Children show highest levels of polybrominated diphenyl ethers in a California family of four: a case study

Polybrominated diphenyl ethers (PBDEs), a major class of flame retardants, are ubiquitous environmental contaminants with particularly high concentrations in humans from the United States. This study is a first attempt to report and compare PBDE concentrations in blood drawn from a family. Serum samples from family members collected at two sampling occasions 90 days apart were analyzed for PBDE congeners. Concentrations of the lower-brominated PBDEs were similar at the two sampling times for each family member, with children's levels 2- to 5-fold higher than those of their parents. Concentrations of, for example, 2,2',4,4'-tetrabromodiphenyl ether (BDE-47) varied from 32 ng/g lipid weight (lw) in the father to 60, 137, and 245 ng/g lw in the mother, child, and toddler, respectively. Decabromodiphenyl ether (BDE-209) concentrations differed significantly between the two samplings. September concentrations in the father, mother, child, and toddler were 23, 14, 143, and 233 ng/g lw, respectively. December concentrations (duplicate results from the laboratory) were 2 and 3, 4 and 4, 9 and 12, and 19 and 26 ng/g lw, respectively. Parents' summation operatorPBDE concentrations approached U.S. median concentrations, with children's concentrations near the maximum (top 5%) found in U.S. adults. The youngest child had the highest concentrations of all PBDE congeners, suggesting that younger children are more exposed to PBDEs than are adults. Our estimates indicate that house dust contributes to children's higher PBDE levels. BDE-209 levels for all family members were 10-fold lower at the second sampling. The short half-life of BDE-209 (15 days) indicates that BDE-209 levels can decrease rapidly in response to decreased exposures. This case study suggests that children are at higher risk for PBDE exposures and, accordingly, face higher risks of PBDE-related health effects than adults.     

Polybrominated diphenyl ethers in Swedish human liver and adipose tissue

Paired samples of human liver and adipose tissue were analyzed for polybrominated diphenyl ethers (PBDEs) containing 3–6 bromine atoms. The samples were obtained at autopsy from one woman and four men at the age of 47 and 66–83 years, respectively. PBDEs were found in all samples. The sum of nine PBDE congeners ranged 5–18 ng/g lipids and 4–8 ng/g lipids in liver and adipose tissue, respectively. In three paired samples the concentrations were similar in liver and adipose tissue, while in two of the pairs the concentrations were higher in liver than in adipose tissue. The PBDE congeners 2,2′,4,4′-tetraBDE (BDE-47), 2,2′,4,4′,5-pentaBDE (BDE-99), and 2,2′,4,4′,5,5′-hexaBDE (BDE-153) occurred at highest levels and constituted together 87–96% and 84–94% of the total sum of PBDEs in liver and adipose tissue, respectively. The levels of PBDEs were compared to those of polychlorinated biphenyls (PCBs), polychlorinated naphthalenes (PCNs), 1,1-bis(4-chlorophenyl)-2,2-dichloroethene (p,p′-DDE), and hexachlorobenzene (HCB). Received: 13 June 2000/Accepted: 1 October 2000     

Distribution of organobrominated and organochlorinated contaminants in Belgian human adipose tissue

We have measured the levels of flame retardants, polybrominated diphenyl ethers (PBDEs), in 20 recent human adipose tissues from Belgium and compared them to other organohalogen compounds such as polychlorinated biphenyls (PCBs), hexachlorobenzene, 2,2-bis(4-chlorophenyl)-1,1,1-trichloroethane (p,p'-DDT), and its metabolite, 2,2-bis(4-chlorophenyl)-1,1-dichloroethylene (p,p'-DDE). After Soxhlet extraction and cleanup on acidified silica solid-phase extraction cartridges, analysis was achieved by capillary gas chromatography/electron impact mass spectrometry. The method allowed the determination of 5 PBDE and 35 PCB congeners. Concentrations of PBDEs (sum of congeners IUPAC Nos. 28, 47, 99, 100, and 153) ranged between 2.2 and 11.7 ng/g lipid weight and were on the lower end of reported PBDE concentrations in European countries. The median value for the sum of PCBs (35 congeners) was 841 ng/g lipid weight and ranged from 286 to 1802 ng/g lipid weight. The median value for the sum of DDTs (calculated from p,p'-DDE and p,p'-DDT) was 290 ng/g lipid weight and ranged from 47 to 2802 ng/g lipid weight. The sum of PCBs showed a good correlation with the sum of DDTs (r=0.77, P<0.05), while the correlation with the sum of PBDEs was weaker (r=0.56, P<0.05). No age dependency was found for PBDEs (r=0.09), while PCBs and DDTs showed higher correlation coefficients with age (r=0.59 and 0.40, respectively, P<0.05).     

