Biomarkers of pesticide exposure and diabetes in the 1999–2004 National Health and Nutrition Examination Survey

The associations of 8 pesticides and pesticide metabolites with total diabetes (diagnosed and undiagnosed) and pre-diabetes (glycohemoglobin 5.7–6.4%) were evaluated using the National Health and Nutrition Examination Survey (NHANES), 1999–2004. Six of the pesticides were found to be associated with total diabetes in separate adjusted logistic regressions. These pesticides and pesticide metabolites were beta-hexachlorocyclohexane, p,p′-DDE, p,p′-DDT, oxychlordane, trans-nonachlor, and heptachlor epoxide. When the number of compounds elevated was tested, 4 or more, of the 6, elevated had an odds ratio of 4.99 (95% CI 1.97–12.61) compared to none elevated. When the 6 compounds were tested together in a single combined adjusted logistic regression only oxychlordane, a metabolite of chlordane, and heptachlor epoxide, a metabolite of heptachlor, were significantly associated with total diabetes. In the combined adjusted logistic regression, oxychlordane ≥ 14.5 ng/g lipid adjusted had an odds ratios of 1.90 (95% CI 1.09–3.32) compared to oxychlordane < 14.5 ng/g lipid adjusted, and heptachlor epoxide ≥ 14.6 ng/g lipid adjusted had an odds ratio of 1.70 (95% CI 1.16–2.49) compared to heptachlor epoxide < 14.6 ng/g lipid adjusted. Heptachlor epoxide and p,p′-DDT were significantly associated with pre-diabetes in separate adjusted logistic regressions. When these 2 compounds were tested together only heptachlor epoxide remained significantly associated with pre-diabetes. The evidence supporting the relationship between pesticides and pesticide metabolites, with diabetes, was strongest for heptachlor epoxide and oxychlordane, intermediate for p,p′-DDT, and least for beta-hexachlorocyclohexane, p,p′-DDE, and trans-nonachlor. Mirex and dieldrin were not associated with total diabetes or pre-diabetes.     

Chlorinated biphenyls and pesticides in migrating and resident seabirds from East and West Antarctica

The unhatched eggs of the following seabirds were analyzed to quantify PCBs, hexachlorobenzene (HCB), α-, β-, γ-, δ-hexachlorocyclohexanes (HCHs), o,p′ and p,p′ isomers of DDT, DDD and DDE: resident Adèlie (Pygoscelis adèliae, ADPE) and Emperor (Aptenodytes forsteri, EMPE) penguins, migrating snow petrel (Pagodroma nivea, SNPT) and South Polar skua (Catharacta maccormicki, SPSK) from the Ross Sea (East Antarctica); and migrating Brown skua (Catharacta antartica, BRSK) and resident ADPE from the Brainsfield Strait (West Antarctica). The general aims were to evaluate the contaminant accumulation in eggs of migrating and resident species in the two study areas, and to compare levels in penguins and skuas nesting in East and West Antarctica. PCB congener and HCH and DDT isomer profiles were also assessed. Comparisons were evaluated using seven PCB congeners (IUPAC nos. 28, 52, 101, 118 + 149, 138, 153, and 180), p,p′-DDE, ΣDDTs, and ΣHCHs. Higher contaminant concentrations were detected in migrating seabirds (South polar skua and brown skua) > sub-Antarctic species (snow petrel) > Antarctic species (penguins) from both the sampling sites, suggesting contamination events at lower latitudes for those birds migrating northward. HCHs showed the lowest concentrations in all species (from 0.03 ± 0.03 ng/g wet wt in SPSK to 1.81 ± 1.23 ng/g wet wt in ADPE from West Antarctica), and PCBs were the most abundant contaminants (from 4.34 ± 2.15 ng/g wet wt. in EMPE to 53.41 ± 19.61 ng/g wet wt. in brown skua). Among pesticides, it is relevant the detection of p,p′-DDT in Adèlie penguin from West Antarctica and in both species of skua; the detection of this pesticide can confirm its actual use in certain malaria-endemic countries from where it is transferred through the long range transport to the polar regions. Contaminants did not show any significant temporal trend during a ten year time span, from 1994/95 to 2004/05, in organisms collected in East Antarctica and they did not indicate any latitudinal gradient along the Ross Sea coasts.     

