Perfluoroalkyl substances and food allergies in adolescents

Perfluoroalkyl and polyfluoroalkyl substances (PFASs) are a class of organic compounds that are persistent in the environment due to their stable carbon-fluorine backbone, which is not susceptible to degradation. Research suggests these chemicals may exert an immunotoxic effect. The aim of this study is to investigate the associations between four PFASs – perfluorooctane sulfonic acid (PFOS), perfluorooctanoic acid (PFOA), perfluorononanoic acid (PFNA), and perfluorohexane sulfonic acid (PFHxS) – with food sensitization and food allergies in adolescent participants (ages 12–19 years) in the National Health and Nutrition Examination Survey (NHANES) 2005–2006 and 2007–2010, respectively. We performed multivariate logistic regression to analyze the association between individual PFASs with food sensitization (defined as having at least 1 food-specific IgE level ≥ 0.35 kU/L) in NHANES 2005–2006 and food allergies (self-reported) in NHANES 2007–2010. Serum PFOA, PFOS, and PFHxS were statistically significantly associated with higher odds to have self-reported food allergies in NHANES 2007–2010. When using IgE levels as a marker of food sensitization, we found that serum PFNA was inversely associated with food sensitization (NHANES 2005–2006). In conclusion, we found that serum levels of PFASs were associated with higher odds to have self-reported food allergies. Conversely, adolescents with higher serum PFNA were less likely to be sensitized to food allergens. These results, along with previous studies, warrant further investigation, such as well-designed longitudinal studies.     

Perfluoroalkyl substances in polar bear mother–cub pairs: A comparative study based on plasma levels from 1998 and 2008

Perfluoroalkyl substances (PFASs) are protein-binding blood-accumulating contaminants that may have detrimental toxicological effects on the early phases of mammalian development. To enable an evaluation of the potential health risks of PFAS exposure for polar bears (Ursus maritimus), an exposure assessment was made by examining plasma levels of PFASs in polar bear mothers in relation to their suckling cubs-of-the-year (~ 4 months old). Samples were collected at Svalbard in 1998 and 2008, and we investigated the between-year differences in levels of PFASs. Seven perfluorinated carboxylic acids (∑₇PFCAs: PFHpA, PFOA, PFNA, PFDA, PFUnDA, PFDoDA, and PFTrDA) and two perfluorinated sulfonic acids (∑₂PFSAs: PFHxS and PFOS) were detected in the majority of the mothers and cubs from both years. In mothers and cubs, most PFCAs were detected in higher concentrations in 2008 than in 1998. On the contrary, levels of PFOS were lower in 2008 than in 1998, while levels of PFHxS did not differ between the two sampling years. PFOS was the dominating compound in mothers and cubs both in 1998 and in 2008. Concentration of PFHpA did not differ between mothers and cubs, while concentrations of PFOA, PFNA, PFDA, PFUnDA, PFDoDA, PFTrDA, PFHxS, and PFOS were higher in mothers than in their cubs. Except from PFHpA, all compounds correlated significantly between mothers and their cubs. The mean cub to mother ratios ranged from 0.15 for PFNA to 1.69 for PFHpA. On average (mean ± standard error of mean), the levels of ∑₇PFCAs and ∑₂PFSAs in cubs were 0.24 ± 0.01 and 0.22 ± 0.01 times the levels in their mothers, respectively. Although maternal transfer appears to be a substantial source of exposure for the cubs, the low cub to mother ratios indicate that maternal transfer of PFASs in polar bears is relatively low in comparison with hydrophobic contaminants (e.g. PCBs). Because the level of several PFASs in mothers and cubs from both sampling years exceeded the levels associated with health effects in humans, our findings raise concern on the potential health effects of PFASs in polar bears from Svalbard. Effort should be made to examine the potential health effects of PFASs in polar bears.     

