Trends Of Polybrominated Diphenyl Ethers Research Articles

Spatiotemporal Trends of Legacy and Alternative Flame Retardants in Harbor Seals from the Coasts of California, the Gulf of Maine, and Sweden.

Temporal trends of polybrominated diphenyl ethers (PBDEs) have been extensively studied in various environmental compartments globally. However, despite the increasing use of alternative flame retardants following PBDE bans, the spatiotemporal trends of these replacements have rarely been studied, and the available results are often inconsistent. In the present study, we retrospectively investigated the spatiotemporal trends of PBDEs and a suite of alternative brominated FRs (aBFRs) and chlorinated FRs (i.e., dechloranes or DECs) in three harbor seal (Phoca vitulina) populations from the coasts of California, the Gulf of Maine, and southern Sweden during 1999-2016. We observed significantly decreasing trends of ΣPBDEs in all the three populations at an annual rate of 9-11%, which were predominantly driven by the declining concentrations of tetra- and penta-BDEs. The levels of ΣaBFRs decreased significantly in seals from California (mainly 1,3,5-tribromobenzene) and Sweden (mainly hexabromobenzene), while no trend was observed for those from Maine. By contrast, DECs (dominated by DEC 602) did not decrease significantly in any population. Compared with the consistent PBDE congener profiles across regions, aBFRs and DECs exhibited varying compositional profiles between regions, likely indicating region-specific sources of these alternative FR mixtures. Spatial analysis also revealed regional differences in the concentrations of PBDEs, aBFRs, and DECs in harbor seals. Our reconstructed spatiotemporal trends suggest the effective regulation of commercial penta-BDE mix in these regions and warrant further monitoring of the higher brominated BDEs and alternative FRs.

Contamination levels and temporal trends of legacy and current-use brominated flame retardants in a dated sediment core from Beppu Bay, southwestern Japan

Contamination levels and temporal trends of polybrominated diphenyl ethers (PBDEs) and some alternative brominated flame retardants (BFRs) were examined in a dated sediment core from the deepest part of the Beppu Bay, southwestern Japan. PBDEs were found in the upper layers of 0–15 cm depth at concentrations ranging from 5200 to 32,600 pg g−1 with the peak estimated at 1995. Decabromodiphenyl ether (BDE-209) was the most abundant congener, accounting for 96% in average of total PBDEs. The vertical profile of BDE-209 observed in our sediment core generally agreed with the historical pattern of domestic demand of commercial deca-BDE mixtures in Japan, and perfectly matched with maximum stock of these products (i.e., 42,000 tons in 1995). Among alternative BFRs, only decabromodiphenyl ethane (DBDPE), a replacement of deca-BDE, was found at significant levels with concentrations of 69–850 pg g−1 in sediment layers dated between 1991 and 2011. Ratios of DBDPE to BDE-209 gradually increased during this period, implying opposite trends of these two compounds and the role of DBDPE as a deca-BDE’s alternative. The occurrence of deca-BDE components in sediments may pose medium risk to benthic aquatic life, while the ecological risk of other PBDE homologs and DBDPE was negligible.

Global distribution and trends of polybrominated diphenyl ethers in human blood and breast milk: A quantitative meta-analysis of studies published in the period 2000–2019

Polybrominated diphenyl ethers (PBDEs) are a class of flame-retardants that are found throughout the human body. However, global trends and diversity of the concentrations in human body and the potential risks remain largely unresolved. Based on published data during 2000–2019, we conducted a systematic meta-analysis to understand the burden and risks of PBDEs in humans and their spatiotemporal variations. The report provides a global picture of PBDE concentrations in human blood and breast milk. We found the levels of body PBDE burden in the North American population were higher than those from Asia and Europe. However, high concentrations of blood PBDEs in occupational population from Asia were observed, largely because of poorly controlled e-waste recycling operations. Penta- and deca-BDE were the main contributors in North America and Asia, respectively, reflecting the difference in the production and use of these chemicals. On a global scale, no substantial decreases in the concentrations of PBDEs in the blood and breast milk were observed, although most of the chemicals have been phased out. The results suggested that humans will be exposed to PBDEs with relatively high concentrations in a certain period because of the legacy in products and the environmental media. And the potential health risks necessitate careful study in the future. Our results also remind that the uses of degradation-resistant chemicals should be attached great importance to their safety.

