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.     

Novel brominated flame retardants in food composites and human milk from the Chinese Total Diet Study in 2011: Concentrations and a dietary exposure assessment

On the basis of the fifth Chinese total diet study (TDS) performed in 2011, the dietary exposure of the Chinese population to novel brominated flame retardants (NBFRs) was assessed. Six NBFRs were determined in 80 composite samples from four animal origin food groups and 29 pooled human milk samples. Based on gas chromatography-negative chemical ionization mass spectrometry (GC-NCI/MS) analysis, the levels of the total NBFRs ranged from < LOD to 70.2 ng/g lipid weight (lw) in food composites and from 2.48 to 23.9 ng/g lw in human milk samples. Decabromodiphenyl ethane (DBDPE), with mean levels of 9.03 ng/g lw in food composites and 8.06 ng/g lw in human milk, was the most abundant compound in the total NBFRs. No obvious spatial distribution patterns in China were observed in food samples or human milk. The average estimated daily intake (EDI) of total NBFRs via food consumption for a “standard Chinese man” was 4.77 ng/kg bodyweight (bw)/day, with a range of 0.681 to 18.9 ng/kg bw/day. Meat and meat products were the main dietary source of NBFRs, although levels of NBFRs in aquatic food were found to be the highest among the four food groups. The average EDI of total NBFRs for nursing infants was 38.4 ng/kg bw/day, with a range of 17.4 to 113 ng/kg bw/day, which was approximately eight-fold higher than the EDI for adults, suggesting the heavy body burden of NBFRs on nursing infants. The levels and EDI of DBDPE in the present study were similar to or higher than those of legacy BFRs (i.e., PBDEs and HBCD) in the TDS 2007, indicating that DBDPE, as a main alternative to PBDEs, might have become the primary BFR used in China.     

Pharmacokinetics of bisphenol A in humans following a single oral administration

BackgroundHuman exposures to bisphenol A (BPA) are widespread. The current study addresses uncertainties regarding human pharmacokinetics of BPA.ObjectiveTo reduce uncertainties about the metabolism and excretion of BPA in humans following oral administration.MethodsWe exposed six men and eight women to 100 μg/kg bw of deuterated BPA (d6-BPA) by oral administration and conducted blood and urine analysis over a three day period. The use of d6-BPA allowed administered d6-BPA to be distinguished from background native (unlabeled) BPA. We calculated the rate of oral absorption, serum elimination, half-life, area under the curve (AUC), urinary excretion, and metabolism to glucuronide and sulfate conjugates.ResultsMean serum total (unconjugated and conjugated) d6-BPA C_max of 1711 nM (390 ng/ml) was observed at T_max of 1.1 ± 0.50 h. Unconjugated d6-BPA appeared in serum within 5–20 min of dosing with a mean C_max of 6.5 nM (1.5 ng/ml) observed at T_max of 1.3 ± 0.52 h. Detectable blood levels of unconjugated or total d6-BPA were observed at 48 h in some subjects at concentrations near the LOD (0.001–0.002 ng/ml). The half-times for terminal elimination of total d6-BPA and unconjugated d6-BPA were 6.4 ± 2.0 h and 6.2 ± 2.6 h, respectively. Recovery of total administered d6-BPA in urine was 84–109%. Most subjects (10 of 14) excreted > 90% as metabolites within 24 h.ConclusionsUsing more sensitive methods, our study expands the findings of other human oral pharmacokinetic studies. Conjugation reactions are rapid and nearly complete with unconjugated BPA comprising less than 1% of the total d6-BPA in blood at all times. Elimination of conjugates into urine largely occurs within 24 h.     

Daily intake of bisphenol A and triclosan and their association with anthropometric data,thyroid hormones and weight loss in overweight and obese individuals