Time trends of perfluorinated alkyl acids in serum from Danish pregnant women 2008–2013

We aimed to estimate the levels and time trends of perfluorinated alkyl acids (PFAAs) in serum of 1533 Danish pregnant nulliparous women between 2008 and 2013. The selection criterion of only including nulliparous women was chosen to avoid confounding from parity. The serum samples were analyzed for sixteen PFAAs using solid phase extraction and liquid chromatography tandem mass spectrometry (LC-MS/MS). We investigated the time trends for seven PFAAs, which were detected in more than 50% of the samples: perfluorohexane sulfonate (PFHxS), perfluoroheptane sulfonate (PFHpS), perfluorooctane sulfonate (PFOS), perfluorooctanoic acid (PFOA), perfluorononanoic acid (PFNA), perfluorodecanoic acid (PFDA), and perfluoroundecanoic acid (PFUnA). We found that the serum levels of all seven PFAAs decreased during the period from 2008 to 2013; on average PFHxS decreased with 7.0% per year, PFHpS with 14.8%, PFOS with 9.3%, PFOA with 9.1%, PFNA with 6.2%, PFDA with 6.3%, and PFUnA with 7.1% per year. Adjustment for maternal age, body mass index (BMI), educational level and gestational age at blood sampling did not change the time trends much. To our knowledge, we are the first to report decreasing trends of PFNA, PFDA and PFUnA since year 2000, thereby indicating that the phase-out of these compounds are beginning to show an effect on human serum levels.     

Circulating levels of Persistent Organic Pollutants (POPs) among elderly men and women from Sweden: Results from the Prospective Investigation of the Vasculature in Uppsala Seniors (PIVUS)

Persistent Organic Pollutants (POPs) are a huge group of chemicals that have been linked to various adverse health effects in humans. Large epidemiological studies investigating gender differences in levels of POPs in the elderly are limited and the results from these are not always consistent. The present study was undertaken to examine the background levels of a broad range of POPs in human plasma samples among elderly men and women from Sweden and to assess the influence of gender. Levels of 23 POPs were determined in plasma samples collected during 2001–2004 from 1016 (50.2% women) 70 year-old participants from the population-based Prospective Study of the Vasculature in Uppsala Seniors (PIVUS). Measurements were performed using high resolution gas chromatography with high resolution mass spectrometry (HRGC-HRMS) and the POPs studied were 16 polychlorinated biphenyls (PCBs), five organochlorine (OC) pesticides, one dioxin, and one brominated flame retardant. The concentrations of the selected POPs were found similar, or comparable, to other studies of non-occupationally exposed populations from Sweden and Europe. Differences in levels of POPs between men and women were assessed by using Wilcoxon rank-sum (Mann–Whitney) test. Significant (p < 0.0001) gender differences in levels of specific POPs were observed and a number of POP concentrations were found to differ between men and women. More specifically, levels of HCB, OCDD, and PCB congeners #74, #105, and #118 were found to be higher in women, while the rest of the majority of POPs were higher in men.     

Perfluorinated chemicals in blood of residents in Catalonia (Spain) in relation to age and gender: a pilot study

Fluorinated organic compounds (FOCs) are a group of chemicals widely used as surfactants, lubricants, polymers, and fire-fighting foams. Recent studies have shown the ubiquitous distribution of FOCs in the environment, wildlife, and humans. We here report the results of a pilot study conducted to provide preliminary data on the levels of 13 FOCs in the blood of 48 residents in Catalonia, Spain, in relation to gender and age (25+/-5 and 55+/-5 years). The highest mean concentration was obtained for perfluorooctane sulfonate (PFOS, 7.64 ng/ml), followed by perfluorohexane sulfonate (PFHxS, 3.56 ng/ml) and perfluorooctanoic acid (PFOA, 1.80 ng/ml). Four other FOCs showed mean levels between 0.30 and 0.44 ng/ml, whereas those of the remaining 6 compounds were below the detection limit. Regarding gender, the blood levels of PFHxS and PFOA were significantly higher (p<0.05) in men than in women, while differences according to age were only noted for PFHxS (p<0.05) and perfluorooctane sulfonamide (PFOSA) (p<0.001), for which the levels were higher in the younger (25+/-5 years) group of subjects. A significant correlation between PFOS levels and those of the remaining detected FOCs (except PFDA) was found. In general terms, the current FOC concentrations were lower than those found in recent studies concerning levels of these chemicals in human blood and serum of subjects from different countries.     

