Abstract  The objective of the Control of Hazardous Substances in the Baltic Sea (COHIBA) project is to support the implementation of the HELCOM Baltic Sea Action Plan regarding hazardous substances by developing joint actions to achieve the goal of "a Baltic Sea with life undisturbed by hazardous substances". One aim in the project was to identify the most important sources of 11 hazardous substances of special concern in the Baltic Sea. Among them are perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA). In this study, four perfluorinated alkyl acids (PFAAs) were studied: PFOA, PFOS, perfluorohexanoic acid (PFHxA) and perfluorodecanoic acid (PFDA). The occurrence of PFAAs in municipal and industrial wastewater treatment plant effluents (MWWTP1-3, IWWTP1), target industry effluent, storm water, landfill leachate and sludge was studied. Effluents were analysed six times and storm water, leachate and sludge were analysed twice, once in the warm season and once in the cold, during a 1-year sampling campaign. PFOS prevailed in two municipal effluents (MWWTP1 and 3) and industrial effluent (IWWTP1; 7.8-14, 8.0-640 and 320-1,300 ng/l, respectively). However, in one municipal effluent (MWWTP2) PFOA was, in a majority of sampling occasions, the predominant PFAA (9-15 ng/l) followed by PFOS (3.8-20 ng/l). The highest PFAA loads of the municipal effluents were found in the MWWTP3 receiving the biggest portion of industrial wastewater. In storm water the highest concentration was found for PFHxA (17 ng/l). The highest concentration of PFOS and PFOA were 9.9 and 5.1 ng/l, respectively. PFOS, PFOA and PFHxA were detected in every effluent, storm water and landfill leachate sample, whereas PFDA was detected in most of the samples (77%). In the target industry, PFOS concentrations varied between 1,400 and 18,000 μg/l. In addition, on one sampling occasion PFOA and PFHxA were found (0.027 and 0.009 μg/l, respectively). For effluents, PFAA mass flows into the Baltic Sea were calculated. For municipal wastewater treatment plants average mass flows per day varied for PFOS between 1,073 and 38,880 mg/day, for PFOA 960 and 2,700 mg/day, for PFHxA 408 and 1,269 mg/day and for PFDA 84 and 270 mg/day. In IWWTP mass flows for PFOS, PFOA, PFHxA and PFDA were 495 mg/d, 28 mg/d, 23 mg/d and 0.6 mg/g, respectively.

Abstract  Products containing perfluorinated compounds (PFCs) have been widely used during the last 50 years. As a result, worldwide environmental pollution by PFCs has been reported. The sources of PFC pollution in the aquatic environment have been poorly understood. In this study, river water and sewage treatment plant (STP) effluent were sampled along the stretch of the Tsurumi River and also at a fixed station in the river. The concentrations of perfluorooctanesulfonate (PFOS), perfluorohexanoic acid (PFHxA), perfluoroheptanoic acid (PFHpA), perfluorooctanoic acid (PFOA), perfluorononanoic acid (PFNA) and perfluorodecanoic acid (PFDA) were measured. With an increase in river flow rate, it was observed that the PFC concentrations in the river water at fixed station were remained the same or increased for PFOS (179.9+/-34.4-179.6+/-69.5 ng l(-1)), PFHxA (5.5+/-0.8-9.0+/-2.6 ng l(-1)), PFHpA (3.1+/-0.3-4.4+/-1.0 ng l(-1)), and PFOA (15.9+/-0.3-13.4+/-2.5 ng l(-1)) whereas the concentration of PFNA (38.0+/-3.3-15.4+/-3.0 ng l(-1)) and PFDA (3.9+/-0.3-2.1+/-0.3 ng l(-1)) were decreased. On the other hand, the loads of every PFC increased with an increase in river flow rate. The loads of PFCs in rain runoff were estimated to be 2-11 times greater than those in STP effluents that are discharged into the river. These results indicate the existence of a PFC nonpoint source (NPS) and its impact to the total PFC load of river is significant.