Concentration profile, spatial distributions and temporal trends of polybrominated diphenyl ethers in sediments across China: Implications for risk assessment

Polybrominated diphenyl ethers (PBDEs) in sediments of China have been extensively investigated; however, most studies conducted to date have focused on specific locations, and the pollution and risk posed by these chemicals in sediments at the national scale remain unknown. Therefore, we analyzed the concentrations and risks of PBDEs in sediments in China and their spatiotemporal variations based on available literature. Overall, the sediments across China contain moderate to high levels of PBDEs, with BDE-209 being the dominant congener, followed by BDE-47 and BDE-99. The sediment concentrations of PBDEs were highest in southern China and lowest in northeastern China. Additionally, based on their PBDE concentrations, 18.4%, 30.0%, and 11.9% of sediment samples from rivers, lakes, and coastal waters, respectively, posed low to moderate eco-toxicological risks, but 6.90% of river sediments posed high risks. Between 2001 and 2017, the concentrations and risks of PBDEs in the sediments from rivers and coastal waters tended to decrease gradually. Additionally, there were low to moderate risks from PBDEs in lake sediments, and the risks in 2012–2017 were 3.30 times higher than those in 2006–2011. However, more studies about the spatial and temporal trends in PBDEs in sediment across China and their impacts on aquatic organisms are needed because there is still a general lack of relevant information.

Recent findings of halogenated flame retardants (HFR) in the German and Polar environment

To get an overview about distribution, levels and temporal trends of polybrominated diphenyl ethers (PBDE) and halogenated flame retardants (HFR) of emerging concern, different types of environmental samples archived in the German Environment Specimen Bank as well as fish filet samples from the Arctic (n = 13) and Antarctica (n = 5) were analysed for 43 substances (24 PBDE, 19 HFR) using a multi-column clean-up and GC-API-MS/MS or GC-MS. Sample types were herring gull egg (n = 3), blue mussel (n = 3) and eelpout filet (n = 3) from the German North- and Baltic Sea, bream filet (n = 7), zebra mussel (n = 6) and suspended particulate matter (SPM, n = 7) from German freshwater ecosystems as well as tree leaves (n = 9)/shoots (n = 10), soil (n = 4), earthworm (n = 4) and deer liver (n = 7) as representatives of German terrestrial ecosystems. PBDE and emerging HFR were present in each investigated matrices from Germany and Polar regions showing their widespread distribution. The presence in Arctic and Antarctic fish samples confirms their long-range transport potential. Average concentrations of total emerging HFR were highest in SPM (26 ng g−1 dry weight (dw)), zebra mussel (10 ng g−1 dw) and herring gull egg (2.6 ng g−1 dw). Lowest levels were measured in fish filet samples from Antarctica (0.02 ng g−1 dw). Average total PBDE concentrations were highest in bream filet (154 ng g−1), herring gull egg (61 ng g−1 dw), SPM (21 ng g−1 dw), and zebra mussel 18 (ng g−1) and lowest in deer liver (0.04 ng g−1 dw). The patterns of non-fauna terrestrial samples (leaves, shoots, soil) as well as SPM were dominated by DBDPE and BDE209. Elevated proportions of DPTE and in most cases the absence of DBDPE characterized all fauna samples with the exception of Polar samples. Overall, emerging HFR appeared to be less bioaccumulative than PBDE. Temporal trends were generally decreasing with few exceptions such as DBDPE.

Temporal trends of polybrominated diphenyl ethers in the sediment cores from different areas in China

This paper presented the historical data on the temporal trends of polybrominated diphenyl ethers (PBDEs) in the sediment cores collected from the Huaihe River, Yellow River and Chaohu Lake, China. Among the 40 targeted PBDE congeners, only 10, 6, and 9 of them were detected respectively in the samples from the Huaihe River, Yellow River and Chaohu Lake. On average, the total PBDEs concentrations in sediments were highest in Chaohu Lake followed by the Huaihe River and the Yellow River. As compared to other PBDE congeners, BDE-209 had higher concentrations and detection rates. The similar down core variation between PBDEs and total organic carbon (TOC) suggests that TOC is an important factor influencing PBDEs distribution in the sediments. The total PBDEs concentrations showed an increasing trend from bottom to upper sediments before a decreasing trend in the topmost sediments. The rapid urbanization and industrialization of these regions in recent decades may cause the historically increasing concentrations of sedimentary PBDEs, especially BDE-209. The decreasing PBDEs concentrations in topmost sediments was probably related to the strict environmental policies at present.