Trophodynamics of polybrominated diphenyl ethers and methoxylated polybrominated diphenyl ethers in a marine food web

The current study measured the concentrations of 14 polybrominated diphenyl ethers (PBDEs) and eight methoxylated polybrominated diphenyl ethers (MeO-PBDEs) in a marine food web and estimated their trophic magnification factors (TMFs), to highlight the differences between invertebrates, fish, and seabirds. Concentrations of PBDEs were orders of magnitude greater in seabirds (184.07 ± 161.63 ng/g lipid wt) compared with invertebrates and fish (19.01 ± 14.14 ng/g lipid wt). Although the congener profiles in invertebrates, fish, and juvenile seabirds were dominated by BDE-47, the contributions of BDE-99 and BDE-153 in adult seabirds were also significant. Unlike PBDEs, however, higher average MeO-PBDE concentrations were detected in fish (126.27 ± 189.27 ng/g lipid wt) and bivalves (15.96 ± 11.82 ng/g lipid wt) than in seabirds (2.61 ± 2.87 ng/g lipid wt). Correlations between lipid-normalized PBDE concentrations and trophic levels confirmed that seven PBDE congeners were magnified in the invertebrate-fish-seabird food web and that PBDE concentrations increased at a much greater rate across trophic levels in seabirds than in invertebrates and fish. This result indicates that estimating TMFs of PBDEs separately for seabirds, invertebrates, and fish is preferable. For MeO-PBDEs, no significant relationships were obtained in the invertebrate-fish-seabird food web.     

Polybrominated diphenyl ether congener patterns, hexabromocyclododecane, and brominated biphenyl 153 in eggs of peregrine falcons (Falco peregrinus) breeding in Sweden

Previous analyses of 52 peregrine falcon (Falco peregrinus) eggs collected from two wild and one captive population in Sweden 1987 through 1999 were complemented by including additional polybrominated diphenyl ether (PBDE) congeners (BDE-35, -183, -184, -185, -196, -197, -203, and -207). In addition, 31 eggs not previously analyzed for hexabromocyclododecane (HBCD) and BDE-209 were analyzed for these. Geometric mean concentrations of BPBDEs, HBCD, and the hexabrominated biphenyl (BB-153) were 3,100, 140, and 81 ng/g of lipid weight for the southern population; 2,500, 110, and 84 ng/g of lipid weight for the northern population; and 47, not detected, and 8 ng/g of lipid weight for the captive population. The BDE congener pattern was dominated by BDE-153, -99, and -100. The results were used to investigate whether a difference in PBDE congener pattern could be distinguished between the two wild populations of peregrine falcons due to different diets, as the southern population preys mainly on birds belonging to the terrestrial food chain while the northern population preys more on aquatic birds. A multivariate t-test showed a subtle but significant (p < 0.001) difference in PBDE congener pattern between the two populations. However, our hypothesis that higher-brominated congeners of PBDEs would be present to a greater extent in the terrestrial food chain was not supported by principal component analysis. The average brood size for individual females from the southern population decreased with increasing concentrations of IPBDE in the eggs (log-linear regression p < 0.01).     

Bioaccumulation and biotransformation of 61 polychlorinated biphenyl and four polybrominated diphenyl ether congeners in juvenile American kestrels (Falco sparverius)