Bisphenol A (BPA) and triclosan (TCS) were determined in urine of Belgian overweight and obese (n = 151) and lean (n = 43) individuals. After the first urine collection (0 M), obese patients started a diet program or have undergone bariatric surgery. Hereafter, three additional urine samples from obese patients were collected after 3 (3 M), 6 (6 M) and 12 (12 M) months. Both compounds were detected in > 99% of the samples. BPA had median concentrations of 1.7 and 1.2 ng/mL in obese and lean groups, respectively, while TCS had median concentrations of 1.5 and 0.9 ng/mL in the obese and lean groups, respectively. The obese group had higher urinary concentrations (ng/mL) of BPA (p < 0.5), while no significant differences were found for TCS between the obese and lean groups. No time trends between the different collection moments were observed. The BPA concentrations in the obese group were negatively associated with age, while no gender difference or relationship with body mass index was observed. For TCS, no relationships with gender, BMI, or age were found. The temporal variability of BPA and TCS was assessed with calculation of the intraclass correlation coefficient, Spearman rank correlation coefficients, and surrogate category analysis. We observed evidence that single spot urine samples might be predictive of exposure over a longer period of time. Dietary intakes of BPA and TCS did not differ significantly among the time points considered after obese individuals started losing weight (6 and 12 months). Multiple linear regression analyses after adjusting for age and weight loss revealed negative associations between urinary TCS and serum FT4 in the 0 M and 3 M female obese individuals and positive associations between urinary BPA and serum TSH in the lean group.     

Perfluoroalkyl substances in soft tissues and tail feathers of Belgian barn owls (Tyto alba) using statistical methods for left-censored data to handle non-detects

Perfluoroalkyl substances (PFASs) were investigated in tail feathers and soft tissues (liver, muscle, preen gland and adipose tissue) of barn owl (Tyto alba) road-kill victims (n = 15) collected in the province of Antwerp (Belgium). A major PFAS producing facility is located in the Antwerp area and levels of PFASs in biota from that region have been found to be very high in previous studies. We aimed to investigate for the first time the main sources of PFASs in feathers of a terrestrial bird species. Throughout this study, we have used statistical methods for left-censored data to cope with levels below the limit of detection (LOD), instead of traditional, potentially biased, substitution methods.Perfluorooctane sulfonate (PFOS) was detected in all tissues (range: 11 ng/g ww in muscle–1208 ng/g ww in preen oil) and in tail feathers (< 2.2–56.6 ng/g ww). Perfluorooctanoate (PFOA) was measured at high levels in feathers (< 14–670 ng/g ww), but not in tissues (more than 50% < LOD). Perfluorohexane sulfonate (PFHxS) could only be quantified in liver and preen oil, while other PFASs were sporadically detected in liver. PFOS levels in feathers and liver were highly correlated (r = 0.78, p < 0.01), in contrast to PFOA (r = − 0.11, p = 0.78). Combined with high PFOA levels in feathers this suggests that PFOA may be present on the external surface of feathers, due to external contamination originating from the air in the vicinity of point sources. Therefore the possibility of using feathers as a passive air sampler for high PFOA levels should be investigated in the future.     

The contribution of diet to total bisphenol A body burden in humans: Results of a 48 hour fasting study

Human biomonitoring studies measuring bisphenol A (BPA) in urine have shown widespread exposure in the general population. Diet is thought to be a major route of exposure. We studied urinary BPA patterns in five individuals over a 48-h period of fasting (bottled water only). Personal activity patterns were recorded with a diary to investigate non-dietary routes of exposure. All urine void events during the fast were collected, as well as events before and after the fast. The pattern of BPA concentrations was similar for all participants: they rose near the beginning of the fast (after the pre-fast meal), declined over the next 24 h, fluctuated at lower levels during the second day, and then rose after the post-fast meal. Concentrations (~ 2 μg/g creatine) and calculated BPA intakes (~ 0.03 μg/kg-day) in these individuals during the first 24 h were consistent with general population exposures. For the second 24 h, concentrations and intakes declined by about two-thirds. One of the individuals had an extraordinary pre-fast exposure event with concentrations rising as high as 98 μg/g creatine but declining to < 5 μg/g creatine by day 2. Given patterns found in day 1 and the subsequent decline to lower levels in day 2, we hypothesize that BPA exposures in these individuals were diet-driven. No events in the diary (use of personal care products, e.g.) appear associated with exposures. On day 2, non-dietary sources may still be present, such as from dust. Another hypothesis is that small reservoirs of BPA from past exposures are released from storage (lipid reservoirs, e.g.) and excreted.     

