Polybrominated diphenyl ethers (PBDEs) in sediment and bivalves from Korean coastal waters

Concentrations of polybrominated diphenyl ethers (PBDEs) were determined in sediment and bivalves collected from 25 coastal locations in Korea. Twenty major PBDE congeners were found in all sediment and bivalve samples. SigmaPBDE20 concentrations ranged from 0.45 to 494 ng/g, dry weight (average 27.8 ng/g dry weight) in sediments, and from 0.38 to 9.19 ng/g, wet weight (average 2.94 ng/g wet weight) in bivalves. The highest concentrations were found at locations near industrial complexes and large harbors, suggesting that human activities contribute to PBDEs contamination in Korean coastal environment. PBDE concentrations measured in our study, excluding BDE congener 209 (deca-BDE), in sediment and bivalves were lower than those reported from other countries; whereas BDE 209 concentrations were comparable to or higher than those reported from other countries. The predominant PBDE congener in sediments and bivalves was deca-BDE, which accounted for >90% and >60% of the total PBDE concentrations in sediment and bivalves, respectively. This is consistent with high consumption of deca-BDE for the flame-retardant market in Korea. Significant correlations existed among BDEs 28, 47, 99, 100, 153 and 154 in sediments and bivalves; however, BDEs 183 and 209 showed little correlation compared with less highly brominated congeners.     

Polybrominated diphenyl ether in sewage sludge in Germany

Sewage sludge samples from 11 municipal waste water treatment plants in Germany were collected from March 2002 to June 2003. Total Tri- to HpBDE concentrations (sum of significant congeners BDE 28, 47, 99, 153, 154 and 183) ranged from 12.5 to 288 (median 108) and DeBDE (BDE 209) concentrations from 97.1 to 2217 (median 256) ng/gd.m. BDE 209 dominated the congener profile. A significant change of the Tri- to HpBDE congener profile (% of total BDE 28, 47, 99, 153, 154, 183 without 209) in sludge from different stages of the waste water treatment process (primary sludge, secondary excess sludge and (dewatered) digested sludge), indicating a degradation of DeBDE to these congeners, was not observed.     

Accumulation, tissue-specific distribution and debromination of decabromodiphenyl ether (BDE 209) in European starlings (Sturnus vulgaris)

In this study we investigated the accumulation, tissue-specific distribution and possible debromination of BDE 209 in a terrestrial songbird species, the European starling, using silastic implants as a method of exposure. BDE 209 accumulated in the blood of the exposed starlings to a mean peak concentration of 16+/-4.1 ng/ml on day 10. After this peak, there was a decline to 3.3+/-0.4 ng/ml blood at the end of the exposure period of 76 days, which suggests elimination of BDE 209. In the exposed group, the muscle concentrations (461 ng/g lipid weight [lw], 430 ng/g lw) were about twofold those in liver (269 ng/g lw, 237 ng/g lw). In addition to BDE 209, other PBDE congeners, particularly octa- and nonaBDEs, were also present in the muscle and liver, suggesting bioformation from BDE 209. To our knowledge, these results are the first indications for the debromination of BDE 209 in birds.     

Polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs) in human liver and adipose tissue samples from Belgium

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.     

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.     

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   

Levels and distribution of polybrominated diphenyl ethers in plant, shellfish and sediment samples from Laizhou Bay in China

Polybrominated diphenyl ethers (PBDEs) are potentially harmful and persistent environmental pollutants. PBDEs concentrations are reported in plant, shellfish and sediment samples collected from Chinese Laizhou Bay. The summation operator(11)PBDE concentrations in plant and shellfish samples from Laizhou Bay were in the range of 70-5900ngg(-1) and 230-720ngg(-1) lipid, respectively. The summation operator(11)PBDEs concentrations in river sediment intervals samples ranged from 1.3 to 1800ng g(-1) dry weight. Pearson correlation analyses were performed on concentrations of PBDEs congeners of different sediment sample intervals. There were significant positive correlations for BDE 28 and BDE 100 (r=0.945, p<0.01), BDE 47 and BDE 99 (r=0.879, p<0.01), BDE 153 and BDE 154 (r=0.934, p<0.01), nona-BDEs and BDE 209 (r>0.934, p<0.01). BDE 209 was the predominant congener in all analyzed samples, consistent with the fact that deca-BDE technical mixtures are the dominant PBDEs product in Laizhou Bay. Data showed that PBDEs should be considered as an increasing pollution problem in the Laizhou Bay region.     