Perfluoroalkyl and polyfluoroalkyl substances in cord blood of newborns in Shanghai,China: Implications for risk assessment

Perfluoroalkyl and polyfluoroalkyl substances (PFASs) are commonly used in industrial applications and consumer products, and their potential health impacts are of concern, especially for vulnerable population like fetuses. However, in utero exposure to PFASs and health implications are far from fully characterized in China. To fill in the gap, we analyzed 10 PFASs in cord plasma samples (N = 687) collected in Shanghai between 2011 and 2012, one of the regions widely polluted with PFASs in China. A questionnaire survey on maternal and diet-related factors was conducted. Except for perfluoroheptanoic acid (PFHpA) and perfluorooctane sulfonamide (PFOSA), all other PFASs were detected in ˃90% of the samples. Perfluorooctanoic acid (PFOA) was the most predominant PFAS (median value: 6.96 ng/mL), followed by perfluorooctane sulfonate (PFOS) (2.48 ng/mL). PFOA and PFOS combined contributed to 80% of the total PFASs. The final multiple regression models showed that maternal factors including maternal age, body mass index, gestational age, economic status and educational level as well as consumption of fish and wheat were significantly related with concentrations of PFASs in cord blood. The risk assessment using the hazard quotients (HQs) approach on the basis of plasma PFAS levels indicated no potential concern for developmental toxicity in the local newborns. The results demonstrate the unique profiles of local prenatal exposure to PFASs, suggesting that PFOA has been the primary human exposure due to its widespread use and pollution. Special attention to high PFOA exposure and confirmation of potential determinants should be taken as a priority in the future plan for risk management and actions in this area.     

Fate,distribution, and contrasting temporal trends of perfluoroalkyl substances (PFASs) in Lake Ontario,Canada

Lake Ontario water and sediment collected from tributary, nearshore, and open lake sites were analyzed for perfluoroalkyl substances (PFASs), namely perfluoroalkyl carboxylic acids (PFCAs, F(CF₂)_nCO₂⁻; n = 6-11,13) and perfluoroalkane sulfonic acids (PFSAs, F(CF₂)_nSO₃⁻; n = 6,8,10). Survey results of surface sediment and water indicated that shorter chained PFASs were predominant in and near urban/industrial area watersheds, while longer chained PFASs were predominant in fine-grained sediment from major depositional basins. Niagara River suspended solids (1981–2006) demonstrated temporal trends that may have been influenced by recent changes in North American production and use of PFASs. Perfluorooctane sulfonate (PFOS) reached a peak concentration in 2001 of 1.1 ng/g, followed by a decrease from 2001 to 2006 (half-life = 9 years). Perfluorooctanoic acid (PFOA) increased from 2001 to 2006 (doubling time = 2 years) reaching a peak concentration of 0.80 ng/g. In contrast, three sediment cores from western, central, and eastern Lake Ontario showed increasing temporal trends to surface sediment for all PFASs. PFOA and PFOS concentrations increased from 1988 to 2004 (doubling time = ~ 4 years) in the western Lake Ontario core. The observed variations in temporal trends from different environmental compartments may be a result of the physico-chemical properties of PFASs, ongoing emissions, and the environmental transformation and degradation of PFAS precursor compounds.     

Exposure to per- and polyfluoroalkyl substances through the consumption of fish from lakes affected by aqueous film-forming foam emissions — A combined epidemiological and exposure modeling approach. The SAMINOR 2 Clinical Study

Releases of aqueous film-forming foams (AFFFs) from airport firefighting activities have been identified as important local point sources of per- and polyfluoroalkyl substances (PFASs) in nearby waterways. PFASs can be taken up by fish, and in turn by the humans that consume them. Despite the global extent of AFFF emissions, few studies exist on related impacts on humans. We aimed to investigate the associations between the consumption of fish from AFFF-affected waters and serum PFAS concentrations in humans using a combination of statistical tools, empirical data, and toxicokinetic modeling. Participants of the SAMINOR 2 Clinical Study were the basis for this study sample, which comprised 74 persons. Fifty-nine participants who reported consuming fish from AFFF-affected waters and 15 nonconsumers completed a questionnaire and gave serum samples. Participants were classified based on their consumption of trout and char: high (n = 16), moderate (n = 16), low (n = 27), and nonconsumers (n = 15); and serum samples were tested for the presence of 15 PFASs. Perfluorooctane sulfonic acid (PFOS) was found in all participants, with the highest concentrations detected in the high consumption group (geometric means, 28 ng/mL) compared to the low consumption group and nonconsumers (10 and 11 ng/mL, respectively). In an analysis of variance contrast model, a significant, positive increasing trend was seen for fish consumption and PFOS, perfluorohexane sulfonic acid (PFHxS), and perfluorononanoic acid (PFNA). Toxicokinetic modeling allowed us to predict the median increases in serum concentrations of PFOS, PFHxS, and PFNA among high consumers within a factor of 2.2. The combination of statistical evaluation and toxicokinetic modeling clearly demonstrated a positive relationship between consumption of fish from AFFF-affected waters and serum PFAS concentrations. Further studies on dietary exposure to other PFASs present in AFFF and its consequences on human health are warranted.     

