Polybrominated Diphenyl Ether Flame Retardants in the U.S. Population: Current Levels, Temporal Trends, and Comparison With Dioxins, Dibenzofurans, and Polychlorinated Biphenyls

Brominated flame retardants have come into common use in the United States during the past 3 decades. This study reports levels of polybrominated diphenyl ether (PBDE) flame retardants in blood from the U.S. population at the present time and 30 years previously and also current human milk levels. This is also the first study to report measured congeners and dioxin toxic equivalents (TEQs) of dioxins, dibenzofurans, and dioxin-like polychlorinated biphenyls (PCBs) from archived, 1973, blood and compare them with current levels. The findings indicate there have been significant changes in levels of each class of these persistent organic pollutants (POPs) in U.S. human blood. Although dioxin, dibenzofuran, and PCB levels are markedly higher in the 1973 blood, the opposite is true for PBDEs. Furthermore, unlike dioxins, dibenzofurans, and PCBs, which increase with age, there was no significant correlation found in our study between PBDE levels and age. Current total PBDE levels in U.S. blood are the highest reported worldwide to date, with 2 pooled samples (N = 100 each) measuring 61.7 and 79.7 parts per billion (ppb) lipid, and in a series of 39 individual analyses, the range was 4.6 to 365.5 ppb with a median of 29 ppb and a mean of 52.6 ppb. The median for women in this study was 43.3 ppb, and for men it was 25.1 ppb. Although women have a higher level of PBDEs in blood than men, in our study, this is not statistically significant. Blood levels are similar to levels in U.S. human milk from 59 women, 6.2 to 418.8 ppb lipid. Levels of PBDE in pooled 2003 serum are far higher at 61.7 ppb than in 1973 archived pooled serum in which almost no PBDEs were quantified, although the estimated level using half the detection limit for nondetects was 0.77 ppb. Although no human health studies have been conducted on PBDEs, they are of concern because in vivo and in vitro animal studies show nervous system, reproductive, developmental, and endocrine effects, as well as cancer in high-dose studies.

[1]  P. B. Larsen,et al.  Polybrominated diphenyl ethers: occurrence, dietary exposure, and toxicology. , 2001, Environmental health perspectives.

[2]  J. Startin,et al.  Dioxins in Food , 1994 .

[3]  Eva Jakobsson,et al.  Flame retardant exposure: polybrominated diphenyl ethers in blood from Swedish workers. , 1999 .

[4]  Linda S. Birnbaum,et al.  Polybrominated diphenyl ethers contamination of United States food. , 2004 .

[5]  G. O. Thomas,et al.  Polybrominated diphenyl ethers (PBDEs) in grey seals during their first year of life--are they thyroid hormone endocrine disrupters? , 2003, Environmental pollution.

[6]  W. Sonzogni,et al.  Comparison of polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs) in Lake Michigan salmonids. , 2001, Environmental science & technology.

[7]  K. Norén,et al.  Certain organochlorine and organobromine contaminants in Swedish human milk in perspective of past 20-30 years. , 2000, Chemosphere.

[8]  Ronald A Hites,et al.  Polybrominated diphenyl ethers in the environment and in people: a meta-analysis of concentrations. , 2004, Environmental science & technology.

[9]  K. Hooper,et al.  Lessons from the polybrominated diphenyl ethers (PBDEs): precautionary principle, primary prevention, and the value of community-based body-burden monitoring using breast milk. , 2002, Environmental health perspectives.

[10]  J. Jacobson,et al.  Prenatal exposure to polychlorinated biphenyls: effects on birth size and gestational age. , 1984, The Journal of pediatrics.

[11]  L. Birnbaum,et al.  Brominated flame retardants: cause for concern? , 2003, Environmental health perspectives.

[12]  Jean-François Focant,et al.  Retrospective time-trend study of polybrominated diphenyl ether and polybrominated and polychlorinated biphenyl levels in human serum from the United States. , 2004, Environmental health perspectives.

[13]  Safe,et al.  Toxic equivalency factors (TEFs) for PCBs, PCDDs, PCDFs for humans and wildlife. , 1998, Environmental health perspectives.

