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1.
Cetin B  Odabasi M 《Chemosphere》2008,71(6):1067-1078
Atmospheric concentrations of 7 PBDE congeners (BDE-28, -47, -99, -100, -153, -154 and -209) were determined at four sites (i.e. Suburban, Urban 1, Urban 2, Industrial) in Izmir, Turkey and their gas/particle partitioning was investigated. Total PBDE ( summation operator(7)PBDE) concentrations ranged between 11 (Urban 1) and 149pgm(-3) (Industrial) in summer, while in winter, they ranged from 6 (Suburban) to 81pgm(-3) (Industrial). BDE-209 was the dominant congener at all sites, followed by BDE-99 and -47. Investigation of source profiles indicated that the air samples were dominated by congeners of the penta and deca-technical BDE mixtures. The measured PBDE particle fractions were compared to the predictions of the K(OA) (octanol-air partition coefficient)-based equilibrium partitioning model and to the dynamic uptake model developed by others for passive samplers, which was adapted to model gas-particle partitioning in this study. For BDE-28, good agreement was observed between the experimental particle fractions and those predicted by the equilibrium partitioning model. However, this model overestimated the particle fractions of other congeners. The predictions of the dynamic uptake model supported the hypothesis that the unexpectedly high partitioning of BDEs (except BDE-28) to the gas-phase is due to their departure from equilibrium partitioning. When congeners with very large octanol-air partition coefficients (i.e. BDE-100, -99, -154, -153, and -209) are emitted from their sources in the gas-phase, they may remain in that phase for several months before reaching equilibrium with atmospheric particles. This may also have important implications for the transport of atmospheric PBDEs. For example, in addition to particle-bound transport, the gas-phase transport of highly brominated congeners (i.e. BDE-209) may also be important.  相似文献   

2.
Weekly high-volume air samples have been collected in the Canadian High Arctic (Alert, Nunavut) since 1992. Fifteen polybrominated diphenyl ethers (PBDEs) are quantified in 104 samples over the time period of 2002–2004. To our knowledge, this study reports the first continuous multi-year measurements of PBDEs in Arctic air. Average air concentrations (in pg m−3) were 7.7 (0.40–47) and 1.6 (0.091–9.8) for 14 PBDEs (excluding BDE-209) and BDE-209, respectively, over the entire sampling period. BDE-28/33, 47, 99, 100, 153, 154, and 209 accounted for 90% (72–97%, n=104) of the 15 PBDEs. Occurrence of BDE-47, 99, and 209 suggests that PBDEs in Alert air were likely associated with the usage of “penta-BDE” and “deca-BDE” technical mixtures worldwide. Natural logarithm of concentrations for less brominated PBDEs correlated significantly with ambient temperatures in the summertime, suggesting importance of volatilization emissions in a local and/or regional scale. On the other hand, episodically elevated concentrations of the less brominated PBDEs in the wintertime and lack of seasonality for the non-volatile BDE-209 indicate potential inputs of particle-bound PBDEs through long-range transport (LRT), especially during the Arctic haze season. Inter-annual trend data further show that concentrations of the eight PBDEs increased inter-annually in 2002–2004 with doubling times of 2–6 years, which were similar to growth rates found in Arctic biotic samples. The results of this study and previous measurements suggest that potential sources of PBDEs in Arctic air include both volatilization emissions and LRT inputs.  相似文献   

3.
The uptake and elimination of six PBDE congeners (BDE-28, -47, -99, -100, -153, -209) were studied in juvenile common sole (Solea solea L.) exposed to spiked contaminated food over a three-month period, then depurated over a five-month period. The results show that all of the studied PBDEs accumulate in fish tissues, including the higher brominated congener BDE-209. Several additional PBDE congeners were identified in the tissues of exposed fish, revealing PBDE transformation, mainly via debromination. The identified congeners originating from PBDE debromination include BDE-49 and BDE-202 and a series of unidentified tetra-, penta-, and hepta- BDEs. Contaminant assimilation efficiencies (AEs) were related to their hydrophobicity (log Kow) and influenced by PBDE biotransformation. Metabolism via debromination appears to be a major degradation route of PBDEs in juvenile sole in comparison to biotransformation into hydroxylated metabolites.  相似文献   