Brominated flame retardants in the hair and serum samples from an e-waste recycling area in southeastern China: the possibility of using hair for biomonitoring

Hair samples and paired serum samples were collected from e-waste and urban areas in Wenling of Zhejiang Province, China. The PBDE and DBDPE concentrations in hair and serum samples from e-waste workers were significantly higher than those of non-occupational residents and urban residents. BDE209 was the dominating BFRs in hair and serum samples from the e-waste area, while DBDPE was the major BFRs from the urban area. Statistically significant correlations were observed between hair level and serum level for some substances (BDE209, DBDPE, BDE99, BDE47, BDE28, and BDE17), although the PBDE congener profiles in hair were different from those in the serum. A statistically significant positive correlation between the PBDE concentrations and the working age, as well as gender difference, was observed in e-waste workers. Different sources of PBDEs and DBDPE in three groups were identified by principal component analysis and spearman correlation coefficient. Hair is suggested to be a useful matrix for biomonitoring the PBDE exposure in humans.     

Patterns and concentration levels of polybrominated diphenyl ethers (PBDEs) in placental tissue of women in Denmark

The levels and congener patterns of PBDEs were investigated in human placental samples in Denmark. The median concentrations of ∑PBDE_tri-hepta and BDE-209 in the 50 samples were 1.22 and 1.14 ng g⁻¹ lw, respectively, with the total sum ranging from 0.51 to 17.1 ng g⁻¹ lw, which is similar to previous placental studies. The PBDE content in placental tissue was dominated by BDE-209, which accounted for approximately 50% of the total amount of PBDEs. BDE-47, -99, and -153 were detected in all samples. Approximately equal amounts of BDE-47 and BDE-153 were observed in the placental tissue, which is in agreement with previous European studies of human serum. Principal Component Analysis (PCA) was performed to analyze congener patterns within and between mothers. The loading plot showed groupings of the measured PBDE variables in three groups, representative of Penta-, Octa- and Deca-BDE technical mixtures. Congeners representing the individual technical mixtures were close to orthogonal or inversely correlated, indicating variation in the congener patterns of internal exposure corresponding to the patterns of technical mixtures used in products. Visualisation of the participant objects according to body mass index (BMI), revealed inherent congener patterns (19% X-variance) showing increased frequency for participants within the highest BMI group to have elevated concentrations of BDE-209 in the placental tissue.     

Age and seasonal variability of polybrominated diphenyl ethers in free-ranging East Greenland polar bears (Ursus maritimus)

Polybrominated diphenyl ethers (PBDEs) were analysed in adipose tissue from 92 East Greenland polar bears (Ursus maritimus) sampled during 1999-2001. Mean SigmaPBDE concentrations were 70 ng/g lipid weight (lw) (range: 22-192 ng/g lw) and showed no relationship with age or sex. Of the 32 analysed PBDE congeners; BDE47, BDE153, BDE99 and BDE100 dominated, and comprised 99.6% of the SigmaPBDE concentration. The SigmaPBDE concentration had a highly significant correlation with SigmaPCB, SigmaCHL, dieldrin, HCB and SigmaHCH concentrations. We found a seasonal pattern of median SigmaPBDE concentration with 1.2 to 1.8 times higher concentrations in March to July than the rest of the year. The seasonal variation also provides a clue to the seasonal exposure, bio-availability, toxic exposure and degradation. We suggest that future geographical PBDE data comparisons may not need corrections for sex or age, but such data sets should be corrected for seasonal variability, using the presented correctional trigonometric regression.     

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.     

