Flame retardants and organochlorines in indoor dust from several e-waste recycling sites in South China: Composition variations and implications for human exposure

Several classes of flame retardants, such as polybrominated diphenyl ethers (PBDEs), novel brominated flame retardants (NBFRs), dechlorane plus (DPs), and organophosphate flame retardants (PFRs), together with polychlorinated biphenyls (PCBs) were measured in indoor dust from five villages located in three e-waste recycling regions in Guangdong Province, South China. The medians of PBDEs, NBFRs, and PFRs in dust in five sites ranged from 685–67,500, 1460–50,010, and 2180–29,000 ng/g, respectively. These concentrations were much higher than the medians of PCBs (52–2900 ng/g). BDE 209 and decabromodiphenyl ethane (DBDPE) were the two major halogen flame retardants in dust, while tris-(1-chloro-2-propyl) phosphate (TCIPP) and triphenyl phosphate (TPHP) were the major PFRs. Principle component analysis revealed the different pollutant patterns among different sites. The estimated median human exposures of PBDEs, NBFRs, PFRs, and PCBs via dust ingestion were 1.1–24.1, 0.73–20.3, 1.36–23.5, and 0.04–0.93 ng/kg bw/day for adults, and 16.2–352, 10.7–296, 19.9–343, 0.05–0.61, 0.65–13.6 ng/kg bw/day for toddlers, respectively. Residents from Site 5 had the highest exposure (95 percentile levels and high dust ingestion for toddlers) of PBDEs (3920 ng/kg bw/day), NBFRs (3200 ng/kg bw/day), and PFRs (5280 ng/kg bw/day). More attention should be paid to the contamination with NBFRs and PFRs, instead of PCBs, in these e-waste recycling regions, and local public health threat from PBDE alternatives should remain of concern. To the best of our knowledge, this is the first study on human exposure assessment of PFRs at e-waste sites.     

Human dietary intake of organohalogen contaminants at e-waste recycling sites in Eastern China

This study reports concentrations and human dietary intake of hexabromocyclododecanes (HBCDs), polychlorinated biphenyls (PCBs) as well as selected “novel” brominated flame retardants (NBFRs) and organochlorine pesticides, in ten staple food categories. Samples were sourced from areas in Taizhou City, eastern China, where rudimentary recycling and disposal of e-waste is commonplace, as well as from nearby non-e-waste impacted control areas. In most instances, concentrations in foods from e-waste recycling areas exceeded those from control locations. Concentrations of 2-ethylhexyl-2,3,4,5-tetrabromobenzoate (EH-TBB) and bis-(2-ethylhexyl)-3,4,5,6-tetrabromophthalate (BEH-TBP) in samples from e-waste sites were 3.09–62.2 ng/g and 0.81–16.3 ng/g lipid weight (lw), respectively; exceeding consistently those in foods acquired from control sites by an order of magnitude in many cases. In contrast, while concentrations of HBCD in some foods from e-waste impacted areas exceed those from control locations; concentrations in pork, shrimp, and duck liver are higher in control samples. This highlights the potential significance of non-e-waste sources of HBCD (e.g. building insulation foam) in our study areas. While concentrations of DDT in all foods examined except pork were higher in e-waste impacted samples than controls; our exposure estimates were well below the provisional tolerable daily intake of 0.01 mg/kg bw/day derived by the Joint FAO/WHO Meeting on Pesticide Residues. Concentrations of ΣPCBs resulted in exposures (650 and 2340 ng/kg bw/day for adults and children respectively) that exceed substantially the Minimal Risk Levels (MRLs) for ΣPCBs of 20 ng/kg bw/day derived by the Agency for Toxic Substances & Disease Registry. Moreover, when expressed in terms of dioxin-like toxicity equivalency based on the four dioxin-like PCBs monitored in this study (DL-PCBs) (PCB-105, 118, 156, and 167); concentrations in e-waste impacted foods exceed limits set by the European Union in 6 of the 8 food groups studied and result in dietary exposures for children (10.2 pg TEQ/kg bw/day) that exceed the WHO tolerable daily intake of 1–4 pg TEQ/kg bw/day.     

