Validation of a passive atmospheric deposition sampler for polybrominated diphenyl ethers

An atmospheric deposition sampler was validated with respect to polybrominated diphenyl ethers (PBDEs), a compound group that is widely used as flame retardants in many types of consumer products. The deposition sampler consists of an adsorption cartridge that is connected to a glass funnel. Extraction tests with spiked cartridges using soxhlet extraction with acetone revealed recoveries of >80% for all of the investigated PBDEs. Once adsorbed, PBDEs are stable, as proven by extractions of spiked cartridges that were stored outdoors and collected after different periods of time, up to 84 days. High recoveries indicate that degradation of adsorbed PBDEs does not play a role under realistic field conditions. Bulk deposition rates of PBDEs were determined in a field test with 3 replicates, and a possible breakthrough of target compounds was assessed in the field using a second adsorption cartridge in series. No breakthrough of target compounds could be observed within a sampling period of 61 days, and a bulk deposition rate of approximately 1 ng m(-2) day(-1) for the sum of all analysed PBDEs was measured. The highest deposition rates were measured for octa-brominated congeners, followed by BDEs 99, 183, 153, and 47. Overall, the sampler was successfully validated regarding the atmospheric deposition of PBDEs.     

Dehalogenation of polychlorinated biphenyls and polybrominated diphenyl ethers using a hybrid bioinorganic catalyst

The environmentally prevalent polybrominated diphenyl ether (PBDE) #47 and polychlorinated biphenyls (PCBs) #28 and #118 were challenged for 24 hours with a novel biomass-supported Pd catalyst (Bio-Pd(0)). Analysis of the products via GC-MS revealed the Bio-Pd(0) to cause the challenged compounds to undergo stepwise dehalogenation with preferential loss of the least sterically hindered halogen atom. A mass balance for PCB #28 showed that it is degraded to three dichlorobiphenyls (33.9%), two monochlorobiphenyls (12%), and biphenyl (30.7%). The remaining mass was starting material. In contrast, while PCB #118 underwent degradation to yield five tetra- and five trichlorinated biphenyls, no less chlorinated products or biphenyl were detected, and the total mass of degraded products was 0.3%. Although the Bio-Pd(0) material was developed for treatment of PCBs, a mass balance for PBDE #47 showed that the biocatalyst could prove a potentially useful method for treatment of PBDEs. Specifically, 10% of PBDE #47 was converted to identifiable lower brominated congeners, predominantly the tribrominated PBDE #17 and the dibrominated PBDE #4, 75% remained intact, while 15% of the starting mass was unaccounted for.     

A national probabilistic study of polybrominated diphenyl ethers in fish from US lakes and reservoirs

Polybrominated diphenyl ethers (PBDEs) are persistent, bioaccumulative, and toxic chemicals that are present in air, water, soil, sediment, and biota (including fish). Most previous studies of PBDEs in fish were spatially focused on targeted waterbodies. National estimates were developed for PBDEs in fish from lakes and reservoirs of the conterminous US (excluding the Laurentian Great Lakes) using an unequal probability design. Predator (fillet) and bottom-dweller (whole-body) composites were collected during 2003 from 166 lakes selected randomly from the target population of 147,343 lakes. Both composite types comprised nationally representative samples that were extrapolated to the sampled population of 76,559 and 46,190 lakes for predators and bottom dwellers, respectively. Fish were analyzed for 34 individual PBDE congeners and six co-eluting congener pairs representing a total of 46 PBDEs. All samples contained detectable levels of PBDEs, and BDE-47 predominated. The maximum aggregated sums of congeners ranged from 38.3 ng/g (predators) to 125 ng/g (bottom dwellers). Maximum concentrations in fish from this national probabilistic study exceeded those reported from recent targeted studies of US inland lakes, but were lower than those from Great Lakes studies. The probabilistic design allowed the development of cumulative distribution functions to quantify PBDE concentrations versus the cumulative number of US lakes from the sampled population.     