Toxicokinetics of dioxins and other organochlorine compounds in Japanese people: Association with hepatic CYP1A2 expression levels

Concentrations of persistent organochlorine compounds (OCs) including polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), and polychlorinated biphenyls (PCBs) in the liver and adipose tissue of Japanese cadavers were measured, and their toxicokinetics were examined in association with hepatic cytochrome P450 (CYP) 1A protein expression levels. Total 2,3,7,8-tetrachlorodibenzo-p-dioxin toxic equivalents (TEQs) were 66 ± 74 and 65 ± 57 pg/g lipid weight (mean ± S.D.) in the liver and adipose tissue, respectively. Total PCBs (sum of 62 congeners targeted), p,p′-dichlorodiphenyl-dichloroethylene (p,p′-DDE) and β-hexachlorocyclohexane (β-HCH) were detected at concentrations over 1 μg/g lipid in both tissues of some specimens. For most of the dioxin-like congeners, total PCBs, p,p′-DDE, oxychlordane, α- and β-HCH, hexachlorobenzene (HCB), and tris(4-chlorophenyl)methane (TCPMe), age-dependent increases in concentrations were found in the adipose tissue of males. No such age-dependent trend was observed in the liver, suggesting that there are different mechanisms underlying the hepatic concentrations of OCs. Immunoblot analyses indicated detectable expression of hepatic CYP1A2 protein, whereas no CYP1A1 protein was detected. The CYP1A2 expression levels were positively correlated with concentrations (on wet weight basis) of 2,3,4,7,8-P₅CDF, the dominant TEQ-contributed congeners in the liver, indicating the induction of this CYP. Hepatic CYP1A2 protein levels were strongly correlated with the liver to adipose concentration (L/A) ratios of PCDD/F congeners with more than 5 chlorine atoms. Together with higher concentrations of the congeners in the liver than in the adipose tissue, the observation on L/A ratios of highly chlorinated PCDD/Fs suggests that induced hepatic CYP1A2 protein is involved in their sequestration in this human population, as observed in model animals (rodents). Nonetheless, the magnitude of hepatic sequestration (L/A ratio) of PCDD/Fs in this human population was lower than in other mammals and birds, reported previously. This study emphasizes the fact that toxicokinetics of some OCs can be affected at least partly by CYP1A2 protein levels in humans. For the extrapolation of their toxicokinetics from model animals to humans, knowledge on the induction and sequestration potencies of CYP1A is necessary.     

Selective transfer of persistent organic pollutants and their metabolites in grey seals during lactation

Twenty grey seal (Halichoerus grypus) mother–pup pairs from the colony of the Isle of May (Scotland) were sampled at early and late lactation in order to study the transfer of polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs) and their metabolites (HO-PCBs and HO-PBDEs) as well as organochlorine pesticides (OCPs), such as DDT and metabolites (DDXs) and hexachlorobenzene (HCB). The transfer of the naturally produced MeO-PBDEs was also investigated. Generally, concentrations (on a lipid weight basis) of the sum of PCBs, PBDEs and DDXs tended to be higher in all tissues at late lactation (for maternal outer blubber ΣPCBs = 3860 ± 2091 ng/g, ΣPBDEs = 120 ± 74 ng/g and ΣDDXs = 559 ± 207 ng/g; for maternal inner blubber ΣPCBs = 4229 ± 3274 ng/g, ΣPBDEs = 148 ± 118 ng/g and ΣDDXs = 704 ± 353 ng/g; for maternal serum ΣPCBs = 1271 ± 796 ng/g, ΣPBDEs = 27 ± 16 ng/g and ΣDDXs = 242 ± 125 ng/g; for milk ΣPCBs = 1190 ± 747 ng/g, ΣPBDEs = 55 ± 36 ng/g and ΣDDXs = 357 ± 160 ng/g; for pup serum ΣPCBs = 1451 ± 901 ng/g, ΣPBDEs = 48 ± 31 ng/g and ΣDDXs = 395 ± 201 ng/g). In all tissues, ΣMeO-PBDEs were found at very low levels or even undetected and their concentrations appeared to increase at late lactation only in maternal inner blubber (2.7 ± 1.3 to 5.3 ± 2.9 ng/g for early and late lactation, respectively) and milk (0.6 ± 0.3 to 1.1 ± 0.5 ng/g for early and late lactation, respectively). The transfer from inner blubber to maternal serum was selective and strongly depended on the log K_ow value of the compounds, with less lipophilic compounds being more efficiently released. Only a limited amount of HO-PCBs was transferred during lactation as 4-HO-CB-107 was the only metabolite detected in milk (29 to 40 pg/g lw). On the contrary, most of HO-PCB metabolites found in maternal serum were also detected in pup serum. These findings suggest not only a transplacental transfer of HO-PCBs from mothers to pups but also the possibility of endogenous biotransformation in suckling pups or accumulation of undetectable low amounts from milk.     