Monitoring of PBDEs concentration in umbilical cord blood and breast milk from Korean population and estimating the effects of various parameters on accumulation in humans

In this study, we investigated concentration, congener distribution pattern, and effects of potential environmental factors that affect PBDE accumulation. We also estimated correlation between PBDE concentration and health status or thyroid function by analyzing 90 cord blood and 21 breast milk samples obtained from Korean population. Seven from tri- to hepta-BDEs were analyzed by solid phase extraction-high-resolution gas chromatography/high-resolution mass spectrometry (SPE-HRGC/HRMS). The total concentration of 7 PBDEs in cord blood was 2.786-94.64 ng g(-1) lipid and that in breast milk was 1.076-8.664 ng g(-1) lipid. Tetra-BDE (#47) was the predominant type of PBDE and was present at concentrations of over 40% in both sample types. A weak correlation was observed between the concentration of BDE28 and 153 and thyroid hormone concentration only in the breast milk samples. In children, a weak negative correlation was observed between free thyroxine (FT4) concentration and BDE28 concentration (0.302, p<0.05), while in mothers, a weak positive correlation was observed between thyroid hormone concentration and BDE153 concentration (0.403, p<0.05). No significant correlations between PBDE concentration and work and residential environments were found in this study, but a weak correlation between BDE concentration in cord blood and potential PBDE sources was confirmed by investigating the frequency of oil paint usage (0.510, p<0.001). A weak correlation was also found between PBDE concentration in breast milk during pregnancy and dietary habits such as green tea drinking (0.541, p=0.025) and Trichiuridae intake (0.565, p=0.015).     

Congener distribution of polybrominated diphenyl ethers in feral carp (Cyprinus carpio) from the Llobregat River, Spain

Feral carp were collected at two Spanish rivers, Anoia and Cardener, showing PBDE levels from 29 to 638 ng/g lipid weight (lw) and from 54 to 744 ng/g lw, respectively. Sediments were also collected, showing PBDE contamination between 2 and 10 ng/g dry weight (dw). Differences in PBDE profiles between sediments and fish were noticed. Contribution of BDE-47 in sediment was up to 11%, whereas it contributed 37-90% of PBDEs in fish. Similar results were observed for BDE-154, which was only detected in one sediment sample, but presented high contribution in carp. In contrast, BDE-99 contributed up to 32% in sediments, but it was not detected in fish. Similar results were observed for BDE-153, BDE-183 and BDE-209. The main reason for their concentration decrease or absence in biota may be due to low bioavailability potential or due to biotransformation processes.     

Polybrominated diphenyl ethers in whitefish from Swiss lakes and farmed rainbow trout

A method for trace analysis of polybrominated diphenyl ethers (PBDE) in fish based on gas chromatography/electron ionization high resolution mass spectrometry (GC/EI-HRMS) was developed, and levels of PBDE were determined in whitefish (Coregonus sp.) from eight Swiss lakes and in rainbow trout (Oncorhynchus mykiss) from four Swiss fish farms. PBDE concentrations (sum of PBDE congeners BDE-28, BDE-47, BDE-99, BDE-100, BDE-153, BDE-154, and BDE-183) in filet from whitefish between 36 and 165 ng/g lipid weight (lw) were found, corresponding to wet weight (ww) concentrations of 1.6-7.4 ng/gww. PBDE contents in filet from farmed rainbow trout were significantly lower than in wild whitefish (12-24 ng/glw, 0.74-1.3 ng/gww), and the PBDE congener patterns were different for both species (a higher BDE-47 to BDE-99 ratio for farmed rainbow trout compared to wild whitefish was found). Whitefish PBDE levels [ng/glw] correlate better with the surface/volume ratio of the respective lakes (r(2)=0.70) than with other lake properties such as catchment area (size or number of inhabitants) or residence time, suggesting atmospheric deposition as an input pathway for PBDE. Based on an average daily consumption of 20 g whitefish (Switzerland) with a PBDE content of 7.4 ng/gww (highest PBDE concentration detected in this study), a maximum daily intake of 0.15 microg PBDE was estimated (0.026 microg/day for farmed trout). This number corresponds to the lower end of the estimate for the total PBDE intake of the Nordic consumer of 0.2-0.7 microg/day.     