Organochlorines and polybrominated diphenyl ethers in four geographically separated populations of Atlantic salmon (Salmo salar)

Atlantic salmon (Salmon salar) populations from four locations, two from isolated Swedish lake systems, one of the Baltic Sea and one of the North Atlantic, were analyzed to determine the concentrations and spatial variations of polybrominated diphenyl ethers (PBDEs) and organochlorines (DDT, PCB and HCH). Levels in both liver and muscle were in the same range as previously reported in Atlantic salmon, except for elevated concentrations found per lipid weight (lw) in the muscle samples of salmon from the North Atlantic ( summation PBDE 263 ng g(-1) lw, summation PCB 3262 ng g(-1) lw, summation DDT 4063 ng g(-1) lw summation HCH 131 ng g(-1)). In general, elevated concentrations in the muscles compared to the liver were observed, especially in lipid depleted migrating salmon, possibly caused by a faster lipid depletion compared with the redistribution of PBDEs, PCBs and DDTs. These findings indicated that the life stage and thereby the lipid dynamics of the fish must be considered prior to comparison based on lipid weight, especially as Atlantic salmon experience large variations in lipid content during periods of migration. The dominating PBDE congener was BDE-47, representing more than 25% in all fish. The PBDE pattern changed between locations, with a significant separation of the fish from the freshwater and marine environment when analyzed using principal component analysis.     

Detection of polybrominated diphenyl ethers in tilapia (Oreochromis mossambicus) from O'ahu, Hawai;i

Polybrominated diphenyl ethers (PBDEs) have been detected for the first time at a range from 231.58 to 685.61 ng g(-1) lipid weight in the muscles of tilapia (Oreochromis mossambicus) collected from O'ahu, an island of the geographically isolated Hawaiian archipelago.     

New evidences in the complexity of contamination of the lagoon of Venice: polybrominated diphenyl ethers (PBDEs) pollution

This study presents the first evaluation of the current pollution by polybrominated diphenyl ethers (PBDEs) of surface sediments from the Lagoon of Venice. We focused the research on tri-to hepta-BDEs, the main components of penta- and octa-mixtures, which are considered to be the most toxic for the biocoenosis. The results pointed out a quite homogeneous contamination of this keystone European transitional environment, with ∑ ₁₃PBDEs values ra nging from 0.39 to 6.78 ng/g dry weight; these values reflect low to moderate pollution levels, which is in conformity to other coastal European ecosystems. The average PBDE profile of the lagoon sediments follows this decreasing trend of congeners: BDE-47>BDE-99> >BDE-190>BDE-28>BDE-153>BDE-154>BDE-138, BDE-183, and BDE-17, which is similar to the worldwide distribution pattern. BDE-47 and BDE-99 revealed a recent use of a penta-BDE mixture, while the presence of hepta-BDEs (BDE-183 and BDE-190) in all of the sites can indicate the actual use of a deca-BDE formulation, because these congeners are considered to be debrominated byproducts of BDE-209 degradation.     

Preliminary assessment of polybrominated diphenyl ethers (PBDEs) in the Scottish aquatic environment, including the Firth of Clyde

This paper presents preliminary data on polybrominated diphenyl ethers (PBDEs) in the Scottish aquatic environment. Sediment and biota (fish liver, fish muscle and mussels) from a number of locations around Scotland were analysed for PBDEs with samples being from both remote and from potentially contaminated areas such as the former sewage sludge dump site at Garroch Head in the Clyde. PBDEs were measured in both cultivated, rope grown mussels and wild mussels collected from 5 sites around Scotland in 2006. Total PBDE concentrations (sum of tri- to hepta-BDEs) ranged from 相似文献   

Occurrence, distribution, and source of polybrominated diphenyl ethers in soil and leaves from Shenzhen Special Economic Zone, China

Polybrominated diphenyl ethers (PBDEs) were measured in soil and three plant species samples taken at different land use areas in Shenzhen China. The concentrations of ??₇BDEs (BDE-28, BDE-47, BDE-99, BDE-100, BDE-153, BDE-154, and BDE-183) and BDE-209 in the surface soils ranged from 0.23 to 271 and 8.9 to 5,956 ng/g dry weight (dw), respectively. These figures are comparable to that in the soils of electronic waste dismantling sites. BDE-209 was the predominant congener (contributes 85?C99% of ??₈PBDEs (??₇PBDEs plus BDE-209)) in soils. The regression slopes of total organic carbon and individual BDE congeners were rather gentle, indicating that factors other than soil organic matter regulated the soil concentrations. Proximity to sources of deposition processes might be the major factors. In the plant leaves, ??₇BDEs and BDE-209 concentrations ranged from 1.29 to 5.91 and 5.49 to 28.2 ng/g dw, respectively. BDE-209 is also the dominant component, but the contribution was much lower compared with that in soils. Bauhinia purpurea Linn. and Michelia alba DC. show some similarities on the uptake of PBDEs, while Ficus microcarpa var. pusillifolia is different from them. The correlations between plant leaf concentrations and predicted gaseous concentrations were moderate, indicating that gaseous concentration did not influence the leaf concentration significantly.     