Can starling eggs be useful as a biomonitoring tool to study organohalogenated contaminants on a worldwide scale?

Large-scale international monitoring studies are important to assess emission patterns and environmental distributions of organohalogenated contaminants (OHCs) on a worldwide scale. In this study, the presence of OHCs was investigated on three continents (Europe, North America and Australasia), using eggs of starlings (Sturnus vulgaris and Sturnus unicolor) to assess their suitability for large-scale monitoring studies. To the best of our knowledge, this is the first study using bird eggs of the same species as a biomonitor for OHCs on an intercontinental scale. We found significant differences in OHC concentrations of the eggs among sampling locations, except for hexachlorocyclohexanes (HCHs). Mean concentrations of sum polychlorinated biphenyls (PCBs) in eggs ranged from 78 ± 26 ng/g lipid weight (lw) in Australia to 2900 ± 1300 ng/g lw in the United States. The PCB profile was dominated by CB 153 and CB 138 in all locations, except for New Zealand, where the contribution of CB 95, CB 101 and CB 149 was also high. The highest mean sum polybrominated diphenyl ether (PBDE) concentrations were found in Canada (4400 ± 830 ng/g lw), while the lowest mean PBDE concentrations were measured in Spain (3.7 ± 0.1 ng/g lw). The PBDE profile in starling eggs was dominated by BDE 47 and BDE 99 in all countries, but in Belgium, the higher brominated PBDEs had a higher contribution compared to other countries. For the organochlorine pesticides (OCPs), dichlorodiphenyltrichloroethanes (DDTs) ranged from 110 ± 16 ng/g lw in France to 17,000 ± 3400 ng/g lw in New Zealand, while HCHs and hexachlorobenzene were generally in low concentrations in all sampling locations. Chlordanes were remarkably high in eggs from the United States (2500 ± 1300 ng/g lw). The OCP profile in all countries was largely dominated by p,p′-DDE. In general, the worldwide trends we observed in starling eggs were in accordance with the literature on human and environmental OHC data, which suggests that there is potential for using starling eggs as a biomonitoring tool on a large geographical scale.     

Polychlorinated dibenzo-p-dioxins/furans (PCDD/Fs), polychlorinated biphenyls (PCBs), and polybrominated diphenyl ethers (PBDEs) in breast milk from Zhejiang,China

Breast milk samples (n = 74) from the general maternal population of Zhejiang province were analyzed for polychlorinated dibenzo-p-dioxins/furans (PCDD/Fs), polychlorinated biphenyls (PCBs), and polybrominated diphenyl ethers (PBDEs). Samples were divided into urban and rural groups. Mean ∑PCDD/F, ∑PCB and ∑PBDE concentrations were 71.4 ± 40.8, 42774 ± 27841 and 2679 ± 944 pg g^− 1 lipid in the urban group and 38.6 ± 38.1, 26546 ± 11375 and 2731 ± 1093 pg g^− 1 lipid in the rural group, respectively. WHO-TEQ concentrations for dioxin-like PCBs and PCDD/Fs were 2.66 ± 1.43 and 3.90 ± 2.60 pg g^− 1 lipid in the urban group and 1.83 ± 0.93 and 2.27 ± 1.55 pg g^− 1 lipid in the rural group, respectively. Congener profiles for these pollutants were compared between human samples (adipose tissue and breast milk) and foodstuffs (seafood, hen eggs, and freshwater fish). Similar PCB and PCDD/F congener patterns were observed, suggesting that dietary intake is a significant source for human exposure to PCBs and PCDD/Fs. However, much lower PBDE congener levels were detected in breast milk than in foodstuffs, which implies that pathways other than dietary intake may also account for human exposure to PBDEs.     