Perfluoroalkyl carboxylates and sulfonates and precursors in relation to dietary source tracers in the eggs of four species of gulls (Larids) from breeding sites spanning Atlantic to Pacific Canada

In the present study, we identified and examined the spatial trends, sources and dietary relationships of bioaccumulative perfluorinated sulfonate (PFSA; C(6), C(8), and C(10) chain lengths) and carboxylate (PFCA; C(6) to C(15) chain lengths) contaminants, as well as precursor compounds including several perfluorinated sulfonamides, and fluorotelomer acids and alcohols, in individual eggs (collected in 2008) from four gull species [glaucous-winged (Larus glaucescens), California (Larus californicus), ring-billed (Larus delawarensis) and herring (Larus argentatus) gulls] from 15 marine and freshwater colony sites in provinces across Canada. The pattern of PFSAs was dominated by perfluorooctane sulfonate (PFOS; >89% of ΣPFSA concentration) regardless of egg collection location. The highest ΣPFSA concentrations were found in the eggs collected in the urbanized areas in the Great Lakes and the St. Lawrence River area [Big Chicken Island 308 ng/g ww, Toronto Harbour 486 ng/g ww, and Ile Deslauriers (HG) 299 ng/g ww]. Also, eggs from all freshwater colony sites had higher ΣPFSA concentrations, which were significant (p<0.05) in many cases, compared to the marine sites with the exception of the Sable Island colony in Atlantic Canada off the coast of Nova Scotia. C(6) to C(15) chain length PFCAs were detected in the eggs, although the pattern was variable among the 15 sites, where PFUnA and PFTrA dominated the pattern for most colonies. Like the ΣPFSA, the highest concentrations of ΣPFCA were found in the eggs from Big Chicken Island, Toronto Harbour, Ile Deslauriers (HG), and Sable Island, although not all freshwater sites had higher concentrations compared to marine sites. Dietary tracers [δ(15)N and δ(13)C stable isotopes (SIs)] revealed that PFSA and PFCA exposure is colony dependent. SI signatures suggested that gulls from most marine colony sites were exposed to PFCs via marine prey. The exception was the Mandarte Island colony in Pacific British Columbia, where PFSA and PFCA exposure appeared to be via terrestrial and/or freshwater prey consumption. The same was true for the freshwater sites where egg SIs suggested both aquatic and terrestrial prey consumption as the source for PFC exposure depending on the colony. Both aquatic (marine and freshwater) and terrestrial prey are likely sources of PFC exposure to gulls but exposure scenarios are colony-specific.     

Serum perfluorinated chemicals,glucose homeostasis and the risk of diabetes in working-aged Taiwanese adults

BackgroundThe link among perfluoroalkyl and polyfluoroalkyl substances (PFASs), abnormal glucose homeostasis and the risk of diabetes has been intensively debated with conflicting evidence.ObjectivesWe evaluated the associations among PFASs, oral glucose tolerance testing (OGTT) curves and diabetes prevalence in 571 working-aged Taiwanese participants.MethodsExposure measures included serum perfluorooctanoic acid (PFOA), perfluorooctane sulfonic acid (PFOS), perfluorononanoic acid (PFNA), and perfluoroundecanoic acid (PFUA). Outcomes were OGTT curves and prevalent diabetes defined by fasting blood glucose (FBG) ≥ 126 mg/dL, 2-h glucose ≥ 200 mg/dL, or glycated hemoglobin ≥ 6.5%. Analyses were performed with multiple logistic regression and functional data analysis.ResultsA total of 39 participants (6.8%) had diabetes in this study. After full adjustment, the increase in the geometric means of FBG, 2-h glucose concentrations, and area under the OGTT curve (AUC₁₂₀) with a doubling increase in PFOS was 3% (95% CI 1–4), 8% (5–12), and 6% (4–9), respectively. Compared to the lowest-quartile of PFOS concentrations (< 2.4 ng/ml), the OGTT trajectories were significantly steeper in participants of the highest-quartile PFOS exposure (> 4.8 ng/ml) and the vertical shifting of the mean curve for each PFOS quartile showed a dose–response pattern. The adjusted odds ratio for diabetes comparing the highest to lowest quartile was 3.37 (95% CI 1.18–9.65). For PFOA, PFNA, and PFUA, the opposite pattern of OGTT trajectory and the opposite risk profile for diabetes were observed.ConclusionsChronic PFOS exposure was associated with impaired glucose homeostasis and the increased prevalence of diabetes. However, PFOA, PFNA, and PFUA showed a potential protective effect against glucose intolerance and the risk of diabetes. Future research focusing on clarifying possible differential effects of different species of PFASs on glucose homeostasis and establishing the prospective associations between PFASs and diabetes is needed.     