Personal air sampling and analysis of polybrominated diphenyl ethers and other bromine containing compounds at an electronic recycling facility in Sweden

Brominated flame retardants (BFRs) have been used extensively and are considered ubiquitous contaminants. To evaluate exposure to brominated flame retardants within an electronic recycling facility personal air monitoring was done during a two year period. A total of 22 polybrominated diphenyl ethers (PBDEs) and 2 other bromine containing organic compounds have been analysed and evaluated in 17 personal air samples. The most abundant congeners of PBDE was #209 (<0.7-61 ng m(-3)), #183 (<0.1-32 ng m(-3)) indicating the use of the commercial octaBDE mixture, followed by PBDE #99 and #47 (<1.3-25 and <0.9-16 ng m(-3), respectively). The second most abundant peak in the chromatogram from all samples was identified as 1,2-bis(2,4,6-tribromophenyxy)ethane (BTBPE) in the concentration range <0.6-39 ng m(-3) (semi-quantitatively calculated against PBDE #191). A second bromine containing compound was also detected, structurally similar to decabromodiphenyl ethane (DeBDethane), however no definite identification could be made. The air samples were also evaluated on a work exposure category basis. The workers represented three different categories: dismantlers, other workers and unexposed. There was a significant difference (p < 0.05 with the Mann-Whitney test) among the dismantlers and the unexposed categories for PBDE congeners #47, #100, #99, #154; #153, #183, #209 and BTBPE. Another observation was that the air concentrations of PBDEs and BTBPE in the breathing zone were negatively correlated (p < 0.05) to the amount of recycled material (in kg). The present work shows that the exposure to brominated flame retardants varied within the electronic facility and that further research is needed to evaluate how the exposure differs with different products being dismantled as well as how the bioavailability of the different BFRs to humans is related to particle exposure.     

Temporal trend studies on polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs) in ringed seals from east Greenland

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%.     

Levels and congener profiles of polybrominated diphenyl ethers (PBDEs) in primipara breast milk from Shenzhen and exposure risk for breast-fed infants

This study aimed at revealing the levels of polybrominated diphenyl ethers (PBDEs) in breast milk from primipara in Shenzhen (China), and estimating daily intake of PBDEs for breast-fed infants. Concentrations of 7 PBDEs were measured in 60 breast milk samples by isotope dilution HRGC/HRMS (high-resolution gas chromatography/high-resolution mass spectrometry). The intake of PBDEs for breast-fed infants was estimated based on the infant's daily milk consumption. The range of total concentration of 7 PBDEs congeners in samples was 2.6-188.6 ng g(-1) lipid (mean: 14.8 ng g(-1) lipid; median: 7.2 ng g(-1) lipid). The mean estimated daily intake of PBDEs by breast-fed infants ranged from 9.9 to 335.9 ng kg(-1) body weight (bw) per day (mean: 52.5 ng kg(-1) bw per day; median: 28.6 ng kg(-1) bw per day). The levels of PBDEs body burden in the recruited mothers of Shenzhen were higher than those reported previously for the general population from other areas in China. No significant correlations were found between the body burden of PBDEs and the mothers' age, pre-pregnancy BMI, dietary habits, duration of residence in Shenzhen, weight and length of the newborns. BDE-47 and BDE-153 were major PBDE congeners in milk samples, while the congeners of BDE-183 and BDE-28 were also high in Shenzhen. The situation may be attributed to the special economic pattern including electronic production in Shenzhen in the past three decades. Continuous surveillance on PBDEs levels in human milk is needed in order to accurately evaluate the environmental impact of PBDEs to human health in Shenzhen.     

Preliminary screening of polybrominated diphenyl ethers (PBDEs), hexabromocyclododecane (HBCDD) and tetrabromobisphenol A (TBBPA) flame retardants in landfill leachate

The occurrence of selected brominated flame retardants, including nine polybrominated diphenyl ether (PBDE) congeners, hexabromocyclododecane (HBCDD) and tetrabromobisphenol A (TBBPA) in leachate samples from eight landfill sites in South Africa, were investigated. In addition, the possible influences of dissolved organic carbon on their levels were also evaluated. Filtered leachate samples were subjected to solid-phase extraction to isolate the various target compounds. PBDEs with six bromine substituents and above, as well as α-HBCDD, β-HBCDD and TBBPA, were generally found below the detection limit. However, the mean value of the total lower PBDE congeners ranged between 0.04 and 0.48 μg L^?1, and the concentrations of γ-HBCDD ranged from not detectable (ND) to 0.05 μg L^?1. No significant correlation was observed between the target compounds and dissolved organic carbon, although weak to moderate correlations were mostly observed for the lower PBDEs.     