Route-specific daily uptake of organochlorine pesticides in food,dust, and air by Shanghai residents,China

Dichlorodiphenyltrichloroethane (DDT) and hexachlorocyclohexanes (HCHs) are widely detected in the environment, although they have been banned in China since 1980s. To better understand the route-specific daily uptake of the pesticides by humans, a total of 322 food, dust, and air samples were collected in Shanghai, China, during 2008–2011. The median concentrations were 0.2–126.6 and 0.03–1.6 ng/g wet weight for DDTs (DDT and its metabolites) and HCHs, respectively, in different types of foods. The values in dust (indoors and outdoors) were 5.7–29.8 and 1.3–5.4 ng/g, and 13.9 × 10^− 3 and 2.6 × 10^− 3 ng/m³ in air (gas + particle) for DDTs and HCHs, respectively. The daily uptake of a pesticide by humans was calculated via the pesticide intake multiplied by its uptake efficiency. The uptake efficiencies of DDTs and HCHs in food through human intestines were estimated using bioaccessibility measured via an in vitro method simulating the human gastrointestinal digestion process. The total daily uptakes of DDTs and HCHs through three routes (i.e., ingestion, inhalation, and dermal contact) were 79.4 and 4.9 ng/day, respectively, for children, and 131.1 and 8.0 ng/day, respectively, for adults. Ingestion via food and dust was the main route of human exposure to the pesticides, and the daily uptake of the pesticides via food consumption accounted for 95.0–99.2% of the total.     

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.     

Analysis of human milk to assess exposure to PAHs,PCBs and organochlorine pesticides in the vicinity Mediterranean city Mersin,Turkey

Assessment of human exposure to environmental persistent organic pollutants such as organochlorine pesticides (OCPs), polychlorinated biphenyls (PCBs), polychlorinated dibenzo-p-dioxins/furans (PCDD/Fs) and polycyclic aromatic hydrocarbons (PAHs) based on the levels in human breast milk provides a reasonable tool not only to assess the contaminant burden in mothers but also to assess potential exposure of breast-fed neonates. There are limited data on levels of PCBs and OCPs in humans but no previous reports from Turkey on chemically determined levels PAHs in human milk. The aim of this study was to report the levels and accumulation profiles of OCPs, PCBs and PAHs in 47 breast milk samples obtained from a Mediterranean city, Mersin. High resolution analyses were performed by a gas chromatography coupled with mass spectrometer (GC–MS). Dichlorodiphenyldichloroethane (4.4′-DDE) was the dominant pollutant. Beta-hexachlorocyclohexane (ß-HCH), dichlorodiphenyltrichloroethane (4.4′-DDT), dieldrin, hexachlorobenzene, oxy-chlordane, cis-heptachlorepoxide were the other main OCPs detected. Mean levels of ΣPCB congeners and WHO_PCB-TEQ were 9.94 and 0.001 ng/g lipid, respectively. PCB 153 showed the highest concentration (3.37 ng/g lipid), followed by PCB 138 and 180. For the dioxin-like PCBs, PCB 118 was the dominant (0.97 ng/g lipid). Naphthalene, phenanthrene, pyrene and fluoranthene were the major PAHs among the 16 PAHs detected. The estimated daily intakes of DDTs, PCBs, HCHs and HCB were not exceeded the tolerable daily intake (TDI) proposed by the Health Canada Guideline. These results indicate that the neonates of Mersin city are exposed to persistent organic pollutants analyzed in this study. However, neonates born in Mersin province are less exposed than the ones born in other regions, considering OCP and PCB levels in breast milk.     