This study examined the bioaccumulation and dietary retention of 61 polychlorinated biphenyl (PCB) and four polybrominated diphenyl ether (PBDE) congeners in juvenile American kestrels (Falco sparverius). American kestrels were exposed to contaminants via egg injection and daily gavage dosing over the posthatch-to-fledgling period. Retention factors for PCBs were dependent on chemical hydrophobicity and chlorine substitution patterns and ranged from less than 1 to 16.4% for PCBs having vicinal hydrogen substitutions at meta-, para- carbons on at least one of the phenyl rings and between 13.2 and 81.5% for congeners containing chlorine substitutions at 4,4'-, 3',4,5'-, 3,4',5-, or 3,3',5,5'-positions. These results indicate that juveniles are capable of biotransforming PCBs according to the same structure-activity rules as adults. A toxicokinetic model, initially parameterized using adult toxicokinetic parameters, was used to describe concentration trends in juveniles over time. The adult model overestimated PCB concentrations but provided an adequate fit when elimination rate constants were increased by a factor of 12.7. Retention factors for the PBDE congeners 2,2',4,4'-tetrabromodiphenyl ether (BDE 47), 2,2',4,4',6-pentabromodiphenyl ether (BDE 100), 2,2',4,4',5-pentabromodiphenyl ether (BDE 99), and 2,2',4,4',5,5'-hexabromodiphenyl ether (BDE 153) were from 7.8 to 45.3% of the total dose. The retention of BDE 47 was similar that observed for readily cleared PCBs, whereas the remaining PBDEs exhibited retention factors consistent with those of persistent PCBs. Half-lives for PBDEs in juveniles were estimated to range from 5.6 to 44.7 d. Assuming differences in PBDE toxicokinetics between juveniles and adults similar to those measured for PCBs, adult American kestrel PBDE half-lives are expected to range from 72 to 572 d.     

Assessment of the Levels of Polybrominated Diphenyl Ethers in Blood Samples from Guadalajara,Jalisco, Mexico

The purpose of this study was to measure levels of polybrominated diphenyl ethers (PBDEs) in the blood of children (50 individuals) living in Guadalajara, Jalisco, Mexico. We analyzed six PBDE congeners by gas chromatography–mass spectrometry. Total PBDE levels ranged from not detectable (nd) to 15.2 μg/L on a whole-weight basis and from nd to 6,435 ng/g lipid on a lipid-weight basis. The dominant congener in our study was BDE-153, followed by BDE-154, BDE-99, BDE-100, and BDE-47. Levels of BDE-209 were below the detection limit. Our data indicate that children living in the areas studied in this work are exposed to high levels of PBDEs.     

Polybrominated diphenyl ethers and polychlorinated biphenyls in commercially wild caught and farm-raised fish fillets in the United States

Wild caught and farm-raised fish fillets collected in fish markets and large-chain super markets located in the Maryland, Washington, DC, and North Carolina were measured for their polybrominated diphenyl ether (PBDE), polychlorinated biphenyl (PCB), and polychlorodibenzo-p-dioxins/dibenzofurans (PCDD/Fs) levels. PCB and PBDE concentrations were the highest in a wild bluefish fillet (800 and 38 ng/g wet weight, respectively) and the lowest in wild Coho salmon fillet (0.35 and 0.04 ng/g, respectively). Levels for both PCBs and PBDEs in ng/g wet weight decreased from bluefish with medians of 200 and 6.2, to rockfish 66 and 4.7, followed by farmed-raised salmon with 9.0 and 1.1, with the lowest in wild salmon, 4.0 and 0.3 ng/g for PCBs and PBDEs, respectively (PCBs are the sum of 25 congeners). The chlorinated biphenyl (CB)-153 and brominated diphenyl ether (BDE)-47 levels correlated in the 22 fish fillets with a Pearson correlation coefficient of 0.94. Bluefish, rockfish (striped bass), wild caught and farm-raised salmons all showed different linear regression slopes between CB-153 and BDE-47 of 7.5, 2.7, 0.97, and 1.5, respectively. A Wilcoxon rank sum test showed no significant difference in the CB-153/BDE-47 ratios between farmed raised and all species of wild salmon combined, but was significant between bluefish and rockfish, farmed raised salmon or wild salmon.     

Measurement of polybrominated diphenyl ethers and metabolites in mouse plasma after exposure to a commercial pentabromodiphenyl ether mixture