Time Trends of Polybrominated Diphenyl Ethers (PBDEs) in Antarctic Biota.

Polybrominated diphenyl ethers (PBDEs) are “emerged” contaminants that were produced and used as flame retardants in numerous consumer and industrial applications for decades until banned. They remain ubiquitously present in the environment today. Here, a unique set of >200 biotic samples from the Antarctic was analyzed for PBDEs, including phytoplankton, krill, fish, and fur seal milk, spanning several sampling seasons over 14 years. PBDE-47 and -99 were the dominant congeners determined in all samples, constituting >60% of total PBDEs. A temporal trend was observed for ∑7PBDE concentrations in fur seal milk, where concentrations significantly increased (R2 = 0.57, p < 0.05) over time (2000–2014). Results for krill and phytoplankton also suggested increasing PBDE concentrations over time. Trends of PBDEs in fur seal milk of individual seals sampled 1 or more years apart showed no clear temporal trends. Overall, there was no indication of PBDEs decreasing in Antarctic biota yet, whereas numerous studies have reported decreasing trends in the northern hemisphere. Similar PBDE concentrations in perinatal versus nonperinatal milk implied the importance of local PBDE sources for bioaccumulation. These results indicate the need for continued assessment of contaminant trends, such as PBDEs, and their replacements, in Antarctica.

Multi-year air monitoring of legacy and current-use brominated flame retardants in an urban center in northeastern China

The occurrence and temporal trends of polybrominated diphenyl ethers (PBDEs) and non-PBDE brominated flame retardants (NBFRs) were investigated in an urban atmosphere of Northeast China in consecutive six years (2008–2013). Among all chemicals, BDE-209, l,2,5,6,9,10-hexabromocyclododecane (HBCD), and decabromodiphenylethane (DBDPE) were the three most dominant compounds. During the period, the levels of pentabromodiphenyl ethers in the gas-phase and octabromodiphenyl ethers in the particle-phase significantly decreased, while the levels of BDE-209 and NBFRs increased in either the gas-phase or particle-phase. Ambient temperature was the most significant variable that influenced the gas-phase and particle-phase concentrations of BFRs, followed by wind speed and relative humidity. A stronger temperature dependence of the atmospheric concentrations was found for lower mass BFRs. Gas-particle partitioning studies suggested PBDEs in the urban atmosphere of Northeast China were at steady-state. Steady-state equation can also well describe the partitioning behavior for NBFRs, suggesting that the atmospheric partitioning behaviors of NBFRs were similar to those of PBDEs.

Time trends of polybrominated diphenyl ethers in East China Seas: Response to the booming of PBDE pollution industry in China

The East China Seas (ECSs) are the receptors of the land-based persistent organic pollutants (POPs), such as polybrominated diphenyl ethers (PBDEs) mainly from China through atmospheric deposition driven by the East Asian winter monsoon and fluvial discharge (e.g., Yangtze River and Yellow River), making the offshore sediments to be a good proxy to reconstruct history of those pollutants in China. In this work, four well-placed sediment cores were extracted from the mud areas in the ECSs, and the 210Pb-dated cores were analyzed to yield historical concentration profiles of PBDEs in the area. The results showed that there was a persistent increase from 1970s and almost no clear sign in the decline of PBDEs until recently in China. More importantly, there was a faster increase of PBDEs from 1990s in China; while this period was just shown as gradually leveling off or even declining trends in developed countries. The persistently increasing trend of PBDEs in China since 1990s could be largely due to the booming of the manufacturing industry and unexpectedly transfer of PBDE pollution from developed countries to China. Besides, the relative high concentrations and fluxes of PBDEs in the core from coastal ECS located near a well-known electrical/electronic waste (e-waste) recycling area suggests an important contribution of PBDE emissions from recycling centers of e-waste in China. Although efforts in environmental monitoring of PBDE contamination have been substantially increased over the last decade, China is still lagging behind in terms of nationwide regulation of PBDE usage and treatment of disposal PBDE-containing products.