Hydroxylated PCB metabolites (OH-PCBs) in archived serum from 1950–60s California mothers: A pilot study

We are studying participants selected from the Child Health and Development Studies (CHDS), a longitudinal birth cohort of over 20,000 California pregnancies between 1959 and 1967, for associations between maternal body burden of organochlorine contaminants and thyroid function. We designed a pilot study using 30 samples selected among samples with high and low PCB concentrations to evaluate the feasibility of measuring OH-PCBs in the larger study population. GC-ECD and GC-NCI/MS were used to determine PCBs and OH-PCBs as methyl derivatives, respectively. Maternal serum levels of Σ₁₁PCBs and Σ₈OH-PCB metabolites varied from 0.74 to 7.99 ng/mL wet wt. with a median of 3.05 ng/mL, and from 0.12 to 0.98 ng/mL wet wt. with a median of 0.39 ng/mL, respectively. Average concentrations of Σ₈OH-PCB metabolites in the high PCB group were significantly higher than those in the low PCB group (p < 0.05). The levels of OH-PCB metabolites were dependent on PCB levels (r = 0.58, p < 0.05) but approximately an order of magnitude lower (p < 0.05). The average ratio of Σ₈OH-PCBs to Σ₁₁PCBs was 0.14 ± 0.08. The primary metabolite was 4-OH-CB187 followed by 4-OH-CB107. Both of these metabolites interfere with the thyroid system in in vitro, animal, and human studies. OH-PCBs were detectable in all archived sera analyzed, supporting the feasibility to measure OH-PCB metabolites in the entire cohort.     

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.     

The bioaccessibility of polychlorinated biphenyls (PCBs) and polychlorinated dibenzo-p-dioxins/furans (PCDD/Fs) in cooked plant and animal origin foods

In this study, we compared the effect of boiling and frying food preparation methods in determining the bioaccessibility of polychlorinated biphenyls (PCBs) and polychlorinated dibenzo-p-dioxins/furans (PCDD/Fs) in rice, cabbage, milk powder, eggs, beef, and fresh water fish. We then used these data to calculate a toxic equivalent (TEQ) for risk assessment and compared it to published values that did not account for bioaccessibility.When the foods were prepared by boiling, the mean bioaccessibility (%) in rice (PCBs: 16.5 ± 1.0, PCDD/Fs: 4.9 ± 0.3) and cabbage (PCBs: 4.2 ± 0.9, PCDD/Fs: 1.9 ± 0.7) were lower than in animal origin foods (beef, PCBs: 49.0 ± 3.3, PCDD/Fs: 7.8 ± 0.9; egg, PCBs: 29.7 ± 3.1, PCDD/Fs: 8.6 ± 1.3; fish, PCBs: 26.9 ± 2.5, PCDD/Fs: 7.9 ± 1.3; milk powder, PCBs: 72.3 ± 1.6, PCDD/Fs: 28.4 ± 1.2).When fried in cooking oil, the bioaccessibilities of all analytes in all foods increased, but the increase in plant based foods (rice, PCBs: 3.4 ×, PCDD/Fs: 3.6 ×; cabbage, PCBs: 10.3 ×, PCDD/Fs: 7.9 ×) was greater than that of animal origin foods (beef, PCBs: 1.6 ×, PCDD/Fs: 3.4 ×; egg, PCBs: 2.1 ×, PCDD/Fs: 1.8 ×; fish, PCBs: 2.8, PCDD/Fs: 3.2 ×).Comparison of PCBs/PCDD/Fs bioaccessibility in rice and cabbage showed that bioaccessibility was greater in the low fat, high carbohydrate/protein content food (rice) than in the low carbohydrate/protein, low fat content food (cabbage), regardless of the method used to prepare the food.Adjusting for bioaccessibility reduced the gross estimated daily intake (EDI) of 112 pg WHO-TEQ/day, by 88% and 63% respectively for foods prepared by boiling and frying.Our results indicate that: 1) The method used for cooking is an important determinant of PCBs/PCDD/Fs bioaccessibility, especially for plant origin foods, 2) there might be a joint fat, carbohydrate and protein effect that influences the bioaccessibilities of PCBs/PCDD/Fs in foods, and 3) use of bioaccessibility estimates would reduce the uncertainty in TEQ calculations.     