[14]  R C Hale,et al.  Polybrominated diphenyl ether flame retardants in Virginia freshwater fishes (USA). , 2001, Environmental science & technology.

[15]  Ǻ. Bergman,et al.  An overview of commercially used brominated flame retardants, their applications, their use patterns in different countries/regions and possible modes of release. , 2003, Environment international.

[16]  Teruyuki Nakao,et al.  Comparison of polybrominated diphenyl ethers in fish, vegetables, and meats and levels in human milk of nursing women in Japan. , 2002, Chemosphere.

[17]  Enrico Alleva,et al.  Effects of perinatal exposure to a polybrominated diphenyl ether (PBDE 99) on mouse neurobehavioural development. , 2002, Neurotoxicology.

[18]  Nathan G Dodder,et al.  Polybrominated diphenyl ethers in maternal and fetal blood samples. , 2003, Environmental health perspectives.

[19]  Arnold Schecter,et al.  Polybrominated diphenyl ethers (PBDEs) in U.S. mothers' milk. , 2003, Environmental health perspectives.

[20]  O. Päpke,et al.  PCDD/PCDF: human background data for Germany, a 10-year experience. , 1998, Environmental health perspectives.

[21]  Kellyn S Betts,et al.  Rapidly rising PBDE levels in North America. , 2002, Environmental science & technology.

[22]  J. J. Ryan,et al.  Recent trends in levels of brominated diphenyl ethers (BDES) in human milks from Canada , 2002 .

[23]  Anders Fredriksson,et al.  Neonatal exposure to the brominated flame-retardant, 2,2',4,4',5-pentabromodiphenyl ether, decreases cholinergic nicotinic receptors in hippocampus and affects spontaneous behaviour in the adult mouse. , 2004, Environmental toxicology and pharmacology.

[24]  A. Schecter,et al.  Dioxin levels in milk and blood from germany and the USA. Are dioxin blood levels decreasing in both countries , 2000 .

[25]  K. Hemminki,et al.  Cancer risk of air pollution: epidemiological evidence. , 1994, Environmental health perspectives.

[26]  D. Helm,et al.  The german environmental specimen bank : Application in trend monitoring of polybrominated diphenyl ethers in human blood , 2000 .

[27]  A. Bergman,et al.  Brominated flame retardants in serum from U.S. blood donors. , 2001, Environmental science & technology.

[28]  J. Sunyer,et al.  Levels of hexachlorobenzene and other organochlorine compounds in cord blood: exposure across placenta. , 2001, Chemosphere.

[29]  D. Smith,et al.  Worldwide trends in DDT levels in human breast milk. , 1999, International journal of epidemiology.

[30]  Åke Bergman,et al.  Brominated flame retardants in serum from us blood donors , 2000 .

[31]  P. Fürst,et al.  Human milk as a bioindicator for body burden of PCDDs, PCDFs, organochlorine pesticides, and PCBs. , 1994, Environmental health perspectives.

[32]  E. Jakobsson,et al.  A brominated flame retardant, 2,2',4,4',5-pentabromodiphenyl ether: uptake, retention, and induction of neurobehavioral alterations in mice during a critical phase of neonatal brain development. , 2002, Toxicological sciences : an official journal of the Society of Toxicology.

[33]  I. Meerts,et al.  In vitro estrogenicity of polybrominated diphenyl ethers, hydroxylated PDBEs, and polybrominated bisphenol A compounds. , 2001, Environmental health perspectives.

[34]  Nathan G Dodder,et al.  Concentrations and spatial variations of polybrominated diphenyl ethers and several organochlorine compounds in fishes from the northeastern United States. , 2002, Environmental science & technology.

[35]  T. Visser,et al.  Interference of polychlorinated biphenyls in hepatic and brain thyroid hormone metabolism in fetal and neonatal rats. , 1993, Toxicology and applied pharmacology.

[36]  Y. L. Guo,et al.  Early development of Yu-Cheng children born seven to twelve years after the Taiwan PCB outbreak. , 1994, Chemosphere.