Brominated flame retardants and organochlorine pollutants in aquatic and terrestrial predatory birds of Belgium: levels, patterns, tissue distribution and condition factors

Liver and muscle samples from 7 species of aquatic and terrestrial predatory birds from Flanders (Belgium) were analysed for polychlorinated biphenyls (PCBs), polybrominated diphenylethers (PBDEs) and organochlorine pesticides (OCPs). PCBs were the predominant compounds in our samples, which showed highest concentrations in the liver of barn owl (Tyto alba) and sparrowhawk (Accipiter nisus) (up to 1000 microg/g lipid weight). PBDEs could be determined in most samples at lower concentrations than PCBs (up to 64 microg/g lipid in sparrowhawk liver). Sparrowhawks had the highest levels of hexachlorobenzene, DDTs and PBDEs. In contrast, kestrels (Falco tinnunculus) had relatively low levels of most measured organochlorines. BDE 47 was the most abundant congener in heron (Ardea cinerea) and grebe (Podiceps cristatus), while BDE 47, 99 and 153 were equally important in the terrestrial species. BDE 183 and BDE 209 were only measured in the terrestrial birds. These results indicate that terrestrial birds may be more exposed to higher brominated BDE congeners than aquatic species.     

Polybrominated diphenyl ethers in surface sediments of the Yangtze River Delta: Levels, distribution and potential hydrodynamic influence

A total of 32 surface sediments collected from the Yangtze River Estuary, Hangzhou Bay and the Qiantang River were analyzed for polybrominated diphenyl ethers (PBDEs). The concentrations of summation operatorPBDEs (sum of 12 PBDE congeners without BDE 209) and BDE 209 varied from n.d. to 0.55 and from 0.16 to 94.6 ng/g, respectively. The spatial variability of summation operatorPBDEs concentrations indicated that waste discharge from the urban areas might been the main source of PBDEs in the Yangtze River Delta. BDE 209 was the predominant congener (approximately 90-100%) detected among the 13 congeners, consistent with the fact that technical deca-BDE mixtures are presently the dominant technical PBDE mixtures used in China. Compared to published data acquired from other locales, PBDE congeners with less than four bromines were more abundant in the present study area. The hydrodynamic conditions may likely be a significant factor in dictating the observed levels and congener distribution patterns of PBDEs.     

Brominated flame retardants and organochlorine pollutants in eggs of little owls (Athene noctua) from Belgium

Residues of brominated diphenylethers (PBDEs), organochlorinated pesticides (OCPs) and polychlorinated biphenyls (PCBs) were measured in 40 eggs of little owls (Athene noctua), a terrestrial top predator from Belgium. The major organohalogens detected were PCBs (median 2,600 ng/g lipid, range 790-23 000 ng/g lipid). PCB 153,138/163, 170, 180 and 187 were the predominant congeners and constituted 71% of total sum PCBs. PBDEs were measurable in all samples, but their concentrations were much lower than for PCBs, with a range from 29-572 ng/g lipid (median 108 ng/g lipid). The most prevalent PBDE congeners in little owl egg samples were BDE 47, 99 and 153. This profile differs from the profile in marine bird species, for which BDE 47 was the dominant congener, indicating that terrestrial birds may be more exposed to higher brominated BDE congeners than marine birds. The fully brominated BDE 209 could be detected in one egg sample (17 ng/g lipid), suggesting that higher brominated BDEs may accumulate in terrestrial food chains. Brominated biphenyl (BB) 153 was determined in all egg samples, with levels ranging from 0.6 to 5.6 ng/g lipid (median 1.3 ng/g lipid). Additionally, hexabromocyclododecane (HBCD) could be identified and quantified in only two eggs at levels of 20 and 50 ng/g lipid. OCPs were present at low concentrations, suggesting a rather low contamination of the sampled environment with OCPs (median concentrations of sum DDTs: 826 ng/g lipid, sum chlordanes: 1,016 ng/g lipid, sum HCHs: 273 ng/g lipid). Hexachlorobenzene (HCB) and octachlorostyrene (OCS) were also found at low median levels of 134 and 3.4 ng/g lipid, respectively. Concentrations of most analytes were significantly higher in eggs collected from deserted nests in comparison to addled (unhatched) eggs, while eggshell thickness did not differ between deserted and addled eggs. No significant correlations were found between eggshell thickness and the analysed organohalogens.     