Mutagenic properties of PM2.5 urban pollution in the Northern Italy: The nitro-compounds contribution

PM2.5 is the breathable fraction of the particulate matter and some adverse health effects, such as respiratory functionality, cardiological diseases and cancer, can be in some measure attributable to this risk factor exposure. Some of the most carcinogen compounds transported by PM2.5 are nitro-compounds. In this study, a strengthened in vitro bioassay — able to predict the mutagenic/carcinogenic activity of the environmental mixtures — was conducted on PM2.5 organic extracts to define the nitro-compounds burden. PM2.5 air pollution was daily monitored, during 2006, in three cities located in the Northern part of Italy (Torino, Pavia and Verona) and the mutagenic properties of the PM2.5 organic extracts were assessed with the Ames test. The bacterial used in this study were three Salmonella typhimurium strains: TA98, nitroreductase-less mutant TA98NR and YG1021 carrying a nitroreductase-producing plasmid. The annual PM2.5 mean level measured in Torino was 46.5 (± 31.6) μg/m³, in Pavia 34.8 (± 25.1) μg/m³, and in Verona 37.3 (± 27.8) μg/m³, while the mutagenicity expressed as TA98 net reverants/m³ was 28.0 (± 22.1), 28.3 (± 24.9), and 34.2 (± 30.9) respectively. Monthly pool bioassays, conducted with the three different strains, showed a greater mutagenic response of the YG1021 in each city. The relationship among the mutagenic answers for YG1021:TA98:TA98NR was about 6:3:1 (p < 0.001). Over nitroreductase activity enhanced the response of 2.2, 2.0 and 1.7 times for Torino, Pavia, and Verona (ANOVA Torino p < 0.05) respectively. Without nitroreductase activity the genotoxicity was limited. These biological findings are able to describe a relevant role played by the nitro compounds in the mutagenic properties of the urban PM2.5 in the Padana plain; moreover the bacterial nitroreductase plays a predominant role in DNA interaction primarily for Torino PM2.5 extracts.     

Persistent organic pollutants in the Scheldt estuary: Environmental distribution and bioaccumulation

Levels of polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs) and organochlorine pesticides (OCPs) were determined in the sediment and several species (European flounder, Platichthys flesus; common sole, Solea solea; Chinese mitten crab, Eriocheir sinensis; shore crab, Carcinus maenas; brown shrimp, Crangon crangon; blue mussel, Mytilus edulis and bristle worms, Polychaeta) from 7 locations in the Scheldt estuary (SE, the Netherlands–Belgium). Overall POP levels in the sediment were low. The average PCB and PBDE concentrations were respectively 31.5 and 115 ng/g dry weight (dw). Highest sediment loads were measured in the vicinity of Antwerp (368 ng PCBs/g dw), a location with intense harbor and industrial activities. Pollution concentrations in the tissues of biota were species-specific. Blue mussels contained the highest lipid concentrations (2.74 ± 0.55%) and reached the highest contamination levels (from 287 to 1688 ng PCBs/g ww, from 2.09 to 12.4 ng PBDEs/g ww). Lowest tissue loads were measured in brown shrimp (from 3.27 to 39.9 ng PCBs/g ww, from 0.05 to 0.47 ng PBDEs/g ww). The PCB congener profile in most of the species was similar with the pattern found in the sediment. PCB 153 was the most abundant congener (16.5–25.7% in biota, 10.4% in sediment). In the sediment, the total amount of PBDEs consisted for more than 99% of BDE 209. Congener BDE 47 had the highest concentrations in all sampled species (38.5–70.1%). Sediment POP loadings and tissue concentrations were poorly correlated, indicating that a simple linear or non-linear relationship is insufficient to describe this relationship, possible caused by the complexity of the bioaccumulation processes and the variability in exposure. Because of the high PCB levels, regular consumption of fish and seafood, especially mussels, from the Scheldt estuary should be avoided.     

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.     