BACKGROUND: Previous studies have shown that polybrominated diphenyl ethers (PBDEs) behave as weak estrogens in animal and cell culture bioassays. In vivo metabolites of PBDEs are suspected to cause these effects. OBJECTIVES: To identify candidate metabolites, mouse plasma samples were collected after continuous oral and subcutaneous exposure to DE-71, a widely used commercial pentabromodiphenyl ether product, for 34 days. METHODS: Samples were extracted, separated into neutral and phenolic fractions, and analyzed by gas chromatographic mass spectrometry. RESULTS: In the plasma samples of orally treated animals, 2,2',4,4',5,5'-hexabromodiphenyl ether (BDE-153) represented 52% of total measurable PBDEs, whereas it represented only 4.3% in the DE-71 mixture. This suggested that BDE-153 was more persistent than other congeners in mice. Several metabolites were detected and quantitated: 2,4-dibromophenol, 2,4,5-tribromophenol, and six hydroxylated PBDEs. The presence of the two phenols suggested cleavage of the ether bond of 2,2',4,4'-tetrabromodiphenyl ether (BDE-47) and 2,2',4,4',5-pentabromodiphenyl ether (BDE-99), respectively. The hydroxylated (HO)-PBDEs might come from hydroxylation or debromination/hydroxylation. Among the quantitated hydroxylated metabolites, the most abundant was 4-HO-2,2',3,4'-tetra-BDE, which suggested that there was a bromine shift during the hydroxylation process. para-HO-PBDEs have been proposed to behave as endocrine disruptors. CONCLUSIONS: THERE SEEM TO BE THREE METABOLIC PATHWAYS: cleavage of the diphenyl ether bond, hydroxylation, and debromination/hydroxylation. The cleavage of the diphenyl ether bond formed bromophenols, and the other two pathways formed hydroxylated PBDEs, of which para-HO-PBDEs are most likely formed from BDE-47. These metabolites may be the most thyroxine-like and/or estrogen-like congeners among the HO-PBDEs.     

High body burdens of 2,2',4,4'-tetrabromodiphenyl ether (BDE-47) in California women

Following our first report on elevated polybrominated diphenyl ether (PBDE) concentrations in California women, we expanded our investigation to include diverse groups of local women. We analyzed additional adipose and serum samples collected in the late 1990s from San Francisco Bay Area women participating in a breast cancer study and in a reproductive study, respectively. Adipose samples (n = 32) were analyzed by low-resolution mass spectrometry in negative-ion chemical ionization mode, whereas serum samples (n = 50) were analyzed by dual-column gas chromatography with electron capture detection. The results confirmed our earlier findings. Concentrations of 2,2,4,4 -tetrabromodiphenyl ether (BDE-47) in contemporary California women ranged between 5 and 510 ng/g lipid, with a median (16.5 ng/g lipid) 3-10 times higher than those reported from Europe. In contrast, PBDEs were not measurable in any of 420 archived serum samples collected in the 1960s from San Francisco Bay Area women participating in a study of child development. BDE-47 concentrations did not increase with age or with concentrations of a polychlorinated biphenyl (PCB-153), suggesting other routes of exposure in addition to diet. Rising body burdens of endocrine-disrupting chemicals such as PBDEs may pose a potential public health threat.     

Negative associations between PBDE levels and thyroid hormones in cord blood

Polybrominated diphenyl ethers (PBDEs) causing thyroidal effects have been demonstrated in in vivo and in vitro studies. PBDEs with structural similarities to thyroid hormones have increased recently, but the health effects for thyroid hormones have not been well studied. The study aimed to determine PBDE levels in cord blood and further to explore associations between prenatal PBDE exposures and thyroid hormones in cord blood. Fifty-four cord blood samples were collected after delivery. Cord-blood levels of BDE-15, 28, 47, 99, 100, 153, 154, and 183 were analyzed using a high resolution gas chromatograph with a high resolution mass spectrometer. Thyroid hormones were determined by an automated chemiluminescence analyzer. The mean, median, and standard deviation of ΣPBDEs were 4.72, 3.49, and 6.36 ng/g lipid, respectively. To adjust for confounding by maternal age, pre-pregnant BMI and gestational age, stepwise multiple linear regression was used after log(2) transformation of the exposure variables. A doubling of BDE-154 was associated with 0.043 ng/mL lower triiodothyronine (T3) values (adjusted r=-0.245, p=0.043). Likewise a doubling of BDE-153 was associated with 0.143 ng/mL lower free T3 (FT3) values and a doubling of BDE-183 with 0.084 ng/mL lower FT3 values (adjusted r=-0.487, p=0.023). In contrast, the T4 (thyroxine)/T3 ratio increased by 4.93 (adjusted r=0.277, p=0.017) when doubling BDE-100 exposure. No significant associations with BDE-47 or any other of the PBDEs was found. Our findings of an inverse relationship between BDE-153, BDE-154 or BDE-184 and thyroid hormones confirm the results of animal experiments but are in contrast to most epidemiological studies.     

Flame retardant exposure: polybrominated diphenyl ethers in blood from Swedish workers.