4.
Guzzella L  Roscioli C  Binelli A 《Chemosphere》2008,73(10):1684-1691
Polybrominated diphenyl ethers (PBDEs) are characterized by chemical properties and toxicological profiles similar to other POPs (persistent organic pollutants) included in the EU Priority Pollutant List (2455/01/CE). However, limited data have been available for these compounds thus far for Italian freshwater abiotic matrices. Lake Maggiore basin, a heavily industrialized and densely populated area, was selected for studying PBDE contamination in Italy. PBDEs and OCs (organochlorine compounds) in the basin were quantified by analysing both sediment cores collected in 2005 from the lake and grab samples from the main tributaries and the emissary. Fourteen PBDEs, from tri-BDE to hepta-BDE congeners and BDE209, were compared with some organochlorine POPs (PCBs and DDTs) characterizing Lake Maggiore basin contamination. Analyses of tri-to hepta-BDEs, PCBs and DDTs were undertaken by GC-MS/MS, while BDE-209 was analysed by GC/ECD. Results showed a dominant presence of BDE-209 (>95% of SigmaBDE) and limited amounts of BDE-47, BDE-99, BDE-100, BDE-153 and BDE-154. Lake core profiles highlighted a decreasing trend in PCB concentrations starting from the year 2000, while PBDEs showed greater concentrations after the beginning of the 1990s (up to 30 ng g(-1)d.w.). Among the tributaries, the Bardello and Boesio rivers were the most PBDE-contaminated (up to 290 ng g(-1)d.w.).  相似文献   

5.
Feathers of two colonial water-birds species (Bubulcus ibis, Egretta garzetta) from four heronries in the Punjab province, Pakistan were analysed for 28 Polybrominated Diphenyl Ethers (PBDEs) congeners. Median concentrations of ∑PBDEs were 2.41 and 1.91 ng/g in little and cattle egrets. PBDE-47, -100, -138, -153 were abundant and detected in >70% of feather samples in both species. Species-specific differences based on dietary preferences indicated higher concentration of PBDE-47, -66, -75, -100, -153, -154, and -183 in fish eating little egret. BDE-47 and -100 were more frequent in little egrets and BDE-99 was more dominant in cattle egret which feed on terrestrial habitat. Higher ∑hexa- and hepta-BDEs congeners showed larger concentrations in feathers from heronries close to water bodies which receive urban and industrial effluents whereas lower-brominated congeners (BDE-47-BDE-100) dominated in rural/agricultural regions. Hazard quotients (HQs) indicated that measured ∑PBDEs pose no risk to egret population.  相似文献   

6.
The uptake, elimination and transformation of six PBDE congeners (BDE-28, -47, -99, -100, -153, -209) were studied in juvenile common sole (Solea solea L.) exposed to spiked contaminated food over a three-month period, and then depurated over a five-month period. Methoxylated (MeO-) and hydroxylated (OH-) PBDEs were determined in fish plasma exposed to PBDEs and compared to those obtained in control fish. While all MeO- and some OH- congeners identified in fish plasma were found to originate from non-metabolic sources, several OH- congeners, i.e., OH-tetraBDEs and OH-pentaBDEs, were found to originate from fish metabolism. Among these, 4′-OH-BDE-49 was identified as a BDE-47 metabolite. Congener 4′-OH-BDE-101, identified here for the first time, may be the result of BDE-99 metabolic transformation. Our results unequivocally showed that PBDEs are metabolised in juvenile sole via the formation of OH- metabolites. However, this was not a major biotransformation route compared to biotransformation through debromination.  相似文献   