Assessing the relationship between perfluoroalkyl substances,thyroid hormones and binding proteins in pregnant women; a longitudinal mixed effects approach

The mechanisms involved in thyroid homeostasis are complex, and perfluoroalkyl substances (PFASs) have been indicated to interfere at several levels in this endocrine system. Disruption of the maternal thyroid homeostasis during early pregnancy is of particular concern, where subclinical changes in maternal thyroid hormones (THs) may affect embryonic and foetal development.The present study investigated associations between THs, thyroid binding proteins (TH-BPs) and PFAS concentrations in pregnant women from Northern Norway.Women participating in The Northern Norway Mother-and-Child contaminant Cohort Study (MISA) donated a blood sample at three visits related to their pregnancy and postpartum period (during the second trimester, 3 days and 6 weeks after delivery) in the period 2007–2009. Participants were assigned to quartiles according to PFAS concentrations during the second trimester and mixed effects linear models were used to investigate potential associations between PFASs and repeated measurements of THs, TH-BPs, thyroxin binding capacity and thyroid peroxidase antibodies (anti-TPOs).Women within the highest perfluorooctane sulfonate (PFOS) quartile had 24% higher mean concentrations of thyroid stimulating hormone (TSH) compared to the first quartile at all sampling points. Women within the highest quartiles of perfluorodecanoate (PFDA) had 4% lower mean concentrations of triiodothyronine (T3) and women within the highest quartile of perfluoroundecanoate (PFUnDA) had 3% lower mean concentrations of free triiodothyronine (FT3). Further, the difference in concentrations and the changes between three time points were the same for the PFAS quartiles. Thyroxin binding capacity was associated with all the THs and TH-BPs, and was selected as a holistic adjustment for individual changes in TH homeostasis during pregnancy. Finally, adjusting for maternal iodine status did not influence the model predictions.Findings in the present study suggest modifications of TH homeostasis by PFASs in a background exposed maternal population. The variation in levels of THs between PFAS quartiles was within normal reference ranges and may not be of clinical significance in the pregnant woman. However, subtle individual changes in maternal THs may have significant consequences for foetal health.     

Perfluoroalkyl substances and thyroid function in older adults

Current understanding of the thyroid disruptive properties of perfluoroalkyl substances (PFASs), particularly in aging populations, is limited. The objectives of this study were to (i) assess associations between thyroid function, as measured by serum thyrotropin (thyroid stimulating hormone, TSH), free thyroxine (fT4), total thyroxine (T4), and total triiodothyronine (T3), and serum perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA) in an aging population and (ii) determine if other persistent organic pollutants with thyroid disruptive properties including polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs) modify such associations. We conducted a cross-sectional study of 87 men and women 55 to 74 years of age, without clinically-diagnosed thyroid disease, who resided in upper Hudson River communities in New York. Geometric means (standard deviations) of serum PFOS and PFOA were 31.6 (1.7) ng/mL and 9.17 (1.72) ng/mL, respectively. Multivariable linear regression analyses indicated that one interquartile range difference in PFOS corresponded to 4% and 9% increases in fT4 and T4 respectively. We detected statistical interactions between PFOA and age for effects on fT4 and T4; joint increases in PFOA and age were associated with increases in fT4 and T4, of 3% and 7%, respectively. We also detected statistical interactions between PFOS and total PCBs for the effect on T3 and between PFOA and total PBDEs for the effect on TSH. Our results suggest that PFASs are associated with subtle alterations in thyroid hormone levels in this population, and that these associations are likely to vary by age, and levels of PCBs and PBDEs.     