Polybrominated diphenyl ethers (PBDEs) are used as additives in polymers and textiles to prohibit the development of fires. Because of the production and use of PBDEs, their lipophilic characteristics, and persistence, these compounds have become ubiquitous environmental contaminants. The aim of the present study was to determine potential exposures of PBDEs to clerks working full-time at computer screens and personnel at an electronics-dismantling plant, with hospital cleaners as a control group. Five PBDE congeners--2,2',4,4'-tetraBDE; 2,2',4,4',5,5'-hexaBDE; 2,2',4,4',5, 6'-hexaBDE; 2,2',3,4,4',5',6-heptaBDE; and decaBDE--were quantified in blood serum from all three categories of workers. Subjects working at the dismantling plant showed significantly higher levels of all PBDE congeners in their serum as compared to the control group. Decabromodiphenyl ether is present in concentrations of 5 pmol/g lipid weight (lw) in the personnel dismantling electronics; these concentrations are comparable to the concentrations of 2,2',4, 4'-tetraBDE. The latter compound was the dominating PBDE congener in the clerks and cleaners. The major compound in personnel at the dismantling plant was 2,2',3,4,4',5',6-heptaBDE. Concentrations of this PBDE congener are almost twice as high as for 2,2',4, 4'-tetraBDE in these workers and seventy times the level of this heptaBDE in cleaners. The total median PBDE concentrations in the serum from workers at the electronics-dismantling plant, clerks, and cleaners were 37, 7.3, and 5.4 pmol/g lw, respectively. The results show that decabromodiphenyl ether is bioavailable and that occupational exposure to PBDEs occurs at the electronics-dismantling plant.     

上海市某医院新生儿脐带血中多溴联苯醚水平及其对出生结局的影响

目的 调查上海市某医院新生儿脐带血中多溴联苯醚(polybrominated diphenyl ethers,PBDEs)浓度水平,并分析胎儿期PBDEs暴露对新生儿出生结局的影响.方法 于2006年9月至2007年4月,对上海市某医院50名入院分娩的孕妇进行问卷调查,孕妇均为单胎妊娠,排除高血压、糖尿病、HIV感染和不良药物史.收集新生儿脐带血样本,使用气相色谱-负化学电离源-质谱法检测脐带血中7种PBDEs[溴代联苯醚(BDE)-28、BDE-47、BDE-99、BDE-100、BDE-153、BDE-154、BDE-183]浓度,计算PBDEs总浓度(∑,PBDEs),并进一步分析脐带血中PBDEs浓度水平对新生儿出生结局的影响.结果 上海市某医院新生儿身长为(50.15±0.75)cm,体重为(3.49±0.42)kg,胸围为(34.76±1.51)cm,头围为(35.03±1.40)cm,体质指数为(13.76±1.36)kg/m2.新生儿脐带血中∑,PBDEs中位数浓度(范围)为14.06(1.03～379.73)ng/g脂重(lipid weight,1w).BDE-28、BDE-47、BDE-99、BDE-100、BDE-153、BDE-154、BDE-183检出率分别为22%(11/50)、22%(11/50)、98%(49/50)、72%(36/50)、76%(38/50)、90%(45/50)、14%(7/50).各同族体中位数浓度(范围)分别为:BDE-28为<检测限(LOD)(＜LOD～137.20 ng/g 1w),BDE-47为＜LOD(＜LOD-33.17 ng/g 1w),BDE-99为7.54(＜LOD-94.01)ng/g 1w,BDE-100为1.57(＜LOD-46.95)ng/g 1w,BDE-153为0.63(＜LOD-79.08)ng/g 1w,BDE-154为0.63(＜LOD-22.30)ng/g 1w,BDE-183为＜LOD(＜LOD-21.63 ng/g 1w).新生儿体质指数与BDE-99(r=-0.347,P＜0.05)和BDE-154(r=-0.292,P＜0.05)浓度呈负相关.将出生结局按照累计频率25%分为低(≤25%)、高(＞25%)两组,BDE-99在低身长组(≤50 cm)和高身长组(＜50 cm)的几何均数分别为10.59 ng/g 1w和3.60 ng/g 1w,二者差异有统计学意义(t=2.32,P=0.03).结论 上海市某医院新生儿脐带血中普遍存在PBDEs,胎儿期PBDEs暴露可影响新生儿出生结局.

