An analytical method comprised of automated solid-phase extraction and determination using gas chromatography mass spectrometry (single quadrupole) has been developed for the determination of 12 polybrominated diphenyl ethers (PBDEs), 26 polychlorinated biphenyls (PCBs), two organochlorine compounds (OCs) (hexachlorobenzene and octachlorostyrene) and two brominated phenols (pentabromophenol, and tetrabromobisphenol-A (TBBP-A)). The analytes were extracted using a sorbent of polystyrene-divinylbenzene and an additional clean-up was performed on a sulphuric acid-silica column to remove lipids. The method has been validated by spiking horse serum at five levels. The mean accuracy given as recovery relative to internal standards was 95%, 99%, 93% and 109% for the PBDEs PCBs, OCs and brominated phenols, respectively. The mean repeatability given as RSDs was respectively 6.9%, 8.7%, 7.5% and 15%. Estimated limits of detection (S/N=3) were in the range 0.2-1.8 pg/g serum for the PBDEs and phenols, and from 0.1 pg/g to 56 pg/g serum for the PCBs and OCs. The validated method has been used to investigate the levels of PBDEs and PCBs in 21 pooled serum samples from the general Norwegian population. In serum from men (age 40-50 years) the sum of seven PBDE congeners (IUPAC No. 28, 47, 99, 100, 153, 154 and 183) increased from 1977 (0.5 ng/g lipids) to 1998 (4.8 ng/g lipids). From 1999 to 2003 the concentration of PBDEs seems to have stabilised. On the other hand, the sum of five PCBs (IUPAC No. 101, 118, 138, 153 and 180) in these samples decreased steadily from 1977 (666 ng/g lipids) to 2003 (176 ng/g lipids). Tetrabromobisphenol-A and BDE-209 were detected in almost all samples, but no similar temporal trends to that seen for the PBDEs were observed for these compounds, which might be due to the short half-lives of these brominated flame retardants (FR) in humans.
In recent years, the relatively high levels of organochlorine contaminants and increasing levels of brominated flame retardants found in tissues of marine mammals have raised concerns that exposure to these marine pollutants may compromise individual health. In this pilot study, levels of 11 polychlorinated biphenyls, 3 polybrominated diphenyl ethers, and the DDT metabolite p,p'-diphenyldichloroethylene were analyzed in whole blood of 7 free-ranging spotted seals (Phoca largha) from Bristol Bay, Alaska, sampled during 2000 and 2001. Blood concentrations of analytes were generally low (
Exposure to persistent organic pollutants (POPs) during prenatal and postnatal life has been extensively studied in relation to adverse health effects in children.
The aim was to identify determinants of the concentrations of polychlorinated biphenyls (PCBs), brominated flame retardants (polybrominated diphenyl ethers, PBDEs; polybrominated biphenyl, PBB), and organochlorine pesticides (OCPs) in blood samples from pregnant women and children in The Norwegian Mother and Child Cohort Study (MoBa).
Blood samples were collected from two independent subsamples within MoBa; a group of women (n=96) enrolled in mid-pregnancy during the years 2002-2008 and a group of 3 year old children (n=99) participating during 2010-2011. PCB congeners (74, 99, 138, 153, 180, 170, 194, 209, 105, 114, 118, 156, 157, 167, and 189), brominated flame retardants (PBDE-28, 47, 99, 100, 153, 154, and PBB-153), as well as the OCPs hexachlorobenzene (HCB), oxychlordane, 4,4'dichlorodiphenyltrichloroethane (DDT), and 4,4'dichlorodiphenyldichloroethylene (DDE) were measured in both pregnant women and children.
Age, low parity, and low pre-pregnant BMI were the most important determinants of increased plasma concentrations of POPs in pregnant women. In 3 year old children, prolonged breastfeeding duration was a major determinant of increased POP concentrations. Estimated dietary exposure to PCBs during pregnancy was positively associated with plasma concentrations in 3 year old children, but not in pregnant women. Plasma concentrations were approximately 40% higher in children compared to pregnant women.
Several factors associated with exposure and toxicokinetics, i.e. accumulation, excretion and transfer via breastmilk of POPs were the main predictors of POP levels in pregnant women and children. Diet, which is the main exposure source for these compounds in the general population, was found to predict PCB levels only among children. For the PBDEs, for which non-dietary sources are more important, toxicokinetic factors appeared to have less predictive impact.