Maternal urinary bisphenol A levels and infant low birth weight: A nested case–control study of the Health Baby Cohort in China

BackgroundExposure to bisphenol A (BPA), a known endocrine disruptor, has been demonstrated to affect fetal development in animal studies, but findings in human studies have been inconsistent.ObjectivesWe investigated whether maternal exposure to BPA during pregnancy is associated with an increased risk of infant low birth weight (LBW).MethodsA total 452 mother-infant pairs (113 LBW cases and 339 matched controls) were selected from the participants enrolled in the prospective Health Baby Cohort (HBC) in Wuhan city, China, during 2012–2014. BPA concentrations were measured in maternal urine samples collected at delivery, and the information of birth outcomes was retrieved from the medical records. A conditional logistic regression was used to evaluate the relationship between urinary BPA levels and LBW.ResultsMothers with LBW infants had significantly higher urinary BPA levels (median: 4.70 μg/L) than the control mothers (median: 2.25 μg/L) (p < 0.05). Increased risk of LBW was associated with higher maternal urinary levels of BPA [adjusted odds ratio (OR) = 3.13 for the medium tertile, 95% confidence interval (CI): 1.21, 8.08; adjusted OR = 2.49 for the highest tertile, 95% CI: 0.98, 6.36]. The association was more pronounced among female infants than among male infants, with a statistical evidence of heterogeneity in risk (p = 0.03).ConclusionsPrenatal exposure to higher levels of BPA may potentially increase the risk of delivering LBW infants, especially for female infants. This is the first case–control study to examine the association in China.     

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.     

Determinants of urinary bisphenol A concentrations in Mexican/Mexican–American pregnant women

Prenatal exposure to bisphenol A (BPA) may be associated with adverse health effects in the developing fetus; however, little is known about predictors of BPA exposure during pregnancy. We examined BPA exposure in 491 pregnant women from the Center for the Health Assessment of Mothers and Children of Salinas (CHAMACOS) cohort and explored the role of living in the United States on significant dietary predictors of BPA exposure. Women provided urine samples up to two times during pregnancy (n = 866 total samples). We computed the intraclass correlation coefficient (ICC) to evaluate variability in concentrations between collections and used generalized estimating equation (GEE) models to assess predictors of exposure. Geometric mean (GSD) BPA concentrations were 0.9 (2.8) μg/L and 1.0 (2.6) μg/L at the first and second prenatal visits, respectively. We observed greater within- than between-woman variability in urinary BPA concentrations (ICC = 0.22). GEE models suggest that women who lived in the United States their entire life had 38% (CI: − 0.1, 89.3) higher urinary BPA concentrations compared with other immigrant women. Additionally, women who consumed ≥ 3 sodas per day or hamburgers three times a week or more had 58% (CI: 18.0, 112.1) and 20% (CI: − 0.2, 45.2) higher urinary BPA concentrations, respectively, compared with women who consumed no sodas or hamburgers. A higher percentage of women who lived their entire life in the United States reported increased consumption of sodas and hamburgers compared with other immigrant women. Independent of other factors, BPA urinary concentrations were slightly higher when the sample was collected later in the day. As in previous studies, high within-woman variability in urinary BPA concentrations confirms that several samples are needed to properly characterize exposure during pregnancy. Results also suggest that some factors could be modified to minimize exposures during pregnancy in our study participants (e.g., reducing soda and hamburger intake) and that factors associated with acculturation might increase BPA concentrations.     

Exposure assessment of adult intake of bisphenol A (BPA) with emphasis on canned food dietary exposures

Bisphenol A (BPA) is a high-volume, synthetic compound found in epoxy resins and plastics used in food packaging. Food is believed to be a major source of BPA intake. In this study, we measured the concentration of BPA in convenience samplings of foodstuffs purchased in Dallas, Texas. Sampling entailed collection of 204 samples of fresh, frozen, and canned foods in two rounds in 2010. BPA was positive in 73% of the canned food samples, while it was found in only 7% of non-canned foods at low concentrations. The results of this food sampling program were used to calculate adult dietary intakes of BPA. A pathway approach combined food intakes, a “canned fraction” parameter which described what portion of total intake of that food came from canned products, and measured food concentrations. Dietary intakes were calculated as 12.6 ng/kg-day, of which 12.4 ng/kg-day was from canned foods. Canned vegetable intakes alone were 11.9 ng/kg-day. This dietary intake was compared to total intakes of BPA estimated from urine measurements of the National Health and Nutrition Examination Survey (NHANES). Total adult central tendency intakes ranged from 30 to 70 ng/kg-day for NHANES cycles between 2005 and 2010. Three possibilities were explored to explain the difference between these two approaches for intake estimation. Not all foods which may have been canned, particularly canned beverages such as soft drinks, were sampled in our food sampling program. Second, non-food pathways of exposure may be important for adults, including thermal paper exposures, and dust and air exposures. Finally, our canned food concentrations may not be adequately representative of canned foods in the United States; they were found to be generally lower compared to canned food concentrations measured in six other worldwide food surveys including three in North America. Our finding that canned food concentrations greatly exceeded non-canned concentrations was consistent with other studies, and underscores the importance of canned foods in the overall exposure of adults of BPA.     