Abstract：

Objective To explore the concentration of polybrominated diphenyl ethers(PBDEs)in umbilical cord serum and analyze the influence of exposure to PBDEs during fetal stage on newborn birth outcomes in Shanghai.Methods Fifty delivery women in a Shanghai hospital were surveyed by questionnaire.and the umbilical cord serum were collected from September 2006 to April 2007.All the delivery women were singleton pregnancies,excluding hish blood pressure,diabetes,HIV infection and adverse medical history.Seven congeners(BDE-28,BDE-47,BDE-99,BDE-100,BDE-153,BDE-154 and BDE-183) were measured by gas chromatography-negative chemical ionization-mass spectrometry and the influencing factors were anatyzed. Results Newborns'length.weight,chest circumference,head circumference and body mass index(BMI)were(50.15±0.75)cm,(3.49±0.42)kg,(34.76±1.51)cm,(35.03 ±1.40)cm,(13.76±1.36)kg/m2,respectively.The median of ∑7 PBDEs concentration in umbilical cord serum was 14.06(1.03-379.73)ng/g lipid weight(1w).The detection rate of BDE-28,BDE-47,BDE-99,BDE-100,BDE-153,BDE-154 and BDE-183 were 22%(11/50),22%(11/50),98%(49/50).72%(36/50),76%(38/50),90%(45/50)and 14%(7/50),respectively.The median(range)of PBDEs (BDE-28,BDE-47,BDE-99,BDE-100,BDE-153,BDE-154,BDE-183)congeners were ＜LOD (＜LOD-137.20 ng/g 1w),＜LOD(＜LOD-33.17 ng/g 1w),7.54.ng/g 1w(＜LOD-94.01 ng/g 1w),1.57 ng/g 1w(＜LOD-46.95 ng/g 1w),0.63.ng/g 1w(＜LOD-79.08 ng/g 1w),0.63 ng/g 1w(＜LOD-22.30 ng/g 1w)and＜LOD(＜LOD-21.63 ng/g 1w),respectiveIy.The newborns'BMI showed a negative correlation with BDE-99(r=-0.347.P＜0.05)and BDE.154(r=-0.292.P＜0.05).BDE-99in low-length group(≤50 cm,10.59 ng/g 1w) was significantly higher(t=2.32,P=0.03)than that in high-length group(＞50 cm,3.60 ng/g 1w).Conclusion PBDEs were commonly detected in newborns'umbilical cord serum in this study.Our findings indicated that exposure to PBDEs adversely affected the development of the newborns.     

2010年太原市普通人群血清中多溴联苯醚负荷水平

目的 研究太原市普通人群血清中多溴联苯醚(PBDEs)负荷水平.方法 2010年在太原市共采集了42份普通人群血清样品,用固相萃取-气相色谱-负化学源-质谱法测定了样品中溴代联苯醚(BDE)-17、BDE-28、BDE-47、BDE-66、BDE-99、BDE-100、BDE-153、BDE-154、BDE-183 和...     

Polybrominated diphenyl ethers in paired samples of maternal and umbilical cord blood plasma and associations with house dust in a Danish cohort

Brominated flame retardants (BFRs), in particular the polybrominated diphenyl ethers (PBDEs), have been used in consumer products for many years to increase fire resistance. Recently, developmental neurotoxicity at very low levels has increased the concern about these compounds. The major objectives of this study were to investigate the maternal and fetal exposure to PBDEs on the basis of maternal and umbilical cord plasma samples and to study the extent of placental transfer for different PBDE congeners. The findings were also compared with previously observed PBDE levels and patterns determined in placental tissue from the same individuals, and the relationship with the external exposure from house dust from the participants’ homes was explored. Samples of maternal and umbilical cord plasma from a cohort of 51 pregnant women from the Copenhagen area were collected. Paired maternal and umbilical cord plasma were analysed for BDE-28, 37, 47, 85, 99, 100, 119, 138, 153, 154, 183, 209 and the brominated biphenyl BB-153 using automated SPE extraction and GC-HRMS for the tri- to hepta-BDEs and GC-LRMS (ECNI) for BDE-209. PBDEs were detected in all maternal and umbilical cord plasma samples. The sum of tri- to hexa-BDEs (ΣPBDE) in maternal plasma varied between 640 and 51,946 pg/g lipid weight (lw) with a median level of 1765 pg/g lw. In the umbilical cord samples ΣPBDE varied between 213 and 54,346 pg/g lw with a median of 958 pg/g lw. The levels observed in fetal and maternal plasma were highly correlated, but the placental transport of PBDE congeners was found to decrease with increasing diphenyl ether bromination. Maternal concentrations were significantly correlated (p < 0.05) for most congeners with the previously determined concentrations in placental tissue from the same individuals. Furthermore, positive correlations (p < 0.05) were found for BDE-28, 47, 100, 209 and ΣPBDE in maternal plasma and house dust as well as for ΣPBDE in umbilical cord plasma and house dust. The positive correlations for PBDEs for both maternal and umbilical cord plasma with house dust showed that domestic house dust is a significant source of human exposure to PBDEs in Denmark including in utero exposure.     