Trends of polybrominated diphenyl ethers and hexabromocyclododecane in eggs of Canadian Arctic seabirds reflect changing use patterns

Due to the substantial use and release of polybrominated diphenyl ether (PBDE) flame retardants in North America, PBDE concentrations in North American marine biota are among the highest in the world. In this study, we compared PBDE concentrations and congener patterns in eggs of five seabird species (thick-billed murres, northern fulmars, black guillemots, glaucous gulls, black-legged kittiwakes) breeding at a colony in the Canadian Arctic in 1993, 2008 and 2013. Temporal trends of PBDEs (1975–2014) and another flame retardant, hexabromocyclododecane (HBCD) (2003–2014), were also examined in eggs of two seabird species, the thick-billed murre and northern fulmar. BDE-47 generally dominated the BDE congener profiles in eggs of all five species. Glaucous gulls had the highest concentrations of both ΣPBDE and BDE-47, and northern fulmars, the lowest. ΣPBDE concentrations increased exponentially in eggs of both thick-billed murres and northern fulmars from 1975 to 2003 with doubling times of 9.1 years in the murres and 7.2 years in the fulmars. From 2003 to 2008/09, ΣPBDE decreased rapidly in the murres and fulmars to concentrations not significantly different from those recorded in 1975 and 1987 for each species. After 2008/09, ΣPBDE concentrations plateaued. BDE-47 followed a similar temporal trend to that of ΣPBDE concentrations. These concentration trends were consistent with the phase-out of the penta- and octa-BDE products from the North American market in the mid-2000s. There was an overall decline in concentrations of HBCD in murre eggs from 2003 to 2014, whereas concentrations in the fulmar eggs increased from 2003 to 2006 followed by a decline to 2014. The ratio of HBCD to BDE-47 suggests that northern fulmars showed more of a European contaminant signature, and thick-billed murres, more of a North American signature.

An overview of polybrominated diphenyl ethers (PBDEs) in the marine environment

Polybrominated diphenyl ethers (PBDEs), which are used extensively as brominated flame retardants, are found ubiquitously in marine environments worldwide. In this paper, we review all available data on the occurrence and trends of PBDEs in marine environments. PBDE levels in different marine environmental compartments vary from nanograms per gram to micrograms per gram, and differ widely, depending on the exposed species and the collection site. The PBDE congener profiles in biota, which are dominated by the lower brominated congeners, such as BDE-47 and BDE-99, are different from those in sediments, where BDE-209 is dominant. Temporal trends in PBDE levels in sediment cores vary considerably, depending on the region or country studied, with possible correlations with the historic and current use of PBDEs. Low brominated BDE congeners have the potential for bioaccumulation in marine organisms, but BDE- 209 has a very low potential for bioaccumulating within the marine food web. The toxicological effects of PBDEs on marine organisms are largely unknown. However, PBDE isomers may be sufficient to elicit adverse effects in some marine organisms. Here, we discuss naturally occurring brominated diphenyl ethers and recommend further research to improve future monitoring.

Polybrominated biphenyl ethers in breast milk and infant formula from Shanghai, China: Temporal trends, daily intake, and risk assessment

To investigate the temporal trend of polybrominated diphenyl ethers (PBDEs) in breast milk and assess the risks to breast- and formula-fed infants, breast milk and infant formula samples were collected from Shanghai, China. The PBDE concentrations decreased from 14.8 to 4.85pmol/g lipid weight during 2006–2012, with a rate of decrease by half approximately every four years. Although there were no significant correlations between the total PBDEs in breast milk and age, parity, and pre-pregnant BMI of mothers, there were significant differences between primiparous and multiparous mothers for tri- to hepta-BDEs. PBDEs in breast milk were much higher than those in infant formula (equivalent to 91.9 vs. 5.25pg/mL). Among the different brand infant formulas, there were no significant differences in their PBDE concentrations. The estimated daily intake of PBDEs by breast- and formula-fed infants suggested that breast-fed infants are exposed to much more PBDEs than formula-fed ones (12.9 vs. 0.72ng/kg-bw/day). However, the hazard quotient values were much smaller than one, indicating that the ingested PBDEs did not exert obvious adverse effects on both breast- and formula-fed infants considering non-carcinogenic effect endpoint. This is the first report on temporal trend of PBDEs in breast milk from China.