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.     

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.     

Levels of selected persistent organic pollutants in blood from delivering women in seven selected areas of São Paulo State,Brazil

Persistent organic pollutants (POPs) present in the living environment are thought to have detrimental health effects on the population, with pregnant women and the developing foetus being at highest risk. We report on the levels of selected POPs in maternal blood of 155 delivering women residing in seven regions within the São Paulo State, Brazil.The following selected POPs were measured in the maternal whole blood: 12 polychlorinated biphenyls (PCBs) congeners (IUPAC Nos. 99, 101, 118, 138, 153, 156, 163, 170, 180, 183, 187, 194); dichlordiphenyltrichloroethane p,p′-DDT, diphenyldichloroethylene p,p′-DDE and other pesticides such as hexachlorocyclohexanes (α-HCH, β-HCH, γ-HCH), hexachlorobenzene (HCB), chlordane derivatives cis-chlordane, trans-chlordane, oxy-chlordane, cis-nonachlor and trans-nonachlor.Statistical comparisons between regions were performed only on compounds having concentrations above LOD in 70% of the samples. PCB118 congener was found to be highest in the industrial site (mean 4.97 ng/g lipids); PCB138 congener concentration was highest in the Urban 3 site (mean 4.27 ng/g lipids) and congener PCB153 was highest in the industrial and Urban 3 sites with mean concentration of 7.2 ng/g lipids and 5.89 ng/g lipids respectively. Large differences in levels of p,p′-DDE between regions were observed with the Urban 3 and industrial sites having the highest concentrations of 645 ng/g lipids and 417 ng/g lipids, respectively; β-HCH was found to be highest in the Rural 1 site; the γ-HCH in Rural 1 and industrial; the HCB in the Rural 1 and industrial sites and oxy-chlordane and t-NC in the Rural 2 sites. An association between levels of some contaminants and maternal age and parity was also found.     

Dietary and sociodemographic determinants of bisphenol A urine concentrations in pregnant women and children

Bisphenol A (BPA) exposure during early life may have endocrine-disrupting effects, but the dietary and sociodemographic predictors of BPA exposure during pregnancy and childhood remain unclear. Our aim was to evaluate the correlations between, and sociodemographic and dietary predictors of, serial urinary BPA concentrations measured during pregnancy and childhood in a Spanish birth cohort study. BPA was measured in two spot urine samples collected from 479 women during the first and third trimester of pregnancy and in one urine sample from their 4-year old children (n = 130). Average dietary intakes were reported in food frequency questionnaires during the first and third pregnancy trimester and at age 4 years. Multivariate mixed models and linear regression models were used to estimate associations between sociodemographic and dietary factors and BPA concentrations. A small, but statistically significant correlation was found between serial maternal BPA concentrations measured during pregnancy (r = 0.17). Pregnant women who were younger, less-educated, smoked, and who were exposed to second-hand tobacco smoke (SHS) had higher BPA concentrations than others. BPA concentrations were also higher in children exposed to SHS. High consumption of canned fish during pregnancy was associated with 21% [GM ratio = 1.21; 95%CI 1.02, 1.44] and 25% [GM ratio = 1.25; 95%CI 1.05, 1.49] higher urinary BPA concentrations in the first and third pregnancy trimester, respectively, compared to the lowest consumption group. This study suggests that canned fish may be a major source of BPA during pregnancy in Spain, a country of high canned fish consumption. Further evaluation of specific BPA exposure sources in the sociodemographic group of younger women who smoke, are exposed to SHS, and have a low educational level is needed. Studies identifying sources of exposure would benefit from repeat BPA measurements and questionnaires specifically focused on dietary and packaging sources.     