上海市某医院产妇乳汁中多溴联苯醚暴露水平

目的 通过对上海市某医院产妇乳汁中多溴联苯醚(PBDEs)含量的测定和分析,了解该地区人群中PBDEs的暴露水平及其相关影响因素.方法 于2006年9月至2007年4月在上海市某医院对48名产妇进行问卷调查,并采集其乳汁样本,产妇均为单胎妊娠,排除高血压、糖尿病、HIV感染和不良用药史.采用气相色谱-负化学电离源-质谱法测定乳汁中7种PBDE同族体[溴代联苯醚(BDE)-28,BDE-47,BDE-100,BDE-99,BDE-154,BDE-153和BDE-183]的含量,并分析其影响因素.结果 产妇乳汁中7种PBDEs(∑,PBDEs)浓度中位数为8.81 ng/g脂重(lipid weight,1w),浓度范围为1.92-41.55 ng/g 1w.BDE-28、BDE-47、BDE-100、BDE-99、BDE-154、BDE-153、BDE-183检出率分别为98%(47/48)、96%(46/48)、86%(41/48)、90%(43/48)、83%(40/48)、98%(47/48)、90%(43/48);浓度中位数分别为0.88、0.99、0.97、1.39、1.14、2.17、1.41 ng/g 1w.不同学历产妇乳汁中PBDEs水平(logΣ7PBDEs)分别为:初中及以下为(0.89±0.24)、高中为(1.02±0.17)、大专及以上为(1.08±0.28);不同月收入水平产妇乳汁中PBDEs水平(log∑7PBDEs)分别为:＜1000元为(0.89±0.12)、1000-3000元为(1.01±0.24)、＞3000元为(1.13±0.21).相关分析发现母亲受教育水平(r=0.322,P＜0.05)和收入水平(r=0.388,P＜0.05)与母乳PBDEs暴露水平呈正相关.结论 产妇乳汁中普遍含有PBDEs,母亲受教育水平和收入水平可能影响母乳中PBDEs水平.

Abstract：

Objective To measure the concentration of polybrominated diphenyl ethers(PBDEs)in human breast milk from a hospital in Shanghai and analyze the influencing factors.Methods Forty-eight puerperas from a hospital in Shanghai were selected to answer a questionnaire.and their breast milk samples were collected from September 2006 to April 2007.All the puerperas were singleton pregnancies.excluding high blood pressure.diabetes,HIV infection and adverse medical history.Seven congenera(BDE-28,BDE47,BDE-100,BDE-99,BDE-154,BDE-153 and BDE-183)were measured by gas chromatography-negative chemical ionization-mass spectrometry and the influencing factors were analyzed.Results The median of total PBDEs concentration in breast milk was 8.81 ng/g lipid weight(1w),and the range was 1.92-41.55,,g/g 1W. The detection rates of seven congeners(BDE-28,BDE-47,BDE-100,BDE-99,BDE-154,BDE-153,BDE-183)were 98%(47/48),96%(46/48),86%(41/48),90%(43/48),83%(40/48),98%(47/48),90%(43/48),and the median of them was,0.88,0.99,0.97,1.39,1.14,2.17,1.41 ng/g 1w,respectively.LogΣ7PBDEs in breast milk from mothers with different education levels were divided into junior high school or lower(0.89 ±0.24),senior high school(1.02±0.17),junior college or higher(1.08±0.28).LogΣ7PBDEs in breast milk from mothers with different income levels were divided as ＜1000 yuan(0.89±0.12),1000-3000 yuan(1.01±0.24),＞3000 yuan(1.13±0.21).Correlation analysis showed that both the mothers'education level(r=0.322.P＜0.05)and income level(r=0.388.P＜0.05)have a positive correlation to PBDEs levels in breast milk. Conclusion It is very common to detect PBDEs in human breast-milk.however,the education and income levels of the mothers my be the influencing factors.     