Human dietary exposure to polycyclic aromatic hydrocarbons: Results of the second French Total Diet Study

In the frame of the second French Total Diet Study (TDS), the 15 + 1 EU priority polycyclic aromatics hydrocarbons (PAHs) were analyzed in 725 foodstuffs habitually consumed by the French population, using gas chromatography coupled to tandem mass spectrometry, after pressurized liquid extraction and purification on PS-DVB stationary phase. The highest PAH concentrations recovered in foodstuffs corresponded to the following contributors: chrysene (25.7%), benzo[b]fluoranthene (15.0%) and benz[a]anthracene (9.0%) whereas the lowest concentrations were those of dibenz[a,h]anthracene, 5 methylchrysene and dibenzo[a,h]pyrene (below 2.0%). By food groups, the current highest levels of total PAH were detected in mollusks and crustaceans, followed by the different oil based products. To estimate French population's exposure, contamination data were combined with national individual food consumption data. Mean daily exposure to the sum of benzo[a]pyrene, benz[a]anthracene, chrysene and benzo[b]fluoranthene (PAH4) was estimated to be 1.48 ng/kg bw/day in adults and 2.26 ng/kg bw/day in children. The main contributors to PAH exposure for adults are fats, bread and dried bread products followed by crustaceans and mollusks. The margin of exposure (MOE) approach indicates that exposure to PAHs through food is not a major health problem for French consumers.     

A comparative assessment of human exposure to tetrabromobisphenol A and eight bisphenols including bisphenol A via indoor dust ingestion in twelve countries

Tetrabromobisphenol A (TBBPA) and eight bisphenol analogues (BPs) including bisphenol A (BPA) were determined in 388 indoor (including homes and microenvironments) dust samples collected from 12 countries (China, Colombia, Greece, India, Japan, Kuwait, Pakistan, Romania, Saudi Arabia, South Korea, U.S., and Vietnam). The concentrations of TBBPA and sum of eight bisphenols (ƩBPs) in dust samples ranged from < 1 to 3600 and from 13 to 110,000 ng/g, respectively. The highest TBBPA concentrations in house dust were found in samples from Japan (median: 140 ng/g), followed by South Korea (84 ng/g) and China (23 ng/g). The highest ∑ BPs concentrations were found in Greece (median: 3900 ng/g), Japan (2600 ng/g) and the U.S. (2200 ng/g). Significant variations in BPA concentrations were found in dust samples collected from various microenvironments in offices and homes. Concentrations of TBBPA in house dust were significantly correlated with BPA and ∑ BPs. Among the nine target chemicals analyzed, BPA was the predominant compound in dust from all countries. The proportion of TBBPA in sum concentrations of nine phenolic compounds analyzed in this study was the highest in dust samples from China (27%) and the lowest in Greece (0.41%). The median estimated daily intake (EDI) of ∑ BPs through dust ingestion was the highest in Greece (1.6–17 ng/kg bw/day), Japan (1.3–16) and the U.S. (0.89–9.6) for various age groups. Nevertheless, in comparison with the reported BPA exposure doses through diet, dust ingestion accounted for less than 10% of the total exposure doses in China and the U.S. For TBBPA, the EDI for infants and toddlers ranged from 0.01 to 3.4 ng/kg bw/day, and dust ingestion is an important pathway for exposure accounting for 3.8–35% (median) of exposure doses in China.     

Occurrence of parabens in foodstuffs from China and its implications for human dietary exposure

Parabens are alkyl esters of p-hydroxybenzoic acid and are used as antimicrobial preservatives in a range of consumer products, including cosmetics, pharmaceuticals, and foodstuffs. Despite their widespread use, prior to this study, paraben concentrations in foodstuffs from China and human dietary exposure to these chemicals have been unknown. In this study, concentrations of six parabens were determined in 13 categories of food samples (n = 282), including cereals and cereal products, meat, fish and seafood, eggs, dairy products, bean products, fruits, vegetables, cookies, beverages, cooking oils, condiments, and others, collected from nine cities in China. Almost all (detection rate: 99%) food samples contained at least one of the parabens analyzed, and the total concentrations (ΣParabens; sum of six parabens) ranged from below limit of quantification (LOQ) to 2530 ng/g fresh weight, with an overall mean value of 39.3 ng/g. Methyl paraben (MeP), ethyl paraben (EtP), and propyl paraben (PrP) were the major paraben analogs found in foodstuffs, and these compounds accounted for 59%, 24%, and 10%, respectively, of ΣParaben concentrations. Although the mean concentrations of ΣParabens varied among different categories of food items (from 0.839 ng/g in beverages to 100 ng/g in vegetables), the concentrations were not statistically significant among the 13 food categories, including canned foodstuffs. Estimated daily intake (EDI) of parabens was based on the measured concentrations in foods and the corresponding daily food ingestion rates. The mean and 95th percentile values for EDI were 1010 and 3040 ng/kg body weight (bw)/day for adult men and 1060 and 3170 ng/kg bw/day for adult women, respectively.     