Sorption of trihalomethanes in foods

Trihalomethanes (THMs, namely, CHCl₃, CHCl₂Br, CHClBr₂ and CHBr₃) are disinfection by-products that are present in drinking water. These toxic chemicals are also present in meat, dairy products, vegetables, baked goods, beverages and other foods, although information regarding their concentrations and origin is very limited. This study investigates sorption of THMs occurring during rinsing and cooking of foods and the significance of food as an exposure source.Initial estimates of THM uptake were measured in experiments representing rinsing with tap water at 25 C using nine types of food, and for cooking in tap water at 90 C for fourteen other foods. A subset of foods was then selected for further study over a range of THM concentrations (23.7–118.7 μg/l), temperatures (25 C and 90 C), food concentrations (0.2–1.4, food weight: water weight), and contact times (5–240 min). Data were analyzed using regression and exponential models, and diffusion models were used to help explain the trends of THM uptake.Among vegetables, sorbed THM concentrations at 25 C were 213 to 774 ng/g for CHCl₃, 53 to 609 ng/g for CHCl₂Br, and 150–845 ng/g for CHClBr₂. Meats at 90 C tended to have higher concentrations, e.g., 870–2634 ng/g for CHCl₃. Sorbed concentrations increased with contact time and THM concentration, and decreased with food concentration in rinsing tests (using spinach, iceberg-head lettuce and cauliflower) and cooking tests (using tomato, potato, beef and miso–tofu soup). For most foods, THM uptake was diffusion limited and several hours were needed to approach steady-state levels. Swelling, hydrolysis and other physical and chemical changes in the food can significantly affect sorption. Screening level estimates for CHCl₃ exposures, based on experimental results and typical food consumption patterns, show that uptake via foods can dominate that due to direct tap water consumption, suggesting the importance of sorption and the need for further evaluation of THM intake due to foods.     

Substantial decline of polychlorinated biphenyls serum levels 10 years after public health interventions in a population living near a contaminated site in Northern Italy

IntroductionPolychlorinated biphenyls (PCBs) are persistent pollutants classified among endocrine disruptors and human carcinogens. In an urban area in Northern Italy (Brescia), a chemical factory producing PCBs from 1938 to 1984 caused soil and food pollution. Since the discovering of the environmental pollution in the area in 2001, various public health interventions have been implemented to avoid human contamination.MethodsTwo independent surveys were carried out in 2003 and 2013 using the same study design and methods. A random sample of the adult general population living in four areas of the town with different soil contamination level was enrolled in both surveys. Investigation included serum levels of 24 PCB congeners and of other common clinical-chemical parameters and questions about residential and occupational history as well as current and past diet and consumption of locally produced food. 537 subjects were tested in the 2003 and 488 in the 2013 survey.ResultsTotal PCB serum levels showed a strong correlation with age (Spearman r = 0.71 in 2003 and r = 0.80 in 2013), but not with gender. Consumers of food produced in the most polluted area had higher total PCB serum levels (median 15.6 and 4.7 ng/ml in 2003 and 2013, respectively) than non-consumers (4.1 and 2.3 ng/ml) and consumers of food produced in non-polluted areas (6.5 and 1.9 ng/ml), with increasing trend of PCB serum levels with cumulative local food intake. PCB serum levels from 2003 to 2013 survey declined by around half in all age groups, especially among the youngest people. The total PCB reduction was found to be due to a combination of a birth cohort effect (− 41% every 10 years) and survey period effect (− 18% in 2013 versus 2003), with medium chlorinated CB congeners showing the most relevant reduction (− 30%) between the two surveys. High chlorinated CBs were more strongly associated with birth cohort (− 46% every 10 years): in the 2013 survey they represented 58% of total PCBs in 60–79 years old while they were 37% among the under 40s with a median value 20 times higher in the oldest than in the youngest (3.1 versus 0.16 ng/ml).ConclusionsPCBs serum levels declined from the 2003 to 2013 survey though they are still high in the elderly mainly because of past intake of locally produced contaminated food. Present findings suggest that PCBs food chain contamination and human absorption have been interrupted successfully in the area since discovery of the pollution in 2001.     