7.
Zhou P  Lin K  Zhou X  Zhang W  Huang K  Liu L  Guo J  Xu F 《Chemosphere》2012,88(11):1375-1382
Twenty-eight sediment samples were collected from the Taihu Lake and analyzed to acquire information about the levels, distribution, possible sources, time trend and inventory of polybrominated diphenyl ethers (PBDEs) in the Taihu Lake. Our results showed that the most abundant BDE congeners in surface sediments were BDE-47, 99 and 209, with a median value of 0.124, 0.279, and 22.72 ng(gdw)(-1), respectively. The levels of BDE-209 in our samples were much higher relative to those of the other BDE congeners and made up more than 80% of the PBDEs levels in almost all samples. Disregarding BDE-209, among the seven PBDEs (BDE-28, 47, 99, 100, 153, 154, 183) more concerned, the most abundant ones were BDE-47 and 99, which contributed 44.65% (ranged from 29.02% to 73.11%), 24.24% (ranged from 2.27% to 39.66%) to ∑(7)PBDEs, respectively. The correlation between PBDE and TOC was poor, indicating that PBDEs concentrations in sediments of the Taihu Lake were controlled not only by TOC contents, but also by a combined effect of transport, mixing, depositional mechanisms associated with PBDEs, uncontaminated sediments, or fresh input of PBDEs. As expected, the time trend of PBDEs concentration in surface sediment from Taihu Lake were increasing, and the inventory of ∑(25)PBDEs and BDE-209 were estimated to be 3668 kg and 26296 kg.  相似文献   

8.
The levels and congener patterns of PBDEs were investigated in human placental samples in Denmark. The median concentrations of ∑PBDEtri-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.  相似文献   

9.
Based on previous findings in dietary studies with carp (Cyprinus carpio), we investigated the mechanism of 2,2',4,4',5-pentabromodiphenyl ether (BDE-99) debromination to 2,2',4,4'-tetrabromodiphenyl ether (BDE-47) using liver and intestinal components. In vitro aerobic and anaerobic experiments tested the ability of carp intestinal microflora to debrominate BDE-99. No debromination of BDE-99 to BDE-47 was observed in microfloral samples; therefore, carp enzymatic pathways were assessed for debromination ability. After sixty-min incubation, intestine and liver microsomes exhibited 83+/-34% and 106+/-18% conversions, respectively, of BDE-99 to BDE-47; with no significant (p>0.05) difference between organ debromination capabilities. Microsomal incubations with BDE-99, enzyme cofactors and competing substrates assessed the potential mechanisms of debromination. The presence of NADPH in the microsomal assay did not significantly (p>0.05) affect BDE-99 debromination, which suggest that cytochrome P450 enzymes are not the main debrominating pathway for BDE-99. Co-incubation of BDE-99 spiked microsomes with reverse thyronine (rT3) significantly (p<0.05) decreased the debromination capacity of intestinal microsomes indicating the potential of catalytic mediation via thyroid hormone deiodinases. The significant findings of this study are that intestinal microflora are not responsible for BDE-99 debromination, however, it is an endogenous process which occurs with approximately equal activity in intestine and liver microsomes and it can be inhibited by rT3.  相似文献   

10.

Background, aim and scope  

The environmental presence of polybrominated diphenyl ethers (PBDEs), among which BDE-47 and BDE-99 are particularly abundant, makes toxicity data necessary to assess the hazard risk posed by PBDE to aquatic organisms. This study examines the effects of BDE-47 and BDE-99 on embryo-larval stages of the marine flatfish turbot.  相似文献   