Country specific comparison for profile of chlorinated,brominated and phosphate organic contaminants in indoor dust. Case study for Eastern Romania, 2010

We have evaluated the levels and specific profiles of several organohalogenated contaminants, including organochlorine pesticides (OCPs), polychlorinated biphenyls (PCBs), and flame retardants (FRs), such as polybrominated diphenyl ethers (PBDEs), hexabromocyclododecanes (HBCDs), novel brominated FRs (NBFRs), and organophosphate FRs (OPFRs), in 47 indoor dust samples collected in 2010 from urban locations from Iasi, Eastern Romania. The dominant contaminants found in the samples were OPFRs (median sum OPFRs 7890 ng/g). Surprisingly, OCPs were also measured at high levels (median 1300 ng/g). Except for BDE 209 (median 275 ng/g), PBDEs were present in dust samples at relatively low levels (median sum PBDEs 8 ng/g). PCBs were also measured at low levels (median sum PCBs 35 ng/g), while NBFRs were only occasionally detected, showing a low usage in goods present on the Romanian market. The results of the present study evidence the existence of a multitude of chemical formulations in indoor dust. FRs are usually associated to human exposure via ingestion of dust, but other chemicals, such as OCPs, are not commonly reported in such matrix. Although OCPs were found at comparable levels with OPFRs in Romanian dust, OCPs possess a higher risk to human health due to their considerably lower reference dose (RfD) values. Indeed, the OCP exposure calculated for various intake scenarios was only 2-fold lower than the corresponding RfD. Therefore, the inclusion of OCPs as target chemicals in the indoor environment becomes important for countries where elevated levels in other environmental compartments have been previously shown.     

Priority and emerging flame retardants in rivers: Occurrence in water and sediment,Daphnia magna toxicity and risk assessment

The occurrence, partitioning and risk of eight polybrominated diphenyl ethers (PBDEs), nine new brominated (NBFRs) and ten organophosphorus flame retardants (OPFRs) were evaluated in three Spanish rivers suffering different anthropogenic pressures (Nalón, Arga and Besòs). OPFRs were ubiquitous contaminants in water (ΣOPFRs ranging from 0.0076 to 7.2 μg L^− 1) and sediments (ΣOPFRs ranging 3.8 to 824 μg kg^− 1). Brominated flame retardants were not detected in waters, whereas ΣPBDEs ranged from 88 to 812 μg kg^− 1 and decabromodiphenyl ethane (DBDPE) reached 435 μg kg^− 1 in sediments from the River Besòs, the most impacted river. The occurrence of flame retardants in river water and sediment was clearly associated with human activities, since the highest levels occurred near urban and industrial zones and after wastewater treatment plants discharge. Daphnia magna toxicity was carried out for OPFRs, the most ubiquitous flame retardants, considering individual compounds and mixtures. Toxicity of nine tested OPFRs differed largely among compounds, with EC₅₀ values ranging over three magnitude orders (0.31–381 mg L^− 1). Results evidenced that these compounds act by non-polar narcosis, since their toxicity was proportional to their lipophilicity (K_ow). Furthermore, their joint toxicity was additive, which means that single and joint toxicity can be predicted knowing their concentration levels in water using quantitative structure activity relationships (QSARs) and predictive mixture models. Based on these results, a risk assessment considering joint effect was performed calculating and summing risk quotients (RQs) for the water and sediment samples. No significant risk to D. magna (ΣRQs < 1) was observed for any of the monitored rivers.     

Brominated and chlorinated flame retardants in San Francisco Bay sediments and wildlife