Dietary exposure and screening-level risk assessment of polybrominated diphenyl ethers (PBDEs) and dechloran plus (DP) in wheat, rice, soil and air along two tributaries of the River Chenab, Pakistan

No scientific report is available for screening level-risk assessment of newly emerging contaminants, including polybrominated diphenyl ethers (PBDEs) and dechloran plus (DP) in food crops and environmental compartments of Pakistan. Dietary exposure of PBDEs and DP via food crops; screening levels, spatial distribution pattern of PBDEs and DP in air, soil, wheat and rice were assessed along the stretch of upstream feeding tributaries (Nullah Aik and Nullah Palkhu), River Chenab, Pakistan. ∑PBDE levels in air, soil, wheat and rice ranged between 0.59 and 7.80pgm−3, 6.88 and 37.7ngg−1, 0.30ngg−1 and 1.43ngg−1 and 0.07 and 46.0ngg−1, respectively. ∑DP concentrations calculated in air, soil, wheat and rice ranged between 0.80 and 0.10pgm−3, 0.17 and 2.61ngg−1, 0.90 and 0.49ngg−1 and 0.00 and 12.5ngg−1, respectively. The trend of PBDEs and DP distribution pattern was found as follows; industrial/urban areas>industrial/peri-urban areas>agricultural/rural areas. Estimated daily intake (EDI) for wheat and rice was ranged between 0.002 and 0.035pgkg−1d−1 and 0.033 and 0.680pgkg−1d−1. Human health risks for adults on the basis of EDI were lower than the recommended MRL (minimal risk level) and lowest observed adverse effect of level (LOAEL).

Differences in the seasonal variation of brominated and phosphorus flame retardants in office dust

This study documents the temporal variability in concentrations of flame retardants (FRs) in floor dust from three offices in Beijing, China. Dust from Office A (OAD) was collected weekly from March to August, 2012, and sampling of dust from Office B and C (OBD and OCD) was conducted fortnightly (each two weeks) from March to December 2012. With intensive and continuous sampling, we report for the first time on clear and coherent temporal trends of polybrominated diphenyl ethers (PBDEs), novel brominated flame retardants (NBFRs) and phosphorus flame retardants (PFRs) in indoor dust. The observed mean concentrations of ∑9PBDEs, ∑4NBFRs and ∑9PFRs, were 554, 11,100 and 128,000ngg−1 in OAD; 7560, 5000 and 17,300ngg−1 in OBD; and 4750, 3550 and 17,200ngg−1 in OCD, respectively. With exception of PBDEs, concentrations of FRs were elevated in OAD than in OBD and OCD. Two to ten-fold variations were observed between the minimum and maximum concentrations of FRs in the same office, indicating that the sampling moment exerts a substantial influence on the level of FR contamination. Different seasonality was distinctively found between BFRs and PFRs. Except for a few occasional abnormal values, BFR levels in office dust were generally constant among different seasons. The abundance rank order for PFRs was: winter>autumn>summer, with peak values occurring in late winter and early spring. This pattern may be attributable to the fact that PFRs are more sensitive to temperature changes compared to PBDEs and NBFRs owning to their higher volatilities. The absence of significant seasonal variation for BFR concentrations in indoor dust compared to outdoor air and dust concentrations is also discussed.