Occurrence of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs) in Lake Maggiore (Italy and Switzerland)

Samples of air (gas and particulate phases), bulk deposition, aquatic settling material and sediments were collected in Lake Maggiore (LM) in order to determine their content of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs). Air (gas and particulate phases) concentrations were 0.5 pg m(-3), 80 pg m(-3), 13 pg m(-3) and 106 pg m(-3) for SigmaPCDD/Fs, SigmaPCBs, Sigma dioxin-like PCBs (DL-PCBs) and SigmaPBDEs, respectively. Deposition fluxes ranged from 0.7 ng m(-2) d(-1) for SigmaPCDD/Fs to 32 ng m(-2) d(-1) for SigmaPCBs. Aquatic settling material presented concentrations of 0.4 ng g(-1) dry weight (dw) for SigmaPCDD/Fs, 13 ng g(-1) dw for SigmaPCB, 3.4 ng g(-1) dw for SigmaDL-PCBs and 5.7 ng g(-1) dw for SigmaPBDEs. Mean sediment concentrations were 0.4 ng g(-1) dw for SigmaPCDD/Fs, 11 ng g(-1) dw for SigmaPCB, 3 ng g(-1) dw for SigmaDL-PCBs and 5.1 ng g(-1) dw for SigmaPBDEs. Similar PCDD/F and DL-PCB congener patterns in all the environmental compartments of LM point to an important, if not dominant, contribution of atmospheric deposition as source of these pollutants into LM. In contrast, PBDE congener distribution was not similar in the different environmental compartments. BDE 47 dominated air and settling material, while BDE 209 was the predominant congener in the bulk atmospheric deposition. Moreover, sediments showed two distinct PBDE congener profiles. Lower PBDE concentrated sediments were dominated by congeners 47 and 99, while BDE 209 dominated in higher PBDE concentrated samples. This suggests the influence of local sources as well as atmospheric input of PBDEs into LM.     

Polybrominated diphenyl ethers and organochlorine pesticides in human breast milk from Massachusetts, USA

Concentrations of polybrominated diphenyl ethers (PBDEs), and organochlorine pesticides (OCPs; DDTs, HCHs, CHLs, and HCB) were measured in human breast milk samples collected across Massachusetts, USA, in 2004. Seventeen PBDE congeners were found in the samples, ranging in concentration from 0.06 to 1910 ng g(-1) lipid wt. BDE-47 (2,2',4,4'-tetraBDE), BDE-99 (2,2',4,4',5-pentaBDE), and BDE-100 (2,2',4,4',6-pentaBDE) were the major congeners detected in breast milk samples. Overall mean (+/-SD) concentrations of DDTs, HCHs, CHLs, and HCB were 64.5 +/- 75, 18.9 +/- 19, 32.4 +/- 36, and 2.3 +/- 2.2 ng g(-1) lipid wt, respectively. Concentrations of PBDEs were strongly correlated with concentrations of OCPs in the samples. Based on the concentrations of organohalogens and the intake rates of breast milk by infants in the United States, daily ingestion rates of contaminants were calculated. The median ingestion rates for PBDEs, HCHs, DDTs, CHLs, and HCB were 4.0, 212, 141, 44, and 5.79 ng kg(-1) body wt day(-1), respectively. The estimated daily intake of organohalogens by infants was compared with threshold reference values suggested by the United States Environmental Protection Agency (USEPA) and the Agency for Toxic Substances and Disease Registry (ATSDR), for calculation of hazard quotients (HQs). HQs for individual organohalogens and the sum of HQ for all organohalogens were calculated as HQ indices (HQI). The results suggest that one or more of the contaminants analyzed in this study exceeded the threshold reference values in at least 26% of the breast milk samples.     

Polybrominated diphenyl ethers (PBDEs) in freshwater mussels and fish from Flanders, Belgium