Restrictions on the use of polybrominated diphenyl ethers (PBDEs) have resulted in the use of alternative flame retardants in consumer products to comply with flammability standards. In contrast to PBDEs, information on the occurrence and fate of these alternative compounds in the environment is limited, particularly in the United States. In this study, a survey of flame retardants in San Francisco Bay was conducted to evaluate whether PBDE replacement chemicals and other current use flame retardants were accumulating in the Bay food web. In addition to PBDEs, brominated and chlorinated flame retardants (hexabromocyclododecane (HBCD) and Dechlorane Plus (DP)) were detected in Bay sediments and wildlife. Median concentrations of PBDEs, HBCD, and DP, respectively, were 4.3, 0.3, and 0.2 ng g^− 1 dry weight (dw) in sediments; 1670, < 6.0, and 0.5 ng g^− 1 lipid weight (lw) in white croaker (Genyonemus lineatus); 1860, 6.5, and 1.3 ng g^− 1 lw in shiner surfperch (Cymatogaster aggregata); 5500, 37.4, and 0.9 ng g^− 1 lw in eggs of double-crested cormorant (Phalacrocorax auritus); 770, 7.1, and 0.9 ng g^− 1 lw in harbor seal (Phoca vitulina) adults; and 330, 3.5, and < 0.1 ng g^− 1 lw in harbor seal (P. vitulina) pups. Two additional flame retardants, pentabromoethylbenzene (PBEB) and 1,2-bis(2,4,6 tribromophenoxy)ethane (BTBPE) were detected in sediments but with less frequency and at lower concentrations (median concentrations of 0.01 and 0.02 ng g^− 1 dw, respectively) compared to the other flame retardants. PBEB was also detected in each of the adult harbor seals and in 83% of the pups (median concentrations 0.2 and 0.07 ng g^− 1 lw, respectively). The flame retardants hexabromobenzene (HBB), decabromodiphenyl ethane (DBDPE), bis(2-ethylhexyl) tetrabromophthalate (TBPH), and 2-ethylhexyl 2,3,4,5-tetrabromobenzoate (TBB), were not detected in sediments and BTBPE, HBB and TBB were not detected in wildlife samples. Elevated concentrations of some flame retardants were likely associated with urbanization and Bay hydrodynamics. Compared to other locations, concentrations of PBDEs in Bay wildlife were comparable or higher, while concentrations of the alternatives were generally lower. This study is the first to determine concentrations of PBDE replacement products and other flame retardants in San Francisco Bay, providing some of the first data on the food web occurrence of these flame retardants in a North American urbanized estuary.     

Levels and congener profiles of polybrominated diphenyl ethers (PBDEs) in breast milk from Shanghai: Implication for exposure route of higher brominated BDEs

Breast milk has been widely used as a bioindicator to assess the extent of human exposure to PBDEs via various exposure routes. In this study, 48 breast milk samples were collected from primiparous women in Shanghai city, and 14 PBDEs congeners (BDE-28, − 47, − 99, − 100, − 153, − 154, − 183, − 196, − 197, − 203, − 206, − 207, − 208, and − 209) were quantified using gas chromatography-electron capture negative ionization-mass spectrometry. The mean concentration of total PBDEs was 8.6 ng/g lipid weight, and ranged from 1.8 to 26.7 ng/g lipid weight. These concentration levels were similar to those reported in Europe and Asia, but one order of magnitude lower than those in North America. The congener profiles in this study exhibited a specific pattern in human milk found worldwide, BDE-153 and BDE-28 accounted for a relatively higher proportion of lower brominated BDEs (from tri- to hepta-BDEs), whereas higher brominated BDEs (from octa- to deca-BDEs) contributed more than 70% of the total PBDEs. The Spearman's correlation coefficient among higher brominated BDEs showed a positive relationship, and concentration levels of higher brominated BDEs were statistically different between office workers and housewives. Due to relatively higher proportion of PBDEs from octa- to deca-BDEs were detected, air inhalation and dust ingestion might be the major exposure routes of higher brominated BDEs. Further research is needed to clarify the major exposure route of higher brominated BDEs to humans.     

The occurrence of perfluorinated alkyl compounds in human milk from different regions of China

Perfluorinated compounds (PFCs), especially perfluorooctanesulfonate (PFOS) and perfluorooctanoate (PFOA), are known to occur throughout the environment and in the human population (Houde et al., 2006). The occurrence of PFCs in human umbilical cord blood and human milk, coupled with the potential developmental toxicity of PFCs, suggests the need for determining the exposure sources and magnitudes of PFCs in infants. In this study, 10 PFCs were measured in 24 pooled samples consisting of 1237 individual human milk samples. The samples were collected from 12 provinces of China in 2007. PFOS and PFOA were the predominant PFCs found in all the samples tested. The geometric mean (GM) and median of the concentrations were 46 pg/mL and 49 pg/mL for PFOS, 46 pg/mL and 34.5 pg/mL for PFOA respectively. A large variation in geographical distribution was observed for PFCs in human milk. High concentrations of PFOA (814 pg/ml for the rural samples and 616 pg/ml for the urban samples) were found in human milk from Shanghai. Estimated dietary intakes (EDI) were established and the median, GM and the highest EDI of the total PFCs were 17.2 ng/kg/d, 17.8 ng/kg/d and 129.1 ng/kg/d respectively. The EDI for PFOA (88.4 ng/kg/d) for Shanghai was close to the tolerable daily intake (100 ng/kg/d) proposed by the German Federal Institute for Risk Assessment and the Drinking Water Commission. The results suggest both mothers and infants have a high exposure to PFCs in the Shanghai region. The potential health impact of postnatal exposure through breastfeeding to infants should therefore be comprehensively evaluated.     