Abstract  In 2013 a contamination of drinking water by perfluoroalkylated substances (PFASs) was discovered in areas of the Veneto Region (northern Italy). In this study the exposure to PFASs of people living in the aforesaid areas was characterized: contaminant serum concentrations were measured and compared with those of a control population group living in neighboring areas at background exposure (based on available drinking water data). The enrolled population was also genotyped for the OATP1A2*3 allelic variant, possibly affecting PFAS excretion and hence the internal dose. The difference in PFAS concentrations between exposed and not exposed subjects was significantly larger for nine of the 12 substances analyzed, and confirmed that water contamination had resulted in an appreciable high exposure of the residing population over time. Within the group of exposed subjects, subgroups at different exposure levels were identified. The contamination of drinking water of the residence area was found to be the main factor influencing PFAS serum levels; in addition to water contamination, other relevant influencing factors were sex, the years of residence and raising own livestock. No relationship with the genetic trait for the studied renal transporter was evidenced. These results provide a baseline characterization of PFAS exposure of the monitored population groups for further studies, planned to be carried out in the near future.

Abstract  The present study was aimed at the development of a strategy for removing and degrading perfluorohexanoic acid (PFHxA) from industrial process waters at concentrations in the range 60-200 mg L(-1). The treatment train consisted of nanofiltration (NF) separation followed by electrochemical degradation of the NF concentrate. Using a laboratory-scale system and working in the total recirculation mode, the DowFilm NF270 membrane provided PFHxA rejections that varied in the range 96.6-99.4% as the operating pressure was increased from 2.5 to 20 bar. The NF operation in concentration mode enabled a volume reduction factor of 5 and increased the PFHxA concentration in the retentate to 870 mg L(-1). Results showed that the increase in PFHxA concentration and the presence of calcium sulfate salts did not induce irreversible membrane fouling. The NF retentate was treated in a commercial undivided electrochemical cell provided with two parallel flow-by compartments separated by bipolar boron doped diamond (BDD) electrode, BDD counter anode, and counter cathode. Current densities ranging from 20 to 100 A m(-2) were examined. The electrochemical degradation rate of PFHxA reached 98% and was accompanied by its efficient mineralization, as the reduction of total organic carbon was higher than 95%. Energy consumption, which was 15.2 kWh m(-3) of treated NF concentrate, was minimized by selecting operation at 50 A m(-2). While most of the previous research on the treatment of perfluoroalkyl substances (PFASs) focused on the removal of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS), these compounds have been phased out by chemical manufacturers. Our findings are relevant for the treatment of PFHxA, which appears to be one of the present alternatives to long-chain PFASs thanks to its lower bioaccumulative potential than PFOA and PFOS. However, PFHxA also behaves as a persistent pollutant. Moreover, our results highlight the potential of combining membrane separation and electrochemical oxidation for the efficient treatment of PFAS-impacted waters.

Abstract  Perfluorooctanesulfonate (PFOS) and perfluorooctanoic acid (PFOA) are the main representatives of an rising class of persistent organic pollutants (POPs), perfluorochemicals (PFCs). In this study, determination of selected PFCs concentration in liver, brain, tail, adipose and peritoneum tissues of free-living European beaver (Castor fiber L.) was addressed. Tissue samples, collected from beavers living in Masurian Lakeland (NE Poland), were analyzed by dispersive Solid Phase Extraction (d-SPE) with micro-UHPLC-MS/MS system. In a group of ten selected pefrluorinated compounds only two perfluorinated acids (PFOA and PFNA) and one perfluorinated sulfonate (PFOS) were quantified. PFOA was detected in all analysed tissue samples in both female and male beavers in a range from 0.55 to 0.98ngg(-1) ww whereas PFOS was identified in all analyzed female beaver tissues and only in liver, subcutaneous adipose and peritoneum tissues of male beavers at the concentration level from 0.86 to 5.08ngg(-1) ww. PFNA was only identified in female beaver tissues (liver, subcutaneous adipose and peritoneum) in a range from 1.50 to 6.61ngg(-1) ww. This study demonstrated the bioaccumulation of PFCs in tissue samples collected from beavers living in area known as green lungs of Poland. The results provided in this study indicate for the increasing risk of PFCs occurrence in the environment and the level of PFCs in tissue of free-living European beavers may serve as bioindicator of environmental pollution by these compounds.