Has the Phase-Out of PBDEs Affected Their Atmospheric Levels? Trends of PBDEs and Their Replacements in the Great Lakes Atmosphere

Air and precipitation samples were collected every 12 days at five sites near the North American Great Lakes from 2005 to 2011 (inclusive) by the Integrated Atmospheric Deposition Network (IADN). The concentrations of polybrominated diphenyl ethers (PBDEs) and selected alternative brominated flame retardants [pentabromoethyl benzene (PBEB), hexabromobenzene (HBB), 1,2-bis(2,4,6-tribromophenoxy)ethane (TBE or BTBPE), decabromodiphenylethane (DBDPE), 2-ethylhexyl-2,3,4,5-tetrabromobenzoate (TBB), and bis(2-ethylhexyl)-tetrabromo-phthalate (TBPH)] were measured in these samples. The concentrations of almost all of these flame retardants were related to the number of people within a 25 km radius of the sampling site, except for HBB, the concentrations of which were relatively high at Sturgeon Point, and PBEB, the concentrations of which were relatively high at Eagle Harbor. The temporal trends of all of these concentrations were variable. For example, BDE-47 vapor phase concentrations were increasing with doubling times of 5-10 years at Sturgeon Point, Sleeping Bear Dunes, and Eagle Harbor, but these concentrations were slowly decreasing in all phases at Chicago. The most consistent trend was for TBE, which showed concentrations that were unchanging or decreasing in all phases at all sites. TBPH concentrations in particles and HBB concentrations in precipitation were rapidly increasing at most sites with doubling times of ~2 years. The concentrations of DBDPE and BDE-209 were strongly and positively correlated, and the concentrations of TBB and TBPH were also strongly and positively correlated. The concentrations of TBB plus TBPH (representing Firemaster 550) and BDE-47, 85, 99, 100, 153, plus 154 (representing the withdrawn penta-BDE commercial mixture) were also strongly and positively correlated. These positive relationships indicate that the replacement of the deca-BDE commercial product by DBDPE and the penta-BDE product by Firemaster 550 have not yet become evident in the Great Lakes' atmospheric environment.

Polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecane (HBCD) in seven different marine bird species from Iceland

Data on distribution, concentration and trends of polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecanes (HBCDs) is scarce in biota from the sub-Arctic region of the Atlantic. The present study is an investigation on PBDE and HBCD concentrations in eggs from seven marine bird species from Iceland, i.e. common eider (Somateria mollissima), arctic tern (Sterna paradisaea), guillemot (Uria aalge), fulmar (Fulmarus glacialis), lesser black-backed gull (Larus fuscus), great black-backed gull (Larus marinus) and great skua (Stercorarius skua). Concentrations of sum PBDEs ranged from 44ngg−1fat in eider eggs to 2400ngg−1fat in great skua eggs. The contribution of different PBDE congeners to the sum concentration differed between species. Concentration of HBCDs (sum of α−,β− and γ−HBCD) ranged from 1.3ngg−1fat in arctic tern eggs to 41ngg−1fat in great black-backed gull. PCA on PBDE and HBCD shows different trends between the two BFR groups, further indicating different sources/usage. Investigations on any potential health or population effects of environmental pollutants on the great skua are advised since both the PBDE and HBCD concentrations are high.

Spatial distributions and temporal trends in polybrominated diphenyl ethers in Detroit River suspended sediments

Suspended sediments from the Detroit River were collected using sediment traps at sites ranging from western Lake Erie to southern Lake St. Clair to assess spatial distributions and temporal trends of polybrominated diphenyl ethers (PBDEs). The distribution of PBDEs in suspended sediments in the Detroit River appeared influenced by shoreline-based contemporary urban and industrial activities, which stood in contrast to PCBs that were associated with areas of historic industrial activity. Temporal trend data indicate that total PBDE concentrations decreased in the period after 2000 in response to cessation of production of the penta- and octa BDE formulations. Concentrations of total PBDEs ranged from roughly 7ngg−1 (4ngg−1 BDE 209) in southern Lake St. Clair to several hundred ngg−1 (60–180ngg−1 BDE 209) in the lower reaches of the Detroit River. The widespread occurrence of PBDEs in Detroit River suspended sediments suggests that large urban areas can act as diffuse sources of these chemicals that are used in modern industrial applications and consumer products.