Concentrations of polybrominated diphenyl ethers in matched samples of indoor dust and breast milk in New Zealand

Polybrominated diphenyl ethers (PBDEs) are present in many consumer goods. There is evidence that PBDEs are toxic to humans, particular young children. The purpose of this study was to assess indoor dust as an exposure source for PBDEs. Concentrations of 16 PBDEs were determined in dust samples from 33 households in New Zealand, and in breast milk samples from 33 mothers living in these households. Associations between dust and breast milk PBDE concentrations were assessed, and children's PBDE intake from breast milk and dust estimated. Influences of household and demographic factors on PBDE concentrations in dust were investigated. Indoor dust concentrations ranged from 0.1 ng/g for BDE17 to 2500 ng/g for BDE209. Breast milk concentrations were positively correlated (p < 0.05) with mattress dust concentrations for BDE47, BDE153, BDE154, and BDE209 and with floor dust for BDE47, BDE183, BDE206, and BDE209. The correlation for BDE209 between dust and breast milk is a novel finding. PBDE concentrations in floor dust were lower from households with new carpets. The estimated children's daily intake of PBDEs from dust and breast milk was below U.S. EPA Reference Dose values. The study shows that dust is an important human exposure source for common PBDE formulations in New Zealand.     

Halogenated flame retardants in home-produced eggs from an electronic waste recycling region in South China: Levels,composition profiles,and human dietary exposure assessment

Three regulated halogenated flame retardants (HFRs), i.e., polybrominated diphenyl ethers (PBDEs), polybrominated biphenyls (PBBs) and hexabromocyclododecanes (HBCDs), and several alternative HFRs (AHFRs) including Dechlorane Plus (DP), decabromodiphenyl ethane (DBDPE), and 1,2-bis(2,4,6-tribromophenoxy) ethane (BTBPE), were investigated in the home-produced eggs from three recycling sites and a reference site in an electronic waste (e-waste) recycling region, South China. Mean levels of HFRs in eggs from the recycling sites ranged 2640–14 100, 700–1620, 44–350, and 720–3920 ng/g lipid weight for ∑PBDEs, ∑PBBs, ∑HBCDs, and ∑AHFRs, respectively, which were one to two orders of magnitude higher than those examined in the reference site. PBDEs were the predominant HFR in those eggs, with contributions > 50% to the total HFRs; followed by PBBs and the AHFRs (contributing 14–22% in average). The α-HBCD was the predominant diastereoisomers of HBCDs, with preferential enrichment of the (−)-enantiomer in most of the eggs; but no significant stereoselective enrichment of the DP isomers was observed in these eggs. The average estimated daily intakes (EDIs) of PBDEs, PBBs, HBCDs, and the AHFRs via eggs from the recycling sites ranged 4200–20 000, 1120–2440, 80–490, and 970–4530 ng/day, respectively, which were one to two orders of magnitude higher than those reported from other parts of the world. The potential adverse effects of these HFRs to human health in the e-waste sites should be further investigated. This is the first report on the isomer compositions of DP and the chiral signatures of HBCDs in hen eggs.     

Dietary intake of polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs) from fish and meat by residents of Nanjing,China

Concentrations of 14 polybrominated diphenyl ether (PBDEs) and 28 polychlorinated biphenyl (PCBs) congers were measured in 137 samples of fish and meat from Nanjing, a city in the Yangtze River Delta, China. Total concentrations of PBDEs were less in fish (mean of 180 pg/g ww; range 8.0–1100 pg/g ww), but more in non fish foods (mean of 180 pg/g ww; range 15–950 pg/g ww) than those reported from other countries. The total dietary intake of PBDEs and PCBs by humans were 9.9 ng PBDE/d and 870 ng PCB/d, respectively. The daily intake by a 60 kg adult of 2,3,7,8-tetrachlorodibenzo-p-dioxin equivalents (TEQ_WHO) from PCBs was estimated to be 49 pg ^PCBTEQ_WHO/d (0.82 pg ^PCBTEQ_WHO/kg bw), which is less than the tolerable daily intake suggested by the World Health Organization (WHO). The daily intake of meat and fish accounted for 57.2% and 42.8% of the total intake of ^PCBTEQ_WHO.     