Polybrominated diphenyl ethers in house dust in Singapore

The use of polybrominated diphenyl ethers (PBDEs) as flame retardants in Singapore is not strictly regulated; therefore these compounds can be readily found in furniture, electronic devices, and building materials. This study was the first of its kind to be conducted in Singapore to measure concentrations of PBDEs in house dust. Samples were collected from 31 homes in various locations across the island-state of Singapore, and a total eight PBDEs congeners were measured. PBDEs were detected in all 31 dust samples and the number of BDE congener detected per home ranged between 3 and 8. The most abundant BDE congeners found were BDE 47, 99 and 209, with a median value of 20 ng g(-1) dust, 24 ng g(-1) dust and 1000 ng g(-1) dust, respectively. BDE 209 contributed 88% to the median of all the congeners, and BDE 47 and 99 contributed 1.8% and 3.5%, respectively. Different congener profiles were observed between this and studies conducted elsewhere, which is consistent with the use of different commercial PBDE around the world. No significant correlations between PBDE dust levels and residential characteristics (number of TVs and computers, floor area or flooring material) were observed. The daily intake of PBDEs via the inhalation pathway was estimated. House dust may be regarded as the most important exposure route of PBDEs for children.     

Time-trend (1973-2000) of polybrominated diphenyl ethers in Japanese mother's milk

The time-trend and recent concentrations of polybrominated diphenyl ethers (PBDEs) in Japanese mother's milk were investigated. The time-trend of 16 PBDEs (BDE-28, 37, 47, 66, 71, 75, 77, 85, 99, 100, 119, 153, 154, 138, 183, and 190) in pooled milk samples from mothers living in Osaka between 1973 and 2000 was analyzed. Additionally, PBDE concentrations in individual milk samples collected from 13 mothers living in Kanagawa and Okayama in 1999 were measured. The total concentration of all PBDE congeners (SigmaPBDEs) measured in the pooled samples increased during the period between 1973 (<0.01 ng/g lipid) and 1988 (1.64 ng/g lipid), and remained low afterwards while showing remarkable changes in PBDE congener profiles. The SigmaPBDEs in the 1999 individual milk samples were also low (0.56-3.97 ng/g lipid), except for a single sample (291 ng/g lipid). The source of this exposure could not be identified.     

Occurrence of polybrominated diphenyl ethers (PBDEs) and 2,2’,4,4’,5,5’-hexabromobiphenyl (BB-153) in water samples from the Diep River, Cape Town, South Africa

Until recently, studies reporting the concentrations of polybrominated diphenyl ethers (PBDEs) as well as polybrominated biphenyls (PBBs) are generally scarce in the literature. Consequently, this study was aimed to investigate the occurrence and concentrations of certain PBDE congeners (BDE 28, 47, 100, 99, 154, 153, 183 and 209) and BB 153 in river water samples collected bi-monthly from the Diep River. The routine analyses of the target compounds were performed using a high-capillary GC–microelectron capture detection, while their structural elucidation was assessed using GC-TOF-MS technique. The overall mean concentrations of the sum of the eight PBDE congeners were 2.60, 4.83 and 4.29 ng/L for the upstream, point of discharge and downstream sampling points, respectively. Similarly, the overall mean concentrations of BB 153 were 0.25, 4.85 and 1.56 ng/L for the upstream, point of discharge and downstream sampling points, respectively. BDE 47 was the dominant congener found in these samples contributing between 19 and 26 % to the total PBDEs across the sampling points. The statistical analyses performed on the results obtained showed that all the congeners, except BDE 209 in certain instances, had strong positive correlations with one another, thus suggesting that these contaminants could be emanating from the same source. In this study, potential sources of these pollutants other than WWTP discharges into the investigated river were also identified. However, the relatively high concentrations of the target compounds found at the point of discharge sampling point coupled with the large volume of treated effluent being discharged suggested that the contributions from this source could be very significant over time.