The levels and distribution of PBDEs in zebra mussels and several freshwater fish species (eel, carp and gibel carp) were investigated for different sites in Flanders, Belgium. In parallel, other organohalogenated contaminants, such as polychlorinated biphenyls (PCBs), p,p[prime or minute]-DDE and hexachlorobenzene (HCB) were also measured and their relationship with PBDEs was investigated. At most sites, individual PBDE congeners were present at detectable levels in mussel tissue, with the mean [summation operator]PBDE concentration ranging from 0.15 to 1.8 ng g(-1) wet weight (ww). The PCB concentrations in mussels ranged from 6.2 to 102 ng g(-1) ww. HCB and p,p[prime or minute]-DDE could be measured in mussels from most sites, mean values ranging from below the limit of quantification (LOQ) to 0.58 ng g(-1) ww and from 0.66 to 6.5 ng g(-1) ww, respectively. Except for one site (Blokkersdijk, Antwerp) where PBDEs were below the LOQ in carp muscle, all fish samples from other sites contained detectable PBDE levels, with the highest concentrations (14 +/- 14 ng g(-1) ww) being measured in eel liver from Watersportbaan (Ghent). The sampled sites covered a broad concentration range of organohalogenated pollutants with the highest values being consistently measured in eel liver. With few exceptions, all correlations between PBDEs and organochlorine pollutants for each species were low (r < 0.50) and most were statistically not significant (p > 0.05). This suggests that the exposure to contaminants arises from local sources possessing different signatures of PBDEs and organochlorine pollutants.     

Polybrominated diphenyl ethers (PBDEs) in the riverine and marine sediments of the Laizhou Bay area, North China

62 riverine and marine sediments were collected from the Laizhou Bay area, where the largest manufacturing base of brominated flame retardants (BFRs) in Asia is located. Eight polybrominated diphenyl ethers (PBDEs) were analyzed to investigate the impact of rapidly-developed bromine industries on the regional aquatic system. PBDE concentrations varied largely in riverine sediments. Σ(7)PBDEs (including BDE 28, 47, 99, 100, 153, 154 and 183) and BDE 209 ranged from 0.01 to 53 ng g(-1) dw and from 0.74 to 285 ng g(-1) dw with a mean value of 4.5 ng g(-1) dw and 54 ng g(-1) dw, respectively, indicating a strong influence of direct pollution discharges from local factories. In marine sediments, Σ(7)PBDEs and BDE 209 ranged from not detected (nd) to 0.66 ng g(-1) dw and from 0.66 to 12 ng g(-1) dw with a mean value of 0.32 ng g(-1) dw and 5.1 ng g(-1) dw, respectively. PBDE concentrations were mostly <10 ng g(-1) dw for Σ(7)PBDEs and <50 ng g(-1) dw for BDE 209, which are at a relatively low level for monitored riverine and coastal sediments around the world. Even at the most contaminated sites in Laizhou Bay area, PBDE concentrations were not among the highest concentrations reported in the literature. Congener compositions were dominated by BDE 209 (57.2-99.9% of the sum of BDE congeners), with minor contributions from penta- and octa-BDE products. Tri- to octa-BDE congeners were well correlated among each other (r > 0.75) and thus sources from similar mixing of penta- and octa-BDE products were suggested in this area. Compared with riverine sediments, a much better correlation between PBDE concentrations with TOC was observed in marine environment. The congener pattern changed and their correlation coefficients among each other were remarkably reduced. Contributions of BDE 28, 47 and 99 to Σ(7)PBDEs were generally the same in almost all the marine sites, while it was distinctively higher for BDE 153. These are probably attributable to several reasons, such as contributions by atmospheric deposition and/or redistribution between particles of various sizes during and/or after fluvial transportation combined with the difference of physiochemical properties of BDE congeners.     

气相色谱法测定空气和废气中联苯-联苯醚

研究了气相色谱法测定环境空气和废气中的联苯-联苯醚.气体样品由中性氧化铝吸收,二硫化碳洗脱,FID检测.方法有较好的精密度(变异系数联苯12.4%,联苯醚10.6%;回收率联苯86.6%～100%,联苯醚88.6%～95.7%)和低的检出浓度(联苯0.056mg/m3,联苯醚0.044mg/m3);方法具有简便、快速、准确的特点.     

Assessment of risk to public health posed by persistent organochlorine pesticide residues in milk and milk products in Mumbai, India

The risk posed by the presence of organochlorine pesticides in milk and milk products was estimated for the population of Mumbai. To determine the levels of organochlorine pesticides in milk and milk products, a monitoring study was carried out in and around Mumbai City. 520 samples of milk and milk products of different brands were considered in this study. A survey was also conducted to determine the mean daily consumption of milk and milk products by different age groups and this data was used to evaluate the daily exposure to the public. Non-cancer effects were evaluated by comparing the predicted exposure distributions to the published guidance values. For chemicals identified as potential human carcinogens, cancer risk was evaluated using standard methodology. The majority of the chlorinated pesticides identified in the milk and milk product samples studied were found to be at levels which do not pose unacceptable risks to the public, with the exception of alpha-HCH. The cancer risk estimated for this chemical slightly exceeds the US EPA guidance value.