Concentrations of polybrominated diphenyl ethers (PBDEs) in matched samples of human milk,dust and indoor air

Polybrominated diphenyl ethers (PBDEs) are lipophilic, persistent pollutants found worldwide in environmental and human samples. Exposure pathways for PBDEs remain unclear but may include food, air and dust. The aim of this study was to conduct an integrated assessment of PBDE exposure and human body burden using 10 matched samples of human milk, indoor air and dust collected in 2007–2008 in Brisbane, Australia. In addition, temporal analysis was investigated comparing the results of the current study with PBDE concentrations in human milk collected in 2002–2003 from the same region.PBDEs were detected in all matrices and the median concentrations of BDEs -47 and -209 in human milk, air and dust were: 4.2 and 0.3 ng/g lipid; 25 and 7.8 pg/m³; and 56 and 291 ng/g dust, respectively. Significant correlations were observed between the concentrations of BDE-99 in air and human milk (r = 0.661, p = 0.038) and BDE-153 in dust and BDE-183 in human milk (r = 0.697, p = 0.025). These correlations do not suggest causal relationships — there is no hypothesis that can be offered to explain why BDE-153 in dust and BDE-183 in milk are correlated. The fact that so few correlations were found in the data could be a function of the small sample size, or because additional factors, such as sources of exposure not considered or measured in the study, might be important in explaining exposure to PBDEs. There was a slight decrease in PBDE concentrations from 2002–2003 to 2007–2008 but this may be due to sampling and analytical differences. Overall, average PBDE concentrations from these individual samples were similar to results from pooled human milk collected in Brisbane in 2002–2003 indicating that pooling may be an efficient, cost-effective strategy of assessing PBDE concentrations on a population basis.The results of this study were used to estimate an infant's daily PBDE intake via inhalation, dust ingestion and human milk consumption. Differences in PBDE intake of individual congeners from the different matrices were observed. Specifically, as the level of bromination increased, the contribution of PBDE intake decreased via human milk and increased via dust. As the impacts of the ban of the lower brominated (penta- and octa-BDE) products become evident, an increased use of the higher brominated deca-BDE product may result in dust making a greater contribution to infant exposure than it does currently.To better understand human body burden, further research is required into the sources and exposure pathways of PBDEs and metabolic differences influencing an individual's response to exposure. In addition, temporal trend analysis is necessary with continued monitoring of PBDEs in the human population as well as in the suggested exposure matrices of food, dust and air.     

Historical intake and elimination of polychlorinated biphenyls and organochlorine pesticides by the Australian population reconstructed from biomonitoring data

Quantifying the competing rates of intake and elimination of persistent organic pollutants (POPs) in the human body is necessary to understand the levels and trends of POPs at a population level. In this paper we reconstruct the historical intake and elimination of ten polychlorinated biphenyls (PCBs) and five organochlorine pesticides (OCPs) from Australian biomonitoring data by fitting a population-level pharmacokinetic (PK) model. Our analysis exploits two sets of cross-sectional biomonitoring data for PCBs and OCPs in pooled blood serum samples from the Australian population that were collected in 2003 and 2009. The modeled adult reference intakes in 1975 for PCB congeners ranged from 0.89 to 24.5 ng/kg bw/day, lower than the daily intakes of OCPs ranging from 73 to 970 ng/kg bw/day. Modeled intake rates are declining with half-times from 1.1 to 1.3 years for PCB congeners and 0.83 to 0.97 years for OCPs. The shortest modeled intrinsic human elimination half-life among the compounds studied here is 6.4 years for hexachlorobenzene, and the longest is 30 years for PCB-74. Our results indicate that it is feasible to reconstruct intakes and to estimate intrinsic human elimination half-lives using the population-level PK model and biomonitoring data only. Our modeled intrinsic human elimination half-lives are in good agreement with values from a similar study carried out for the population of the United Kingdom, and are generally longer than reported values from other industrialized countries in the Northern Hemisphere.     