11.
Birnessite mediated debromination of decabromodiphenyl ether   总被引:3,自引:0,他引:3  
Ahn MY  Filley TR  Jafvert CT  Nies L  Hua I 《Chemosphere》2006,64(11):1801-1807
Decabromodiphenyl ether (BDE-209) is a major component of a commercial flame retardant formulation; however, there is limited information on the fate of BDE-209 in the environment, including metal oxide mediated degradation. Laboratory experiments were conducted to investigate the birnessite (delta-MnO(2))-promoted debromination of BDE-209 in tetrahydrofuran (THF)-water systems as well as catechol solutions. Up to 100% (0.1044 micromol initial charge) of BDE-209 disappeared upon reaction with birnessite in THF/H(2)O (4:6-9:1). The formation of aqueous Br(-) from BDE-209 reduction was determined and up to 16 mole% of initial bromine was released over the course of the reaction indicating approximately 1.7 Br-C bonds were reduced per BDE-209 molecule. The distribution of debrominated congeners, however, indicated a much greater extent of debromination for some products than what was inferred from an average bromine mass balance. The produced congeners varied from tetra- to nona-bromodiphenyl ether, including BDE-47 and -99, during the 24 h reaction. Experiments with deuterated water indicated that water was not the major hydrogen donor in the reduction but rather THF provided the reducing power. This conclusion was supported by the presence of succinic acid, which was produced from oxidation of THF. The reactions with aqueous catechol, rather than THF-water mixtures, were performed to assess the possible role that compounds found in natural environments, such a tannin-like phenols, might have on the chemistry. These experiments indicated that birnessite mediated debromination of BDE-209 might occur in natural settings.  相似文献   

12.
Fourteen and 17 sediment samples were collected from three main rivers of Shanghai in July and November, respectively. Eight polybrominated diphenyl ether (PBDE) congeners (BDE-28, BDE-47, BDE-99, BDE-100, BDE-153, BDE-154, BDE-183, and BDE-209) were detected in these samples to clarify the pollution status in the metropolis. Instrumental analyses showed that the concentrations of ∑8PBDEs ranged from 10.97 to 64.05 ng/g dry weight (dw), with an average value of 29.71 ng/g dw. BDE-209 was the predominant congener accounting for more than 97 % of total PBDEs, followed by BDE-47 and BDE-99. Remarkable spatial and seasonal distributions of PBDE concentrations were observed, suggesting that local sources, seasonal climates, and hydrologic conditions might be the influencing factors. Moderate correlations (r 2?=?0.28–0.51, p?<?0.05) were found between total organic carbon and PBDEs, which indicated that organic carbon content influenced the distributions of PBDEs in sediment of Shanghai at some extent. Hazard quotients revealed PBDEs posed no potential risk to benthic organisms in the study area at present.  相似文献   

13.
Polybrominated diphenyl ethers (PBDEs) were measured in sewage sludge samples collected from major wastewater treatment plants in Guangdong Province, South China. Concentrations of ∑39PBDE (all 39 compounds including tri- to hepta- PBDE congeners except for BDE-209) ranged from 3.6 to 428 ng/g dw with a mean value of 67.4 ng/g dw and a median value of 25.9 ng/g dw, and those of BDE-209 ranged from 9.9 to 5,010 ng/g dw (mean 1,024 ng/g dw and median 824 ng/g dw). The PBDE mixtures detected were mainly comprised of penta-, octa-, and deca-BDEs, with deca-BDE as the dominant constituent. The most abundant congeners, excluding BDE-209, were BDE-47, BDE-99, and BDE-183. Good correlations were found among the concentrations of BDE-47, BDE-99, BDE-100, BDE-138, and BDE-154 (r?>?0.8). However, poor correlations were found between the concentrations of BDE-209 and all other congeners (r?<?0.3). This fact suggests that most tri- to hepta-BDEs detected did not originate from decomposition of deca-BDE. The estimated annual emission of ∑allPBDEs, ∑39PBDEs, penta-BDE, octa-BDE, and deca-BDE to the Pearl River Delta environment (PRD), based on the sludge samples analyzed, amounts to 232, 20.2, 5.5, 1.7, and 212 kg per year, implicating sewage sludge as a significant source of PBDEs to the PRD environment.  相似文献   