Distribution and temporal trend of polybrominated diphenyl ethers in one Shanghai municipal landfill, China

The scarcity of information on polybrominated diphenyl ethers' (PBDEs) flow in landfill restricts the life cycle analysis of PBDEs. In this study, eight PBDE congeners (BDEs 28, 47, 99, 100, 153, 154, 183, and 209) in topsoil, vegetation leaves, leachate, and municipal aged refuse collected from Shanghai Laogang Municipal Landfill (SLML) were investigated. The present study revealed elevated PBDE concentrations in topsoil and proved PBDE leakage from SLML and vegetation uptake. BDE-209 was the predominant congener, and this could be due to massive usage of deca-BDE mixture in Shanghai. ΣPBDE concentrations in leachates treated by reed wetland and A(2)/O process fell in the low end of the worldwide range. ΣPBDE concentrations in aged refuse samples rose from under 50 ng/g dw in 1989 to the range of 5,150-5,718 ng/g dw in 2002. PBDE concentrations increase in aged refuse samples throughout the 1990s into the 2000s paralleled municipal solid waste output from 1991 to 2002 in Shanghai. Exponential increase in BDE-209 concentration in aged refuse suggested the increasing market demands for deca-BDE mixture after 1990 in China. Notably, the inventory of PBDEs in SLML was 28.7 MT, and the doubling time of BDE-209 in aged refuse was calculated to be 1.6 year. SLML can be considered as a source of PBDE and one main recipient of PBDE as well, receiving inputs predominantly from the PBDE-containing waste. Priority should be given to formulate regulation on PBDEs and sorting work before landfill disposal.

Spatial trends of polybrominated diphenyl ethers in Canadian fish and implications for long‐term monitoring

A nationwide study was conducted to examine concentrations of polybrominated diphenyl ethers (PBDEs) in top predatory fish, with a focus on lake trout (Salvelinus namaycush), across Canada, and to explore possible influences of food web processes. Concentrations of the three most abundant PBDE homolog groups (tetra-, penta-, and hexa-PBDEs) were, for the most part, higher in Great Lakes and Lake Champlain fish compared with fish from other systems. The Canadian Federal Environmental Quality Guideline for the penta-homolog was exceeded in 70% of the fish examined. However, virtually no guideline exceedances were found for other congeners. In general, PBDE-47 (a representative lower brominated congener) was significantly and positively correlated with fish length, weight, age, lipid content, and stable isotopes of nitrogen and carbon. Significant differences in the slopes of the PBDE-47/covariate relationships between sites prevented concentrations from being adjusted using an analysis of covariance (ANCOVA). However, plots showed that elevated concentrations of PBDE-47 in Great Lakes and Lake Champlain fish remained after accounting for the influence of covariates. In contrast, for PBDE-183 (a representative higher brominated congener), the relationships between fish concentrations and covariates were not consistent, which could be a result of biotransformation being more important in controlling its bioaccumulation. The data from the current study show an overall disconnect between fish PBDE concentrations and likely loadings, which may be caused by differences in food web processes between systems. Continued long-term fish contaminant monitoring is needed to evaluate potential risk to fish and their consumers. However, we also recommend sediment sampling and focused food web studies to provide information on PBDE inputs to the systems and mechanisms of biomagnification, respectively.

Temporal trends of polybrominated diphenyl ethers and hexabromocyclododecane in Swedish Peregrine Falcon (Falco peregrinus peregrinus) eggs

A temporal trend study of brominated flame retardants in eggs from peregrine falcon ( Falco peregrinus peregrinus), a terrestrial bird of prey, is presented. Eggs collected between 1974 and 2007 were analyzed for the major constituents of the Penta-, Octa- and Decabromodiphenyl ether technical products (BDE-47, -99, -100, -153, -183 and -209), and hexabromocyclododecane (HBCD). Concentrations of BDE-99, -100, -153, -183, -209 and HBCD increased from 1974 to 2000. After the early 2000s, BDE-99, -100, -153 and -183 concentrations decreased, whereas BDE-209 and HBCD concentrations continued to increase. No temporal trend was detected for BDE-47. Rates of increase also differed, with BDE-99 and -100 increasing 3-fold between the 1980s and mid-1990s, and BDE-153 and -183 increasing approximately 10-fold during the same period. The average yearly increase was 15% and 11% for BDE-209 and HBCD, respectively, based on log-linear regression trends. There is a change in BDE congener patterns over time, with a shift from the predominance of BDE-99 and -47 until the late 1980s, to BDE-153 becoming the predominant congener later on. BFR temporal trends in Swedish peregrine falcon eggs reflect European BFR usage patterns.