Biomagnification of naturally-produced methoxylated polybrominated diphenyl ethers (MeO-PBDEs) in harbour seals and harbour porpoises from the Southern North Sea

Harbour seals and harbour porpoises are top predator species from the North Sea, have long life spans and hence, are known to accumulate high levels of anthropogenic contaminants. To gain knowledge about the behaviour of naturally-produced compounds in these marine mammals, the biomagnification of naturally-produced methoxylated polybrominated diphenyl ethers (MeO-PBDEs) was assessed. The biomagnification of MeO-PBDEs (2′-MeO-BDE 68 and 6-MeO-BDE 47) was lower in harbour seals (all biomagnification factors (BMFs) < 1) compared to the same age–gender groups of the harbour porpoises (all BMFs > 1). This may indicate a better metabolic breakdown of MeO-PBDEs in harbour seals, as was previously suggested for polybrominated diphenyl ethers (PBDEs). In both predators, 6-MeO-BDE 47 had the highest concentrations (range: 45–483 ng/g lw and 2–38 ng/g lw for harbour porpoises and seals, respectively) compared to 2′-MeO-BDE 68 (range: 2–28 ng/g lw and 1–6 ng/g lw for harbour porpoises and seals, respectively). In general, the highest concentrations were found in juveniles, suggesting an increased biotransformation capacity with age or the influence of dilution by growth for both species. Here we show that naturally-produced brominated organic compounds can biomagnify and accumulate in North Sea top predators, although to a lesser extent than anthropogenic lipophilic contaminants, such as polychlorinated biphenyls (PCBs) or PBDEs.     

Polybrominated diphenyl ethers (PBDEs) in human samples of mother–newborn pairs in South China and their placental transfer characteristics

There are limited data concerning the placenta transfer characteristics and accumulation of polybrominated diphenyl ethers (PBDEs) in infants. However, PBDEs received increasing health concerns due to their endocrine disrupt and neurodevelopment toxicity effects. The present study assessed the accumulation of PBDEs in 30 paired placenta, breast milk, fetal cord blood, and neonatal urine samples collected from five major cities of the South China. The age of mothers ranged from 21 to 39 (mean 27.6 ± 4.56). The ∑ PBDE concentrations were 15.8 ± 9.88 ng g^− 1 lipid in placenta, 13.2 ± 7.64 ng g^− 1 lipid in breast milk, 16.5 ± 19.5 ng g^− 1 lipid in fetal cord blood, and 1.80 ± 1.99 ng ml^− 1 in neonatal urine. BDE-47 was the predominant congener in all types of human sample. Octa-BDEs such as BDE-196/-197 were detected highly in placenta and cord blood while moderately in breast milk and neonatal urine. Significant (p < 0.01) correlations were observed for both total and most individual PBDEs in cord blood–maternal placenta and breast milk–urine paired individual samples. The extent of placental transfer of higher brominated BDEs such as BDE-196/-197 was greater than that of BDE-47. The estimated daily intake (EDI) analysis for breast-fed infants revealed that newborns in these areas were exposed to relatively high levels of PBDEs via breast milk. Our study not only provided systematic fundamental data for PBDE distribution but also revealed the placenta transfer characteristics of PBDE congeners in South China.     

Levels and profiles of PCDD/Fs,PCBs in mothers' milk in Shenzhen of China: Estimation of breast-fed infants’ intakes

Sixty breast milk samples were collected in Shenzhen, China from July to November in 2007. The samples were analyzed of the concentrations of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs) and polychlorinated biphenyls (PCBs). The range of upper-bound for ∑ TEQ-(PCDD/Fs + PCBs) in the samples was 4.10–35.3 pg TEQ g^− 1 lipid (median: 10.6 pg TEQ g^− 1 lipid; mean: 11.9 pg TEQ g^− 1 lipid). The levels of the measured contaminants in the breast milk had significant correlations with the length of inhabitation period in Shenzhen (r = 0.487, p < 0.05 for PCDD/Fs, r = 0.431, p < 0.05 for PCBs and r = 0.478, p < 0.05 for ∑ TEQ-(PCDD/Fs + PCBs)), and the consumption rate of fish (r = 0.366, p < 0.05 for PCDD/Fs, r = 0.486, p < 0.05 for PCBs and r = 0.416, p < 0.05 for ∑ TEQ-(PCDD/Fs + PCBs)), respectively. Moreover, significant positive correlations were also detected between the participant's age (r = 0.305, p < 0.05 for ∑ TEQ-PCBs and r = 0.275, p < 0.05 for ∑ TEQ-(PCDD/Fs + PCBs)) and the body burdens of these contaminants respectively. It is estimated that the daily intake (EDI) of the sum of PCDD/Fs and DL-PCBs by the breast-fed infants was 5.60–161 pg TEQ kg^− 1 bw per day (mean: 48.2 pg TEQ kg^− 1 bw per day; median: 42.2 pg TEQ kg^− 1 bw per day). The result showed that both the body burdens of PCDD/Fs and PCBs of the recruit population and the calculated EDI of the breast-fed infants were higher than those in the non-exposed areas in mainland China. This suggests that continuous surveillance on PCDD/Fs and PCBs levels in human milk is critical to more precisely evaluate the human health risk posed by the negative environmental impact in Shenzhen in the future.     