Changes in serum levels of perfluoroalkyl substances during a 10-year follow-up period in a large population-based cohort

Poly- and perfluoroalkyl substances (PFASs) are a group of man-made fluorinated chemicals which have, at background levels, been associated with negative health effects in humans. Thus far, most human biomonitoring studies have evaluated the general change in PFAS concentration over time by continuously testing various individuals. This is one of the few studies to report the longitudinal trend of a range of PFAS concentrations in humans. In addition, this is the first known longitudinal study to include a large background level exposed cohort of both men and women with the same age and location who were repeatedly sampled from 2001 to 2014.The longitudinal change in concentration of eight PFASs detected in serum collected from the Prospective Investigation of the Vasculature in Uppsala Seniors (PIVUS) cohort were determined and compared to results from general population studies. The sex-dependent changes in PFAS concentrations over time were also assessed.Serum was sampled from the same individuals at ages 70 (collection period 2001–2004), 75 (2006–2009) and 80 (2011–2014,). Eight (C_6–11) of fourteen (C_4–13) analyzed PFASs were usually detected in over 75% of individuals and assessed using a random effects (mixed) model.In the 579 individuals attending all three examinations, PFOSA and PFOS concentrations significantly decreased, while the remaining six PFASs significantly increased between ages 70 and 75. However, between ages 75 and 80 all PFAS concentrations significantly decreased. Overall from age 70 to 80, concentrations of PFHxS, PFUnDA, PFNA, and PFDA showed a significant increase (7% to 34%), whereas concentrations of PFOSA, PFHpA, PFOS, and PFOA (− 75% to − 27%) significantly decreased. Over time PFHxS concentrations increased more among women, while PFHpA concentrations showed a greater decrease among men.From age 70 to age 80, spanning from 2001‐2004 to 2011–2014, the PIVUS cohort showed decreases in circulating levels of some PFASs phased out of production with the exception of PFHxS and C_>8 PFASs. Contrary to other studies, PFHxS concentrations showed the greatest overall increase, which is likely attributed to a local drinking water contamination incident.     

Determinants of plasma concentrations of perfluoroalkyl substances in pregnant Norwegian women

BackgroundPerfluoroalkyl substances (PFASs) are widespread pollutants that have been associated with adverse health effects although not on a consistent basis. Diet has been considered the main source of exposure. The aim of the present study was to identify determinants of four plasma PFASs in pregnant Norwegian women.MethodsThis study is based in the Norwegian Mother and Child Cohort Study (MoBa) conducted by the Norwegian Institute of Public Health. Our sample included 487 women who enrolled in MoBa from 2003 to 2004. A questionnaire regarding sociodemographic, medical, and reproductive history was completed at 17 weeks of gestation and a dietary questionnaire was completed at 22 weeks of gestation. Maternal plasma samples were obtained around 17 weeks of gestation. Plasma concentrations of four PFASs (perfluorooctane sulfonate (PFOS), perfluorooctanoate (PFOA), perfluorohexane sulfonate (PFHxS), and perfluorononanoate (PFNA)) were examined in relation to demographic, lifestyle, dietary, and pregnancy-related covariates. Predictors were identified by optimizing multiple linear regression models using Akaike's information criterion (AIC).ResultsParity was the determinant with the largest influence on plasma PFAS concentrations, with r² between 0.09 and 0.32 in simple regression models. In optimal multivariate models, when compared to nulliparous women, parous women had 46%, 70%, 19%, and 62% lower concentrations of PFOS, PFOA, PFHxS, and PFNA respectively (p < 0.001 except for PFHxS, p < 0.01). In all these models, duration of breastfeeding was associated with reduced PFAS levels. PFOA showed the largest reduction from breastfeeding, with a 2–3% reduction per month of breastfeeding in typical cases. Levels of PFOS, PFOA, and PFNA increased with time since most recent pregnancy. While pregnancy-related factors were the most important predictors, diet was a significant factor explaining up to 4% of the variance. One quartile increase in estimated dietary PFAS intake was associated with plasma PFOS, PFOA, PFHxS, and PFNA concentration increases of 7.2%, 3.3%, 5.8% and 9.8%, respectively, resulting in small, although non-trivial absolute changes in PFAS concentrations.ConclusionPrevious pregnancies and breastfeeding duration were the most important determinants of PFASs in this sample of pregnant women.     