Abstract  The multixenobiotic resistance (closely related to multidrug resistance) system controls transport across the plasma membrane as a defense against toxic molecules. Multixenobiotic resistance system consists of an efflux pump, ABCB1 (also named P-glycoprotein, P-gp), and/or a molecule of the ABCC family (also named multiple resistance associated protein, MRP). ABCB1 is able to increase efflux of many low-molecular foreign molecules. Measuring system induction may be used as a biomarker of cell/organism exposure to foreign substances. Various established cell lines were tested for constitutive and induced multixenobiotic resistance proteins by Western blotting immunodetection. The pumping function was indirectly assayed with Rhodamine B by visualization of cell fluorescence in the presence of verapamil. Changes in ABC proteins were measured by flow cytometry after exposition to various perfluorinated carboxylic acids. MCF7 and HeLa cells were found to contain the highest constitutive level of both ABCB1 and ABCC1. HEK293 exhibited much less ABCB1 and no activity of pumping out Rhodamine B. The pumping activity was found to be related to the amount of the cell-type specific 170 kDa ABCB1 protein. An 8-day exposure to 10(-4) M perfluorononanoic acid resulted in about 2-2.5-fold increase of ABCB1 level. That was confirmed also for short times by flow cytometry of cells exposed to perfluorinated acids and its natural congeners. Both ABCB1- and ABCC1-related fluorescence increased along with the carbon chain in acids from C-6 up to C-9 and decreased for C-10. Measuring of multixenobiotic resistance changes in vitro induced by chemicals may be a convenient test for screening for their potential toxicity.

Abstract  Perfluorononanoic acid (PFNA) and perfluorodecanoic acid (PFDA), which are classified as perfluoroalkyl and polyfluoroalkyl substances (PFASs), have been widely used in industrial applications as a surface protectant. PFASs have been detected in wildlife and in humans around the globe. The purposes of this study are to develop and validate a physiologically based pharmacokinetic (PBPK) model for detecting PFNA and PFDA in male and female rats, and to apply the model to a human health risk assessment regarding the sex difference. A PBPK model of PFNA and PFDA was established based on an in vivo study in male and female rats. Analytes in biological samples (plasma, nine tissues, urine, and feces) were determined by ultra-liquid chromatography coupled tandem mass spectrometry (UPLC-MS/MS) method. PFNA and PFDA showed a gender differences in the elimination half-life and volume of distribution. The tissue-plasma partition coefficients were the highest in the liver in both male and female rats. The predicted rat plasma and urine concentrations simulated and fitted were in good agreement with the observed values. The PBPK models of PFNA and PFDA in male and female rats were then extrapolated to a human PBPK model based on human physiological parameters. The external doses were calculated at 3.35 ng/kg/day (male) and 17.0 ng/kg/day (female) for PFNA and 0.530 ng/kg/day (male) and 0.661 ng/kg/day (female) for PFDA. Human risk assessment was estimated using Korean biomonitoring values considering the gender differences. This study provides valuable insight into human health risk assessment regarding PFNA and PFDA exposure.

Abstract  The historical use of aqueous film forming foams (AFFF) containing perfluoroalkyl substances (PFASs) for firefighting and training activities has resulted in groundwater contamination. The competitive adsorption of PFASs and the effect of co-existing compounds on the removal of PFASs by anion-exchange resins were studied in this study. Perfluorohexane sulfonate (PFHxS) was selected as the representative PFAS, and resin IRA910 was found to be effective for PFHxS removal. When PFHxS was co-removed with other PFASs in bisolute system, it replaced the adsorbed PFASs with shorter C-F chains on the IRA910, while perfluorooctanesulfonate (PFOS) was not replaced by PFHxS. The competitive adsorption among PFASs decreased in the order of PFOS?>?PFHxS?>?PFOA?>?PFBS>PFHxA?>?PFBA, closely related to the hydrophobicity and functional groups of PFASs. The nonionic organic compounds could not interfere with the PFHxS removal, while ionic ones can reduce the sorption amount and their influence to the sorption of PFHxS was concentration dependent. The presence of inorganic anions slightly decreased the removal efficiency of PFHxS and the influence of different inorganic anions was similar due to multiple effects including competitive anion, screening effect, and salting-out effect in the adsorption process.

