBDE congeners also differs between south polar skua and penguin eggs. The latter exhibited a pattern similar to that found in the local biota. In contrast, the congener pattern in south polar skua eggs suggests that birds breeding at King George Island may winter in the northwestern Pacific Ocean.     

Distribution of polybrominated diphenyl ethers in breast milk,cord blood and placentas: a systematic review

Polybrominated diphenyl ethers (PBDEs) have been extensively used as flame retardants in consumer products. PBDEs rapidly bioaccumulate in the environment, food, wild animals and humans. In this review, we investigated the harmful effects of PBDEs on humans, especially in early life, and summarised the levels of PBDEs in human biological samples (breast milk, cord blood and placentas). In addition, we described the spatiotemporal distribution of PBDEs in this review. PBDE levels in breast milk, cord blood and placentas were generally higher in North America than in other regions, such as Asia, Europe, Oceania and Africa. However, high levels of PBDEs in human biological samples were detected at e-waste recycling sites in South China, East China and South Korea. This finding suggests that newborns living in e-waste regions are exposed to high levels of PBDEs during prenatal and postnatal periods. The time trends of PBDE concentration differed according to the region. Few studies have investigated PBDE levels in humans from 1967 to 2000, but they increased rapidly after 2000. PBDE concentration peaked at approximately 2006 globally. Compared with other PBDE congeners, BDE-47, BDE-153 and BDE-209 were the major components, but the detection rate of BDE-209 was lower than those of others. Future studies should focus on determining the BDE-209 concentration, which requires the implementation of different analytical approaches. Additionally, the levels of PBDEs in human samples and the environment should be monitored, especially in e-waste recycling regions.

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Graphical abstract The figures described the spatial distribution of the lowest (Fig. a1) and highest concentration of ∑PBDE (Fig. a2) in different countries by 2006 and described the spatial distribution of the lowest (Fig. b1) and highest concentration of ∑PBDE (Fig. b2) in different countries from 2007 to 2015. All the figures indicated that the levels of PBDEs in North America were substantially higher than those in many regions of Europe, Asia, Oceania, or Africa. Comparing Fig. a1–b1 or Fig. a2–b2, increasing trends were observed in some countries, especially in some regions in China, Korea and Canada.

     

Determination of polybrominated diphenyl ethers in soil and sediment from an electronic waste recycling facility

In this study samples of ten species of fish were analyzed for concentrations of organochlorine pesticides, PCBs and heavy metals (Pb, Cd, and Cu). Fish were captured using electric fishing on ten sites along the Dr?me river (Rh?ne-Alpes region). Quantitative determination of the organochlorine and PCBs compounds was performed by gas chromatography-electron-capture detection (GC-ECD). The concentrations of heavy metals were determined by atomic absorption spectrophotometry. Samples contained detectable concentrations of lindane, PCBs, and heavy metals but at concentrations below the maximum residue limit (MRL). Non-parametric statistical analysis was performed to distinguish groups of sites with different levels of contamination. PCBs concentrations increased along the river with four groups of sites significantly different from each other. Cadmium concentrations were below the MRL. Lead contamination showed two groups significantly different and a repartition similar to PCBs. Copper contamination was correlated with the localization of vineyards. We assessed the potential effects of contamination the otter (Lutra lutra). The concentrations of all pollutants analyzed in fish sampled in this study are lower than the threshold values described in literature. The Dr?me river is relatively unpolluted river, and the establishment of otter populations should not be affected by pollution.