[37]  P. Taylor,et al.  Polychlorinated biphenyls: influence on birthweight and gestation. , 1984, American journal of public health.

[38]  Chris Halliwell,et al.  Preliminary assessment of U.K. human dietary and inhalation exposure to polybrominated diphenyl ethers. , 2004, Environmental science & technology.

[39]  J. Spengler,et al.  Phthalates, alkylphenols, pesticides, polybrominated diphenyl ethers, and other endocrine-disrupting compounds in indoor air and dust. , 2003, Environmental science & technology.

[40]  T. Vartiainen,et al.  Market basket study on dietary intake of PCDD/Fs, PCBs, and PBDEs in Finland. , 2004, Environment international.

[41]  Abraham Brouwer,et al.  Placental transfer of a hydroxylated polychlorinated biphenyl and effects on fetal and maternal thyroid hormone homeostasis in the rat. , 2002, Toxicological sciences : an official journal of the Society of Toxicology.

[42]  Peter Fürst,et al.  Human milk as a bioindicator for body burden of PCDDs, PCDFs, organochlorine pesticides, and PCBs. , 1994 .

[43]  J. Domingo,et al.  Polybrominated diphenyl ethers (PBDEs) in foodstuffs: human exposure through the diet. , 2003, Journal of agricultural and food chemistry.

[44]  L. Hagmar,et al.  Lowered birth weight among infants born to women with a high intake of fish contaminated with persistent organochlorine compounds. , 2000, Chemosphere.

[45]  P. Fürst,et al.  Determination of polybrominated diphenylethers (PBDEs) in biological tissues with special emphasis on QC/QA measures. , 2004, Talanta.

[46]  P. Darnerud,et al.  Polybrominated diphenyl ethers (PBDEs), polychlorinated biphenyls (PCBs) and chlorinated paraffins (CPs) in rats-testing interactions and mechanisms for thyroid hormone effects. , 2002, Toxicology.

[47]  L. Hagmar,et al.  Flame retardant exposure: polybrominated diphenyl ethers in blood from Swedish workers. , 1999, Environmental health perspectives.

[48]  A. Schecter Dioxins and Health , 2003, Springer US.

[49]  Rajiv Bhatia,et al.  High body burdens of 2,2',4,4'-tetrabromodiphenyl ether (BDE-47) in California women. , 2003, Environmental health perspectives.

[50]  oseph,et al.  INTELLECTUAL IMPAIRMENT IN CHILDREN EXPOSED TO POLYCHLORINATED BIPHENYLS IN UTERO , 2000 .

[51]  Marie Aune,et al.  Polybrominated diphenyl ethers in breast milk from Uppsala County, Sweden. , 2003, Environmental research.

[52]  L S Birnbaum,et al.  Toxicokinetics of BDE 47 in female mice: effect of dose, route of exposure, and time. , 2004, Toxicological sciences : an official journal of the Society of Toxicology.

[53]  A. Brouwer,et al.  Determination of the endocrine disrupting potency of hydroxylated PCB's and flame retardants with in vitro bioassays , 2002 .

[54]  Ǻ. Bergman,et al.  Human prenatal and postnatal exposure to polybrominated diphenyl ethers, polychlorinated biphenyls, polychlorobiphenylols, and pentachlorophenol. , 2003, Environmental health perspectives.

[55]  G. Solomon,et al.  Chemical contaminants in breast milk: time trends and regional variability. , 2002, Environmental health perspectives.

[56]  Enrico Alleva,et al.  Polybrominated diphenyl ethers: neurobehavioral effects following developmental exposure. , 2003, Neurotoxicology.

[57]  D. Carpenter,et al.  Global assessment of polybrominated diphenyl ethers in farmed and wild salmon. , 2004 .

[58]  NTP Toxicology and Carcinogenesis Studies of Decabromodiphenyl Oxide (CAS No. 1163-19-5) In F344/N Rats and B6C3F1 Mice (Feed Studies). , 1986, National Toxicology Program technical report series.

[59]  D. Haines,et al.  Twenty-Five Years of Surveillance for Contaminants in Human Breast Milk , 1998, Archives of environmental contamination and toxicology.