DDTs in mothers' milk,placenta and hair,and health risk assessment for infants at two coastal and inland cities in China

This study is a one of the very few investigating the dichloro-diphenyl-trichloroethanes (DDTs) (summation of o,p′-DDE, p,p′-DDE, o,p′-DDD, p,p′-DDD, o,p′-DDT, and p,p′-DDT) in multiple human matrices in mothers' milk, placenta and hair collected from residents from two coastal cities: Guiyu (GY) and Taizhou (TZ) and one inland city: Lin'an (LA). TZ (milk: 360 ± 319 ng/g lipid wt.) showed significantly higher concentrations of DDTs than those from LA (milk: 190 ± 131 ng/g lipid wt.), whereas, concentrations of DDTs in GY (milk: 305 ± 109 ng/g lipid wt.) were in between TZ and LA. In addition, levels of DDTs in the human tissues from TZ (placenta: 122 ± 109 ng/g lipid wt.; hair: 79.9 ± 215 ng/g dry wt.) were significantly higher than those from Lin'an (placenta: 49.2 ± 30.2 ng/g lipid wt.; hair: 10.8 ± 7.09 ng/g dry wt.). The above concentrations of DDTs in milk exceeded the Codex Maximum Residue Limits/Extraneous Maximum Residue Limits for milk (20 ng/g lipid wt. whole milk), indicating that the human milk samples were grossly polluted. The present study revealed that human specimens collected from the coastal city (TZ) were more contaminated with inland one (LA), based on the levels of DDTs contained in samples which may be due to the higher dietary exposure to DDTs via consumption of contaminated seafood. The estimated daily intakes of DDTs by GY, TZ and LA infants were 1.69 ± 1.86, 1.48 ± 0.79, and 0.95 ± 0.73 μg/kg body wt./day, respectively which did not exceed 10 μg/kg body wt./day, the provisional tolerable daily intake proposed by the Food and Agriculture Organization/World Health Organization.     

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.     

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.     

Measurement and health risk assessment of PM2.5, flame retardants,carbonyls and black carbon in indoor and outdoor air in kindergartens in Hong Kong

Indoor air pollution is closely related to children's health. Polybrominated diphenyl ethers (PBDEs) and dechlorane plus (DP) transmitted through indoor PM_2.5 and dust, along with carbonyl compounds and black carbon (BC) aerosol were analysed in five Hong Kong kindergartens. The results showed that 60% of the median PM_2.5 levels (1.3 × 10¹ to 2.9 × 10¹ μg/m³ for indoor; 9.5 to 8.8 × 10¹ μg/m³ for outdoor) in the five kindergartens were higher than the guidelines set by the World Health Organization (2.5 × 10¹ μg/m³). Indoor PM_2.5 mass concentrations were correlated with outdoor PM_2.5 in four of the kindergartens. The PBDEs (0.10–0.64 ng/m³ in PM_2.5; 0.30–2.0 × 10² ng/g in dust) and DP (0.05–0.10 ng/m³ in PM_2.5; 1.3–8.7 ng/g in dust) were detected in 100% of the PM_2.5 and dust samples. Fire retardant levels in the air were not correlated with the levels of dust in this study. The median BC concentrations varied by > 7-fold from 8.8 × 10² ng/m^− 3 to 6.7 × 10³ ng/m^− 3 and cooking events might have caused BC concentrations to rise both indoors and outdoors. The total concentrations of 16 carbonyls ranged from 4.7 × 10¹ μg/m³ to 9.3 × 10¹ μg/m³ indoors and from 1.9 × 10¹ μg/m³ to 4.3 × 10¹ μg/m³ outdoors, whilst formaldehyde was the most abundant air carbonyl. Indoor carbonyl concentrations were correlated with outdoor carbonyls in three kindergartens. The health risk assessment showed that hazard indexes (HIs) HIs of non-cancer risks from PBDEs and DPs were all lower than 0.08, whilst non-cancer HIs of carbonyl compounds ranged from 0.77 to 1.85 indoors and from 0.50 to 0.97 outdoors. The human intake of PBDEs and DP through inhalation of PM_2.5 accounted for 78% to 92% of the total intake. The cancer hazard quotients (HQs) of formaldehyde ranged from 4.5E − 05 to 2.1E − 04 indoors and from 1.9E − 05 to 6.2E − 05 outdoors. In general, the indoor air pollution in the five Hong Kong kindergartens might present adverse effects to children, although different schools showed distinct pollution levels, so indoor air quality might be improved through artificial measures. The data will be useful to developing a feasible management protocol for indoor environments.