The bioavailability of selenium and risk assessment for human selenium poisoning in high-Se areas,China

Enshi prefecture of Hubei Province is well known for human selenium (Se) poisoning in the early 1960s in China. Sporadic cases of Se poisoning in livestocks are still being found. In this study, Se levels in water, cropland soils and various crops from high-Se areas of Enshi were measured to investigate the distribution and bioavailability of Se in the environments, as well as probable daily intake (PDI) of Se for local residents. The total Se in surface water ranged from 2.0 to 519.3 μg/L with a geometric mean of 46.0 ± 127.8 μg/L (n = 48), 70.5–99.5% of which was present in the form of Se(VI). The soil Se concentration varied from 2.89 to 87.3 μg/g with a geometric mean of 9.36 ± 18.6 μg/g (n = 45), and most of Se was associated with organic matter (OM-Se). The total Se in rice, corn, and vegetable samples were 2.11 ± 2.87 μg/g (n = 21), 3.76 ± 11.6 μg/g (n = 16), and 2.09 ± 3.38 μg/g (n = 25), respectively. Stream water Se is likely leached from carbonaceous shale and mine wastes, leading to Se accumulation in paddy soils. OM-Se may play an important role in Se uptake by rice plant in high-Se area of Enshi.The PDI of Se is approximately 2144 μg/day, and Se concentration in blood is estimated at about 3248 μg/L, posing a potential chronic Se poisoning risk to local residents. Cereal consumption (48.5%) makes a great contribution to human daily Se intake, followed by vegetables (36.6%), meats (8.5%), and drinking water (6.4%). However, when assessing health risk on human in high-Se areas, the contribution of drinking water to daily Se intake cannot be ignored due to high Se content and dominant Se(VI) species. Local inhabitants should be advised not to grow crops in high-Se lands or irrigate using high-Se water. If possible, they should drink pipe water and consume foods mixed with those from outside the high-Se areas.     

Comparing human exposure to emerging and legacy flame retardants from the indoor environment and diet with concentrations measured in serum

This study investigates associations between serum concentrations of emerging and legacy halogenated flame retardants (HFRs) in 46 Norwegian women and measured indoor air and dust concentrations of the HFRs as well as detailed information on diet and household factors. Hexabromobenzene (median 0.03 ng/g lipid) and Dechlorane 602 (median 0.18 ng/g lipid) were detected in about 50% of the samples and Dechlorane Plus syn (median 0.45 ng/g lipid) and anti (median 0.85 ng/g lipid) in more than 78%. The most abundant polybrominated diphenyl ethers were 2,2′,4,4′,5,5′-hexabromodiphenyl ether (BDE-153; median 0.82 ng/g lipid) and 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47; median 0.49 ng/g lipid) detected in more than 70% of the samples. In the bivariate analysis, no consistent associations were observed between the biomonitoring data and measured concentrations in indoor air and dust. On the other hand, consumption of specific food items (mainly lamb/mutton and margarine) correlated significantly with more than two HFR serum concentrations, while this was not the case for household factors (electronic appliances). Only the significant bivariate associations with diet were confirmed by multivariate linear regression analyses, which might indicate a higher contribution from food compared to the indoor environment to the variation of the body burden of these HFRs.     

Concentrations of polybrominated diphenyl ethers (PBDEs) and 2,4,6-tribromophenol in human placental tissues

Legacy environmental contaminants such as polybrominated diphenyl ethers (PBDEs) are widely detected in human tissues. However, few studies have measured PBDEs in placental tissues, and there are no reported measurements of 2,4,6-tribromophenol (2,4,6-TBP) in placental tissues. Measurements of these contaminants are important for understanding potential fetal exposures, as these compounds have been shown to alter thyroid hormone regulation in vitro and in vivo. In this study, we measured a suite of PBDEs and 2,4,6-TBP in 102 human placental tissues collected between 2010 and 2011 in Durham County, North Carolina, USA. The most abundant PBDE congener detected was BDE-47, with a mean concentration of 5.09 ng/g lipid (range: 0.12–141 ng/g lipid; detection frequency 91%); however, 2,4,6-TBP was ubiquitously detected and present at higher concentrations with a mean concentration of 15.4 ng/g lipid (range:1.31–316 ng/g lipid; detection frequency 100%). BDE-209 was also detected in more than 50% of the samples, and was significantly associated with 2,4,6-TBP in placental tissues, suggesting they may have a similar source, or that 2,4,6-TBP may be a degradation product of BDE-209. Interestingly, BDE-209 and 2,4,6-TBP were negatively associated with age (r_s = − 0.16; p = 0.10 and r_s = − 0.17; p = 0.08, respectively). The results of this work indicate that PBDEs and 2,4,6-TBP bioaccumulate in human placenta tissue and likely contribute to prenatal exposures to these environmental contaminants. Future studies are needed to determine if these joint exposures are associated with any adverse health measures in infants and children.     