14.
Xin J  Liu X  Jiang L  Li M 《Chemosphere》2012,87(5):477-482
Three loamy-clay soil samples (LC1-3) with different properties were collected as the geosorbents to preliminarily investigate the sorption and desorption of 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) in single system and binary system with the presence of decabromodiphenyl ether (BDE-209), which can provide information in order to further understand the sorption mechanisms and evaluate the adsorption sites. A concentration of 10 μg L−1 BDE-209 suppressed the sorption of BDE-47, and the trend became more and more significant with the increase of BDE-47 equilibrium concentration, however, BDE-47 caused no competitive effect on BDE-209 sorption, which was related with the better accessibility of more hydrophobic molecules to adsorption sites. In the binary system, nonlinearity of the BDE-47 sorption isotherms for the three samples changed in different ways, which originated from the varied soil properties. Desorption hysteresis was observed in all cases, which was estimated due to irreversible surface adsorption between sorbent and sorbate. BDE-209 made desorption of BDE-47 more hysteretic from soil samples, which was estimated to be ascribed to the accelerated sorbent state transition and new sites creation caused by BDE-209 sorption.  相似文献   

15.
Peng JH  Huang CW  Weng YM  Yak HK 《Chemosphere》2007,66(10):1990-1997
Polybrominated diphenyl ethers (PBDEs) have been used extensively over the past two decades as flame retardants in many types of polymers, and have been found to be a class of contaminants of concern. Measurements of PBDEs in various environmental matrices from Sweden, Holland, Japan, North America, and elsewhere have been reported. We report data of PBDEs in fish samples taken from six rivers and three estuaries in Taiwan. Seven PBDE congeners were observed in all sixty samples. BDE-47 was found to be the dominant congener in all waters, and BDE-154 contributed more than BDE-99 and BDE-100. Nonetheless, BDE-154 and BDE-183 were the predominant congeners in some species studied. These results are somewhat different from those from other countries, where the pattern is typically BDE-47 > 99 >100 >154, 153, and is postulated to be due to the extensive use of octa-BDE rather than penta-BDE in Taiwan. The average concentration distribution across all samples of the sum of PBDE congeners ranged from 30.6 ng/g lipid to 281 ng/g lipid. The concentrations of PBDEs in fishes reported here are higher than those reported from European countries, but lower than those from the United States.  相似文献   

16.
Atmospheric PBDEs were measured on a monthly basis in 2002–2004 at Point Petre, a rural site in the Great Lakes. Average air concentrations were 7.0 ± 13 pg m?3 for Σ14BDE (excluding BDE-209), and 1.8 ± 1.5 pg m?3 for BDE-209. Concentrations of 3 dominant congeners (i.e., BDE-47, 99, and 209) were comparable to previous measurements at remote/rural sites around the Great Lakes, but much lower than those at urban areas. Weak temperature dependence and strong linear correlations between relatively volatile congeners suggest importance of advective inputs of gaseous species. The significant correlation between BDE-209 and 183 implies their transport inputs associated with particles. Particle-bound percentages were found greater for highly brominated congeners than less brominated ones. These percentages increase with decreasing ambient temperatures. The observed gas/particle partitioning is consistent with laboratory measurements and fits well to the Junge–Pankow model. Using air mass back-trajectories, atmospheric transport to Point Petre was estimated as 76% for BDE-47, 67% for BDE-99, and 70% for BDE-209 from west–northwest and southwest directions. During the same time period, similar congener profiles and concentration levels were found at Alert in the Canadian High Arctic. Different inter-annual variations between Point Petre and Alert indicate that emissions from other regions than North America could also contribute PBDEs in the Arctic. In contrast to weak temperature effect at Point Petre, significant temperature dependence in the summertime implies volatilization emissions of PBDEs at Alert. Meanwhile, episodic observations in the wintertime were likely associated with enhanced inputs through long-range transport during the Arctic Haze period.  相似文献   