Probabilistic mercury multimedia exposure assessment in small children and risk assessment

ObjectivesEmissions of mercury in the environment have been decreasing for several years. However, mercury species are still found in different media (food, water, air and breast-milk). Due to mercury toxicity and typical behaviour in children, we have conducted a mercury exposure assessment in French babies, and small children aged 0 to 36 months.MethodConsumption and mercury concentration data were chosen for the exposure assessment. The Monte Carlo technique has been used to calculate the weekly exposure dose in order to integrate inter-individual variability and parameter uncertainty. Exposure values have been compared to toxicological reference values for health risk assessment.ResultsInorganic mercury median exposure levels ranged from 0.160 to 1.649 μg/kg of body weight per week (95th percentile (P95): 0.298–2.027 µg/kg bw/week); elemental mercury median exposure level in children was 0.11 ng/kg bw/week (P95: 28 ng/kg bw/week); and methylmercury median exposure level ranged from 0.247 to 0.273 µg/kg bw/week (P95: 0.425–0.463 µg/kg bw/week). Only elemental mercury by inhalation route (indoor air) and methylmercury by ingestion (fish and breast-milk) seem to lead to a health risk in small children.ConclusionsThese results confirm the importance of assessing total mercury concentration in media like breast-milk, indoor air and dust and methylmercury level in food, other than fish and seafood. In this way, informed monitoring plan and risk assessment in an at-risk sub-population can be set.     

Distribution of persistent organic pollutants in two different fat compartments from obese individuals

There are only few studies defining persistent organic pollutant (POP) concentrations in various fat compartments from living obese individuals. The present study has therefore determined the concentrations of various classes of organohalogenated compounds, such as dichlorodiphenyltrichloroethane and its metabolites (DDTs), chlordane compounds (CHLs), hexachlorocyclohexanes (HCHs), hexachlorobenzene (HCB), polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs) and hexabromocyclododecanes (HBCDs) in visceral fat (VF: n = 52) and subcutaneous abdominal fat (SF: n = 52) samples collected in 2010–2012 from obese individuals in Belgium. Organohalogen compounds were detected in all fat samples in the decreasing order of their concentrations: PCBs > DDTs > HCHs > CHLs > HCB > HBCDs > PBDEs, suggesting that Belgians have been widely exposed to these contaminants. The levels and the patterns of POP distribution in VF and SF tissue depots were not significantly different. Concentrations of PCBs (VF/SF; median: 285/275 ng/g lw) and DDTs (VF/SF; median: 150/155 ng/g lw) were the major POPs in all fat samples. Concerning PCBs, PCB 153 (VF/SF: 27/26%) was the most dominant congener, followed by PCB 180 (VF/SF: 17/18%), PCB 138 (VF/SF: 15/14.5%) and PCB 170 (VF/SF: 8.1/8.4%) to the sum PCBs, respectively. Levels of HBCDs (VF/SF; median: 4.0/3.7 ng/g lw) and PBDEs (VF/SF; median: 2.6/2.7 ng/g lw) were 1–2 orders of magnitude lower than those of PCBs and DDTs. Among PBDEs, BDE 153 (VF/SF: 31/34%) was the dominant congener, followed by BDE 47 (VF/SF: 26/23%), BDE 154 (VF/SF: 16/16%), BDE 100 (VF/SF: 10/11%) and BDE 99 (VF/SF: 9/9%). To our knowledge, this is the first report on HBCD concentrations in Belgian human fat tissues. Total PBDE and HBCD levels in human fat samples could not be correlated with age. In agreement with the literature, a significant correlation (p < 0.05) between age and the concentration of PCBs (r = 0.828), DDTs (r = 0.640), HCHs (r = 0.666), CHLs (r = 0.534) and HCB (r = 0.754), was observed in the present study. Levels of DDTs, HCHs, HCB and CHLs were also significantly correlated to each other, suggesting that they share similar exposure routes. Correlation with computed tomography (CT) scan data revealed that VF and VF/SF ratios are positive for most of the POPs, such as PCBs, PBDEs, p,p′DDE, CHLs, β-HCH, and HCB. To our knowledge, this study is the first to assess the relationship between POP levels in adipose tissue and markers of abdominal adiposity, determined by CT.