Spatiotemporal analysis and human exposure assessment on polycyclic aromatic hydrocarbons in indoor air,settled house dust,and diet: A review

This review summarizes the published literature on the presence of polycyclic aromatic hydrocarbons (PAH) in indoor air, settled house dust, and food, and highlights geographical and temporal trends in indoor PAH contamination. In both indoor air and dust, ΣPAH concentrations in North America have decreased over the past 30 years with a halving time of 6.7 ± 1.9 years in indoor air and 5.0 ± 2.3 years in indoor dust. In contrast, indoor PAH concentrations in Asia have remained steady. Concentrations of ΣPAH in indoor air are significantly (p < 0.01) higher in Asia than North America. In studies recording both vapor and particulate phases, the global average concentration in indoor air of ΣPAH excluding naphthalene is between 7 and 14,300 ng/m³. Over a similar period, the average ΣPAH concentration in house dust ranges between 127 to 115,817 ng/g. Indoor/outdoor ratios of atmospheric concentrations of ΣPAH have declined globally with a half-life of 6.3 ± 2.3 years. While indoor/outdoor ratios for benzo[a]pyrene toxicity equivalents (BaP_eq) declined in North America with a half-life of 12.2 ± 3.2 years, no significant decline was observed when data from all regions were considered. Comparison of the global database, revealed that I/O ratios for ΣPAH (average = 4.3 ± 1.3), exceeded significantly those of BaP_eq (average = 1.7 ± 0.4) in the same samples. The significant decline in global I/O ratios suggests that indoor sources of PAH have been controlled more effectively than outdoor sources. Moreover, the significantly higher I/O ratios for ΣPAH compared to BaP_eq, imply that indoor sources of PAH emit proportionally more of the less carcinogenic PAH than outdoor sources. Dietary exposure to PAH ranges from 137 to 55,000 ng/day. Definitive spatiotemporal trends in dietary exposure were precluded due to relatively small number of relevant studies. However, although reported in only one study, PAH concentrations in Chinese diets exceeded those in diet from other parts of the world, a pattern consistent with the spatial trends observed for concentrations of PAH in indoor air. Evaluation of human exposure to ΣPAH via inhalation, dust and diet ingestion, suggests that while intake via diet and inhalation exceeds that via dust ingestion; all three pathways contribute and merit continued assessment.     

Selenium exposure in subjects living in areas with high selenium concentrated drinking water: Results of a French integrated exposure assessment survey

BackgroundSelenium is an essential element which can be toxic if ingested in excessive quantities. The main human exposure is food. In addition, intake may be boosted by consumption drinking water containing unusual high selenium concentration.ObjectiveWe measured the individual selenium level of people exposed to selenium concentration in drinking water greater than the maximum recommended limit which is 10 μg/L.MethodsWe carried out a prospective cohort study on 80 adults (40 exposed subjects i.e. living in the involved area and 40 non-exposed ones i.e. living elsewhere) in western France. We used three different approaches: (1) direct measurement of ingested selenium by the duplicate portion method, (2) dietary reconstitution with a food frequency questionnaire (FFQ) and (3) evaluation of the individual selenium status by measuring the selenium content in toenail clippings. Analyses were performed by inductively coupled plasma-mass spectrometry. The association between toenail selenium concentration and area of residence was analyzed using linear regression with repeated measurements.ResultsWe estimated selenium intake from FFQ at 64 ± 14 μg/day for exposed subjects as opposed to 52 ± 14 μg/day for the non-exposed ones. On the basis of 305 duplicate diet samples, average intake was estimated at 64 ± 26 μg/day for exposed subjects. Area of residence (p = 0.0030) and smoking (p = 0.0054) were independently associated with toenail selenium concentration.ConclusionWhatever method used for estimating selenium intake, the selenium level in this studied area with high selenium concentrated drinking water is much lower than in seleniferous areas.