17.
In this study we evaluated the use of Talitrus saltator as biomonitor of polybrominated diphenyl ethers (PBDEs) contamination of the supralittoral zone of Mediterranean sandy shores, an area characterized by a strong input of contaminants but not yet investigated about the presence of these pollutants. We detected the presence of twenty PBDE congeners in amphipods and sand samples collected along the Tyrrhenian coast of central Italy. Eight congeners were detected in all samples. Among them, the BDE-209 was the most abundant in both amphipods and sand samples followed by BDE-99, BDE-153 and BDE-47 in animals, and BDE-99, BDE-47 and BDE-100 in sediment. The ΣPBDEs in amphipods was higher (on the average 2.5-5-fold) than in sand for almost the totality of congeners detected and each sampling site, suggesting the good capacity of sandhoppers to accumulate these pollutants. Moreover statistical analysis revealed significant differences in PBDE concentrations recorded in tissues of T. saltator among sampling sites. Therefore our results suggested the possible utilization of T. saltator as a biomonitor of PBDE contamination of the supralittoral zone of Mediterranean sandy shores.  相似文献   

18.
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.  相似文献   

19.
Ninety-six riverine runoff samples collected at eight major outlets in the Pearl River Delta (PRD), South China, during 2005-2006 were analyzed for 17 brominated diphenyl ether (BDE) congeners (defined as Σ17PBDE). Fourteen and 15 congeners were detected, respectively, in the dissolved and particulate phases. These data were further used to elucidate the partitioning behavior of BDE congeners in riverine runoff. Several related fate processes, i.e. air-water exchange, dry and wet deposition, degradation, and sedimentation, within the Pearl River Estuary (PRE), were examined to estimate the inputs of Σ10PBDE (sum of the target BDE congeners, BDE-28, -47, -66, -85, -99, -100, -138, -153, -154, and -183) and BDE-209 from the PRD to the coastal ocean based on mass balance considerations. The results showed that annual outflows of Σ10PBDE and BDE-209 were estimated at 126 and 940 kg/year, respectively from the PRE to coastal ocean. Besides sedimentation and degradation, the majority of Σ10PBDE and BDE-209 discharged into the PRE via riverine runoff was transported to the coastal ocean.  相似文献   

20.
Zhang L  Li J  Zhao Y  Li X  Yang X  Wen S  Cai Z  Wu Y 《Chemosphere》2011,84(5):625-633
Seven polybrominated diphenyl ethers (PBDEs) congeners (BDE-28, BDE-47, BDE-99, BDE-100, BDE-153, BDE-154 and BDE-183) and six indicator polychlorinated biphenyls (PCBs) congeners (CB-28, CB-52, CB-101, CB-138, CB-153 and CB-180) were measured in 24 pooled human milk samples comprised of 1237 individual samples from 12 provinces in China. The samples were taken to estimate the background body burden of general population and assess nursing infant exposure via human milk in China. The median concentrations of ∑7PBDEs and ∑6PCBs were 1.49 and 10.50 ng g−1 lipid weight (lw), respectively. BDE-28, BDE-47 and BDE-153 were predominant PBDE congeners accounting for nearly 70% of ∑7PBDEs. As for indicator PCBs, CB-153 was the most abundant congener, followed by CB-138. In our study, there was no significantly statistical relationship between concentrations of PBDEs in milk samples and maternal age as well as dietary habits. ∑7PBDEs did not correlate to ∑6PCBs in Chinese mothers’ milk. The human exposure to indicator PCBs in China was found to be significantly determined by maternal age, dietary habits and geographical factors. It is suggested that Chinese general population is probably exposed to PBDEs with multiple sources and pathways. The estimated daily intakes (EDI) of BDE-47, BDE-99 and BDE-153 for the Chinese nursing infant were much lower than corresponding threshold reference values suggested by USEPA.  相似文献   

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