The precautionary principle and chemicals management: The example of perfluoroalkyl acids in groundwater

Already in the late 1990s microgram-per-liter levels of perfluorooctane sulfonate (PFOS) were measured in water samples from areas where fire-fighting foams were used or spilled. Despite these early warnings, the problems of groundwater, and thus drinking water, contaminated with perfluoroalkyl and polyfluoroalkyl substances (PFASs) including PFOS are only beginning to be addressed. It is clear that this PFAS contamination is poorly reversible and that the societal costs of clean-up will be high. This inability to reverse exposure in a reasonable timeframe is a major motivation for application of the precautionary principle in chemicals management. We conclude that exposure can be poorly reversible; 1) due to slow elimination kinetics in organisms, or 2) due to poorly reversible environmental contamination that leads to continuous exposure. In the second case, which is relevant for contaminated groundwater, the reversibility of exposure is not related to the magnitude of a chemical's bioaccumulation potential. We argue therefore that all PFASs entering groundwater, irrespective of their perfluoroalkyl chain length and bioaccumulation potential, will result in poorly reversible exposures and risks as well as further clean-up costs for society. To protect groundwater resources for future generations, society should consider a precautionary approach to chemicals management and prevent the use and release of highly persistent and mobile chemicals such as PFASs.     

Relationship between dietary exposure and serum perfluorochemical (PFC) levels—A case study

Daily dietary intake of perfluorinated chemicals (PFCs) in relation to serum levels was assessed by determination of nine PFCs including perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA) in matched daily diet duplicates and serum samples. Diet and serum were collected in year 2004 from 20 women in Osaka and Miyagi, Japan. Only PFOS and PFOA were detected in the diet samples and no significant difference between cities was seen. After adjusted by water content, diet concentration of PFOA was significantly higher in Osaka. The median daily intake calculated using the measured diet concentrations was 1.47 ng PFOS/kg b.w. and 1.28 ng PFOA/kg b.w. for Osaka, and 1.08 ng PFOS/kg b.w. and 0.72 ng PFOA/kg b.w. for Miyagi. A significant difference between cities was seen for the serum concentrations with median of 31 ng/mL PFOS and PFOA in Osaka, compared to 14 ng/mL PFOS and 4.6 ng/mL PFOA in Miyagi. Carboxylates such as perfluorononanoic acid (PFNA) and perfluoroundecanoic acid (PFUnDA) were also detected in serum at median levels 6.9 ng/mL and 3.2 ng/mL (Osaka), and 2.8 ng/mL and 5.1 ng/mL (Miyagi). Based on one-compartment model under steady state, dietary intake of PFOS and PFOA accounted for only 22.4% and 23.7% of serum levels in Osaka females, and in contrast 92.5% and 110.6% in Miyagi females, respectively.     

Cumulative health risk assessment of 17 perfluoroalkylated and polyfluoroalkylated substances (PFASs) in the Swedish population

Humans are simultaneously exposed to a multitude of chemicals. Human health risk assessment of chemicals is, however, normally performed on single substances, which may underestimate the total risk, thus bringing a need for reliable methods to assess the risk of combined exposure to multiple chemicals. Per- and polyfluoroalkylated substances (PFASs) is a large group of chemicals that has emerged as global environmental contaminants. In the Swedish population, 17 PFASs have been measured, of which the vast majority lacks human health risk assessment information. The objective of this study was to for the first time perform a cumulative health risk assessment of the 17 PFASs measured in the Swedish population, individually and in combination, using the Hazard Index (HI) approach. Swedish biomonitoring data (blood/serum concentrations of PFASs) were used and two study populations identified: 1) the general population exposed indirectly via the environment and 2) occupationally exposed professional ski waxers. Hazard data used were publicly available toxicity data for hepatotoxicity and reproductive toxicity as well as other more sensitive toxic effects. The results showed that PFASs concentrations were in the low ng/ml serum range in the general population, reaching high ng/ml and low μg/ml serum concentrations in the occupationally exposed. For those congeners lacking toxicity data with regard to hepatotoxicity and reproductive toxicity read-across extrapolations was performed. Other effects at lower dose levels were observed for some well-studied congeners. The risk characterization showed no concern for hepatotoxicity or reproductive toxicity in the general population except in a subpopulation eating PFOS-contaminated fish, illustrating that high local exposure may be of concern. For the occupationally exposed there was concern for hepatotoxicity by PFOA and all congeners in combination as well as for reproductive toxicity by all congeners in combination, thus a need for reduced exposure was identified. Concern for immunotoxicity by PFOS and for disrupted mammary gland development by PFOA was identified in both study populations as well as a need of additional toxicological data for many PFAS congeners with respect to all assessed endpoints.     