Abstract  Occurrence of per- and poly-fluoroalkyl substances (PFASs) in the environment and biota has raised a great concern to public health because these compounds are persistent, bioaccumulative, and toxic. Biodegradation of polyfluoroalkyl substances, particularly long-chain fluorotelomer-based products, can lead to production of various short-chain PFASs, with 5:3 fluorotelomer carboxylic acid (referred as 5:3 FTCA hereafter) as a dominant polyfluoroalkyl metabolite. Perfluoroalkyl acids, particularly perfluorooctanoic acid (PFOA), are toxic and current removal methods are not cost-effective. This study reports the photodegradation of 5:3 FTCA and PFOA using ZnO as a photocatalyst under neutral pH and room temperature conditions. Under long UV wavelength (365 nm), both tetrapod and commercial ZnO can photodegrade 5:3 FTCA. Five removal products-perfluorohexanoic acid, perfluoropentanoic acid, perfluorobutyric acid, 5:2 fluorotelomer carboxylic acid (5:2 FTCA), and inorganic fluoride-were identified, with PFBA and F- as dominant end products. SEM and XPS high-resolution scans on the surface of the utilized ZnO showed less units of CF2 than that in 5:3 FTCA, supporting occurrence of photodegradation of 5:3 FTCA by ZnO. Defluorination of PFOA was not observed with ZnO only, but at pH 5 and in the co-presence of Fe-citrate. PFOA defluorination increased from 0.93% after 3 days of UV light exposure to 3.9% after additional 135 h under direct sunlight exposure. To the authors' best knowledge, this is the first report studying ZnO-catalyzed photodegradation of 5:3 FTCA, and examining the Fe co-addition for PFOA defluorination.

Abstract  Exposure to chemicals may affect liver enzyme to increase the risk of liver diseases. Perfluoroalkyl acids (PFAAs) are one kind of persistent organic pollutants with hepatotoxic effect in organism. However, data is scarce to characterize the hepatotoxic effects of specific structural PFAA isomers in general population. To address this data gap, we evaluated the association between serum PFAAs concentration and liver function biomarkers in the Isomers of C8 Health Project in China. High performance liquid chromatography-tandem mass spectrometry (HPLC-MS/MS) was used to measure 18 serum PFAAs, except for linear and branched isomers of PFOA/PFOS, nine perfluorinated carboxylic acids (PFCAs) and two perfluorinated sulfonic acids (PFSAs) were also included, in 1605 adult residents of Shenyang, China. Values for nine serum liver function biomarkers were determined by full-automatic blood biochemical analyzer. Linear regression was used to evaluate associations between PFAAs and continuous liver function biomarkers and logistic regression to assess markers dichotomized per clinical reference intervals. Results indicated that serum PFAAs concentrations were associated with liver biomarker levels suggestive of hepatotoxicity, especially for liver cell injury. For example, a 1 ln-unit increase in total- perfluorooctanoic acid (PFOA) exposure was associated with a 7.4% [95% confidence interval (CI): 3.9%, 11.0%] higher alanine aminotransferase (ALT) level in serum. Interestingly, we observed association between branched PFAA isomers and liver biomarkers. For example, one ln-unit increase in branched perfluorooctane sulfonate (PFOS) isomers exposure was associated with a 4.3% increase in ALT level (95% CI: 1.2%, 7.4%) and a 33.0% increased odds of having abnormal ALT (95% CI: 5.0%, 67.0%). Also, we found that PFNA had positive association with ALT [(6.2%, 95% CI: 3.1%, 9.4%) and AST levels (2.5%, 95% CI: 0.5%, 4.5%)]. Logistic regression results showed that PFPeA, PFHxA, PFNA, PFDoDA, PFTrDA and PFTeDA had statistically association with abnormal prealbumin. Conclusively, our results support previous studies showing association between PFAAs exposure and liver function biomarkers. We found new evidence that branched PFAAs isomer exposure is associated with the risk of clinically relevant hepatocellular dysfunction.

