Of the 13, current-use, non-polybrominated diphenyl ether (PBDE) flame retardants (FRs) monitored, hexabromobenzene (HBB), pentabromoethylbenzene (PBEB), pentabromotoluene (PBT), 1,2-bis(2,4,6-tribromophenoxy)ethane (BTBPE) and alpha- and gamma-isomers of hexabromocyclododecane (HBCD), and the syn- and anti-isomers of the chlorinated Dechlorane Plus (DP) were quantified in egg pools of herring gulls (Larus argentatus) collected in 2004 from six sites in all five of the Laurentian Great Lakes of North America. alpha-HBCD concentrations ranged from 2.1 to 20 ng/g (wet weight (ww)). Other "new" FR levels ranged from 0.004 to 1.4 ng/g ww and were much lower than those of the major BDE congeners that are in technical mixtures (namely BDE-47, -99, -100), where sigma3PBDE ranged from 186 to 498 ng/g ww. Nineteen hepta-BDEs (sigma(hepta) = 4.9-11 ng/g ww), octa-BDEs (alpha(octa) = 2.6-9.1 ng/g ww), and nona-BDEs (sigma(nona) = 0.12-5.6 ng/g ww) were detectible at all six colonies, while BDE-209 was low but quantifiable (< 0.1-0.21 ng/g ww) at two colonies. sigma-DP (syn- and anti-isomers) concentrations in eggs from all sites ranged from 1.5 to 4.5 ng/g ww. Our findings indicate that mother herring gulls are exposed to several, current-use flame retardants via their diet, and in ovo transfer occurred to their eggs. Given the aquatic diet of herring gull, this suggests that there are non-PBDE BFRs present in the gull-associated aquatic food web of the Great Lakes.
The production and use of nonpolybrominated diphenyl ether (non-PBDE), brominated flame retardant (BFR) alternatives have been on the rise, although their assessment in environmental samples is largely understudied. In the present study, several non-PBDE BFRs were found in the egg pools of herring gulls (Larus argentatus) from seven colonies in the five Laurentian Great Lakes (collected in 1982 to 2006). Of the 19 BFRs monitored, hexabromobenzene (HBB), 1,2-bis(2,4,6-tribromophe-noxy)ethane (BTBPE), decabromodiphenyl ethane (DBDPE), and alpha-, beta-, gamma-, and delta-isomers of 1,2-dibromo-4-(1,2-dibromoeth-yl)cyclohexane (TBECH) were present in eggs from all the colonies with the highest detection frequencies of 100%, 54%, 9% and 97%, respectively. In 2005 and 2006 eggs, the concentrations of DBDPE were highest at three of the seven colonies (1.3 to 288 ng/g wet weight (ww)) and surpassed decabromodiphenyl ether (BDE-209). HBB (0.10 to 3.92 ng/g ww), BTBPE (1.82 to 0.06 ng/g ww), and Sigma-TBECH (0.04 to 3.44 ng/g ww; mainly the beta-isomer 52 to 100% of Sigma-TBECH) were detected at lower concentrations (and generally <
Tris(1-chloro-2-propyl) phosphate (TCPP) and tris(1,3-dichloro-2-propyl) phosphate (TDCPP) are organic flame retardants detected in the environment and biota for which avian toxicological data are limited. In this study, domestic chicken eggs were injected with TCPP or TDCPP (maximum dose = 51,600 and 45,000ng/g egg, respectively) to determine dose-dependent effects on pipping success, development, hepatic messenger RNA (mRNA) expression levels of genes associated with xenobiotic metabolism and the thyroid hormone (TH) pathway, and TH levels following 20-22 days of incubation. Neither compound reduced pipping success; however, TCPP significantly delayed pipping at 9240 and 51,600ng/g and reduced tarsus length at 51,600ng/g. TDCPP exposure resulted in significant decreases in head plus bill length, embryo mass, and gallbladder size at 45,000ng/g and reduced plasma free T4 levels at 7640ng/g. Type I deiodinase, liver fatty acid-binding protein, and cytochrome P450 (CYP) 3A37 mRNA levels were significantly induced by TCPP, whereas TDCPP induced CYP3A37 and CYP2H1. Chemical analysis of egg contents at incubation days 0, 5, 11, 18, and 19 revealed that > 92% of the injected TCPP or TDCPP concentration was detectable up to day 5; however, < 1% was detected by day 19. The observed phenotypic responses to TCPP and TDCPP exposure may be associated with disruption of the TH axis, which is critical for normal growth and development in birds. The effects of TDCPP on the gallbladder indicate that the disturbance of lipid metabolism is a likely mechanism of toxicity.
DecaBDE is a current-use, commercial formulation of an additive, polybrominated diphenyl ether (PBDE) flame retardant composed of > 97% 2,2',3,3',4,4',5,5',6,6'-decabromoDE (BDE-209). Of the 43 PBDE congeners monitored, we report on the temporal trends (1982-2006) of quantifiable PBDEs, and specifically BDE-209, in pooled samples of herring gull (Larus argentatus) eggs from seven colonies spanning the Laurentian Great Lakes. BDE-209 concentrations in 2006 egg pools ranged from 4.5 to 20 ng/g wet weight (ww) and constituted 0.6-4.5% of sigma39PBDE concentrations among colonies, whereas sigma(octa)BDE and sigma(nona)BDE concentrations constituted from 0.5 to 2.2% and 0.3 to 1.1%, respectively. From 1982 to 2006, the BDE-209 doubling times ranged from 2.1 to 3.0 years, whereas for sigma(octa)BDEs and sigma(nona)BDEs, the mean doubling times ranged from 3.0 to 11 years and 2.4 to 5.3 years, respectively. The source of the octa- and nona-BDE congeners, e.g., BDE-207 and BDE-197, are the result of BDE-209 debromination, and they are either formed metabolically in Great Lakes herring gulls and/or bioaccumulated from the diet and subsequently transferred to their eggs. In contrast to BDE-209 and the octa- and nona-BDEs, congeners derived mainly from PentaBDE and OctaBDE mixtures, e.g., BDE-47, -99, and -100, showed rapid increases up until 2000; however, there was no increasing trend post-2000. The data illustrates that PBDE concentrations and congener pattern trends in the Great Lakes herring gull eggs have dramatically changed between 1995 and 2006. Regardless of BDE-209 not fitting the pervasive criteria as a persistent and bioaccumulative substance, it is clearly of increasing concern in Great Lake herring gulls, and provides evidence that regulation of DecaBDE formulations is warranted.
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