Association of perfluoroalkyl substances exposure in utero with reproductive hormone levels in cord blood in the Hokkaido Study on Environment and Children's Health

BackgroundExposure to perfluoroalkyl substances (PFASs) may disrupt reproductive function in animals and humans. Although PFASs can cross the human placental barrier, few studies evaluated the effects of prenatal PFAS exposure on the fetus' reproductive hormones.ObjectiveTo explore the associations of prenatal exposure to perfluorooctane sulfonate (PFOS) and perfluorooctanoate (PFOA) with cord blood reproductive hormones.MethodsIn the prospective birth cohort (Sapporo cohort of the Hokkaido study), we included 189 mother–infant pairs recruited in 2002–2005 with both prenatal maternal and cord blood samples. PFOS and PFOA levels in maternal blood after the second trimester were measured via liquid chromatography–tandem mass spectrometry. We also measured cord blood levels of the fetuses' reproductive hormones, including estradiol (E2), total testosterone (T), progesterone (P4), inhibin B, insulin-like factor 3, steroid hormone binding globulin, follicle-stimulating hormone, and luteinizing hormone, and prolactin (PRL).ResultsThe median PFOS and PFOA levels in maternal serum were 5.2 ng/mL and 1.4 ng/mL, respectively. In the fully adjusted linear regression analyses of the male infants, maternal PFOS levels were significantly associated with E2 and positively, and T/E2, P4, and inhibin B inversely; PFOA levels were positively associated with inhibin B levels. Among the female infants, there were significant inverse associations between PFOS levels and P4 and PRL levels, although there were no significant associations between PFOA levels and the female infants' reproductive hormone levels.ConclusionsThese results suggest that the fetal synthesis and secretion of reproductive hormones may be affected by in utero exposure to measurable levels of PFOS and PFOA.     

Perfluoroalkyl substances in human milk: A first survey in Italy

Due to their widespread diffusion, perfluoroalkyl substances (PFASs) have been frequently found in the environment and in several animal species. It has been demonstrated that they can easily reach also humans, mainly through diet. Being lactation a major route of elimination of these contaminants, their occurrence in human milk is of particular interest, especially considering that it generally represents the unique food source for newborns. Perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA), the two most important compounds of this family, have been frequently found in human milk at variable concentrations, but still limited data are available. The present study, the first conducted in Italy capable to detect these pollutants at ultra-trace levels by UPLC-MS/MS, confirmed the role of lactation as a relevant source of exposure for breastfed children. The measured concentrations ranged between 15 and 288 ng/L for PFOS and between 24 and 241 ng/L for PFOA. Moreover, mean concentrations and frequencies of both analytes resulted higher in milk samples provided by primiparous women, suggesting that the risk of intake might be higher for first-borns. Finally, comparing these results with previous data, PFOS gradual decrease over time since year 2000 was confirmed.     

Perfluoroalkyl substances and extractable organic fluorine in surface sediments and cores from Lake Ontario

Fourteen perfluoroalkyl substances (PFASs) including short-chain perfluorocarboxylates (PFCAs, C4–C6) and perfluoroalkane sulfonates (PFSAs, C4 and C6) were measured in surface sediment samples from 26 stations collected in 2008 and sediment core samples from three stations (Niagara, Mississauga, and Rochester basins) collected in 2006 in Lake Ontario. Perfluorooctanesulfonate (PFOS), perfluorooctanoate (PFOA), perfluorononanoate (PFNA), perfluorodecanoate (PFDA), and perfluoroundecanoate (PFUnDA) were detected in all 26 surface sediment samples, whereas perfluorohexane sulfonate (PFHxS), perfluorooctane sulfonamide (FOSA), perfluorododecanoate (PFDoDA) and perfluorobutanoate (PFBA) were detected in over 70% of the surface sediment samples. PFOS was detected in all of the sediment core samples (range: 0.492–30.1 ng g^− 1 d.w.) over the period 1952–2005. The C8 to C11 PFCAs, FOSA, and PFBA increased in early 1970s. An overall increasing trend in sediment PFAS concentrations/fluxes from older to more recently deposited sediments was evident in the three sediment cores. The known PFCAs and PFSAs accounted for 2–44% of the anionic fraction of the extractable organic fluorine in surface sediment, suggesting that a large proportion of fluorine in this fraction remained unknown. Sediment core samples collected from Niagara basin showed an increase in unidentified organic fluorine in recent years (1995–2006). These results suggest that the use and manufacture of fluorinated organic compounds other than known PFCAs and PFSAs has diversified and increased.