Lack of human exposure data is frequently reported as a critical gap in risk assessments of environmental pollutants, especially regarding "new" pollutants. The objectives of this study were to assess serum levels of the persistent 2,2',4,4',5,5'-hexachlorobiphenyl (CB-153), hydroxylated polychlorinated biphenyl metabolites (OH-PCBs), polybrominated diphenyl ethers (PBDEs), and hexabromocyclodode-canes (HBCDDs) in a group of Swedish middle-aged and elderly women expected to be relatively highly exposed, and to evaluate the impact of potential determinants (e.g., fish intake, age) for the inter-individual variation, as well as to investigate the association between these pollutants and bone density. No associations were found between bone mineral density or biochemical markers of bone metabolism and the analyzed environmental pollutants. Relatively high levels of CB-153 (median 260 ng/g fat) and sigma 3-OH-PCBs (median 1.7 ng/mL serum), and low concentrations of sigma6PBDEs (median 3.6 ng/g fat) were determined. Total level of HBCDDs in serum was quantified by gas chromatography with mass spectrometric detection (median 0.5 ng/g fat). HBCDD diastereomeric and enantiomeric patterns were determined by liquid chromatography with mass spectrometric detection. The dominating stereoisomer was (-)alpha-HBCDD, but 1-3% of gamma-HBCDD was also detected in the serum samples.
Commercial decabromodiphenyl ether (DecaBDE) is commonly used as a flame retardant in different electrical and textile applications. It is also used in the production of flame-retarded rubber compound. DecaBDE is the major technical polybrominated diphenyl ether (PBDE) in use today and consists mainly of decabromodiphenyl ether (BDE-209). PBDEs, including BDE-209, are well-known environmental pollutants, ubiquitous both in aquatic and terrestrial environments. The aim of the present study was to assess the exposure to PBDEs in workers manufacturing or handling rubber which was flame retarded with DecaBDE. A referent group, abattoir workers (slaughterhouse workers), with no occupational exposure to PBDEs, was also investigated. Moreover, the methodology for analysis of PBDEs in serum was refined, with special emphasis on congeners with a high number of bromine substituents, i.e., octa- to decaBDEs. The highest BDE-209 concentration observed among the rubber workers was 280 pmol/g lipid weight (I.w.) (270 ng/g I.w.). The median concentration of BDE-209 among rubber workers was 37 pmol/g I.w. (35 ng/g I.w.). Among referents, the median was 2.5 (range 0.92-9.7) pmol/g I.w. (median 2.4 ng/g I.w.). In rubber workers the BDE-209 concentrations were up to 32% (median 4%) of the 2,2',4,4',5,5'-chlorobiphenyl (CB-153) concentrations, on a molar basis, whereas the referents had BDE-209 concentrations which were similar to that of 2,2',4,4'-bromodiphenyl ether (BDE-47), below 1.4% (median 0.3%) of the CB-153 concentration. Concentrations of all nonabromodiphenyl ethers (nonaBDEs) and several octabrmodiphenyl ethers (octaBDEs) congeners, including BDE-203, were also elevated among the rubber workers, with 2.5- to 11-fold higher median concentrations, compared to the referents. The results confirm a significant uptake of BDE-209 in the workers exposed to DecaBDE and indicate a potential for in vivo formation of lower BDEs in these persons.
Blood serum from 154 volunteers at 13 UK locations in 2003 were analysed for a range of PCBs, organochlorine pesticides and PBDEs. HCB, p,p'-DDE and p,p'-DDT and beta-HCH were the dominant organochlorine pesticides in most samples. BDEs 47, 99, 100, 153, 154 and 183 were the most regularly detected PBDEs. This study is the first report of BDE209 in UK human blood (found in 11 samples, range
Brominated flame retardants, especially polybrominated diphenyl ethers (PBDEs), have been widely used in North America, but little is known about the level of exposure of human populations to these compounds.
We set out to assess the internal exposure of postmenopausal Canadian women to selected organobromine compounds and to investigate factors associated with this exposure.
We measured concentrations of four PBDEs, one polybrominated biphenyl, and for comparative purposes, 41 polychlorinated biphenyl (PCB) congeners in plasma samples from 110 healthy postmenopausal women who were recruited at a mammography clinic in 2003-2004.
PBDE-47 was the major PBDE congener, with a mean (geometric) concentration of 8.1 ng/g lipids and extreme values reaching 1,780 ng/g. By comparison, the mean concentration of the major PCB congener (PCB-153) was 41.7 ng/g and the highest value was 177 ng/g. PBDEs 47, 99, and 100 were strongly intercorrelated, but weaker correlations were noted with PBDE-153. As the sum of PBDEs (summation operatorPBDEs) increased, the relative contribution of PBDE-47 to the summation operatorPBDEs increased, whereas that of PBDE-153 decreased. PBDE-153 was the only brominated compound correlated to PCB-153. PBDE levels were not linked to any sociodemographic, anthropometric, reproductive, or lifestyle variables documented in the present study. Age and body mass index gain since the age of 18 years were significant predictors of PCB-153 plasma levels.
Our results suggest that exposure to PBDE-47 likely occurs through direct contact with the penta-PBDE formulation, whereas exposure to PBDE-153 may originate in part from the food chain.
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