Secular trends and geographical variations in the dietary intake of polybrominated diphenyl ethers (PBDEs) using archived samples from the early 1980s and mid 1990s in Japan

A retrospective exposure assessment among the general population for polybrominated diphenyl ethers (PBDEs) was conducted using dietary surveys. We analyzed samples of food duplicate portions collected in the early 1980s (1980 survey: N=40) and the mid 1990s (1995 survey: N=39) from female subjects (5 participants from each of 8 sites per survey except for one site) living throughout Japan, from the north (Hokkaido) to the south (Okinawa). The study populations in the 1980 and 1995 surveys were different, but lived in the same communities. We measured four PBDE congeners [2,2',4,4'-tetrabrominated diphenyl ether (tetraBDE): #47; 2,2',4,4',5-pentaBDE: #99; 2,2',4,4',6-pentaBDE: #100; and 2,2',4,4',5,5'-hexaBDE: #153] in the diet. #99 was the most abundant congener in the diet (49% of the total PBDEs), followed by #47 (33%), #100 (12%) and #153 (6%). Regional variations found in the 1980 survey decreased in the 1995 survey. The total daily intake of PBDEs (ng/d) [GM (GSD)] in the 1980 survey [91.4 (4.1)] was not significantly different from that in the 1995 survey [93.8 (3.4)] for the total population, nor did it differ among the sites including Shimane, in which a 20-fold increase in serum concentrations was observed in the same population1). In consideration of the significant increases in the serum concentration, inhalation may be more important than food ingestion as the route of human exposure to PBDEs.     

Polybrominated diphenyl ethers in breast milk from Uppsala County,Sweden

The breast milk concentrations of polybrominated diphenyl ethers (PBDEs; sum of five congeners: BDE-47, -99, -100, -153, and -154) were determined (by GC-ECD) in samples from 93 primiparous women collected from 1996 to 1999 in Uppsala County, Sweden. Dietary and lifestyle factors were also recorded. The mean PBDE concentration was 4.0 ng/g fat and the distribution of samples was skewed with few high values (maximum 28.2 ng/g fat). BDE-47 was the major congener and constituted 59% of the mean concentration of PBDEs. No significant relationship was found between breast milk concentrations of PBDEs and dietary intake of PBDE, age, body mass index, alcohol consumption, or computer usage. After adjustments for these factors, a weak but significant association between PBDE concentrations and smoking was observed. The dietary intake of PBDE for these women was estimated at 27 ng/day, of which fish contributed almost half. After inclusion of 31 additional samples, collected from 2000 to 2001, time trends were studied. The changes in breast milk PBDE levels between 1996 and 2001, similar to the results from another Swedish study on milk from Stockholm mothers, suggest a peak in PBDE concentrations around 1998 and thereafter decreasing levels. However, far-reaching conclusions about PBDE time trends in milk cannot be drawn from this short study.     

Plasma concentrations of selected organobromine compounds and polychlorinated biphenyls in postmenopausal women of Québec, Canada

BACKGROUND: 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. OBJECTIVES: We set out to assess the internal exposure of postmenopausal Canadian women to selected organobromine compounds and to investigate factors associated with this exposure. METHODS: 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. RESULTS: 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. CONCLUSION: 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.     

Time trends and individual characteristics associated with polybrominated diphenyl ethers in breast milk samples 2006-2009 in Lower Saxony, Germany

Background

Since 2006 polybrominated diphenyl ether (PBDE) concentrations have been analyzed within the scope of the breast milk project conducted by the Governmental Institute of Public Health of Lower Saxony.

Objectives

Temporal trends and regional distributions of the resident population as well as the relevance of individual factors influencing PBDE concentration were to be determined.

Methods

Four PBDE congeners (BDE-47, BDE-153, BDE-99, BDE-100) have been analyzed. The concentrations are fitted by linear regression models, whereby individual factors of the mother are surveyed by a standardized questionnaire.

Results

A total of 2173 samples taken between 2006 and 2009 shows an estimated total PBDE mean value of 1.68 ng/g lipid weight (l.w.). In contrast to most other studies, the proportion of BDE-153 exceeds the one of BDE-47 (median: 0.51 ng/g l.w. vs. 0.31 ng/g l.w.).BMI shows a positive correlation with BDE-47 and a negative correlation with BDE-153, both statistically significant (p < 0.001). For BDE-153, other significant factors (former breast feeding periods, birth year of the mother and country of birth) reflect also dilution effects and the time of accumulation. A decreasing temporal trend is observed for BDE-47 but not for BDE-153.

Conclusions

The correlation patterns, the temporal trends and the various influencing factors may reflect differences in exposure sources and/or metabolism between the major congeners BDE-47 and BDE-153. Therefore it seems to be necessary to discuss the concentrations of BDE-47 and BDE-153 separately as leading indicators instead of using a total PBDE.