Abstract  The extent of per- and polyfluoroalkyl substances (PFAS) in groundwater surrounding legacy landfills is currently poorly constrained. Seventeen PFAS were analysed in groundwater surrounding legacy landfills in a major Australian urban re-development precinct. Sampling locations (n = 13) included sites installed directly in waste material and down-gradient from landfills, some of which exhibited evidence of leachate contamination including elevated concentrations of ammonia-N (≤106 mg/L), bicarbonate (≤1,740 mg/L) and dissolved methane (≤10.4 mg/L). Between one and fourteen PFAS were detected at all sites and PFOS, PFHxS, PFOA and PFBS were detected in all samples. The sum of detected PFAS (∑14PFAS) varied from 26 ng/L at an ambient background site to 5,200 ng/L near a potential industrial point-source. PFHxS had the highest median concentration (34 ng/L; range: 2.6-280 ng/L) followed by PFOS (26 ng/L; range: 1.3-4,800 ng/L), PFHxA (19 ng/L; range:

Abstract  Perfluoroalkyl substances (PFASs) are widely-utilized synthetic chemicals commonly found in industrial and consumer products. Previous studies have examined associations between PFASs and renal function, yet the results are mixed. Moreover, evidence on the associations of isomers of PFASs with renal function in population from high polluted areas is scant. To help to address this data gap, we used high performance liquid chromatography-mass spectrometry to measure serum isomers of perfluorooctanoate (PFOA), perfluorooctanesulfonate (PFOS), and other PFASs from 1612 adults residing in Shenyang, China, and characterized their associations with estimated glomerular filtration rate (eGFR) and chronic kidney disease (CKD). Results showed that after adjusted for multiple confounding factors, most of the higher fluorinated PFASs, except for PFOA and PFDA, were negatively associated with eGFR and positively associated with CKD. Compared with linear PFOS (n-PFOS), branched PFOS isomers (Br-PFOS) were more strongly associated with eGFR (Br-PFOS; β = -1.22, 95%CI: 2.02, -0.42; p = 0.003 vs. n-PFOS; β = -0.16, 95%CI: 0.98, 0.65; p = 0.691) and CKD (Br-PFOS; OR = 1.27; 95% CI: 1.02, 1.58; p = 0.037 vs. n-PFOS; OR = 0.98; 95% CI: 0.80, 1.20; p = 0.834). In conclusion, branched PFOS isomers were negatively associated with renal function whereas their linear counterparts were not. Given widespread exposure to PFASs, potential nephrotoxic effects are of great public health concern, Furthermore, longitudinal research on the potential nephrotoxic effects of PFASs isomers will be necessary to more definitively assess the risk.

Abstract  Perfluorohexanoic acid (PFHxA) is a short-chain, six-carbon perfluoroalkyl acid (PFAA) and is a primary impurity, degradant, and metabolite associated with the short-chain fluorotelomer-based chemistry used globally today. The transition to short-chain fluorotelomer-based products as a cornerstone in replacement fluorochemistry has raised questions regarding potential human health risks associated with exposure to fluorotelomer-based substances and therefore, PFHxA. Here, we present a critical review of data relevant to such a risk assessment, including epidemiological studies and in vivo and in vitro toxicity studies that examined PFHxA acute, subchronic, and chronic toxicity. Key findings from toxicokinetic and mode-of-action studies are also evaluated. Sufficient data exist to conclude that PFHxA is not carcinogenic, is not a selective reproductive or developmental toxicant, and does not disrupt endocrine activity. Collectively, effects caused by PFHxA exposure are largely limited to potential kidney effects, are mild and/or reversible, and occur at much higher doses than observed for perfluorooctanoic acid (PFOA). A chronic human-health-based oral reference dose (RfD) for PFHxA of 0.25 mg/kg-day was calculated using benchmark dose modeling of renal papillary necrosis from a chronic rat bioassay. This RfD is four orders of magnitude greater than the chronic oral RfD calculated by the U.S. Environmental Protection Agency for PFOA. The PFHxA RfD can be used to inform public health decisions related to PFHxA and fluorotelomer precursors for which PFHxA is a terminal degradant. These findings clearly demonstrate that PFHxA is less hazardous to human health than PFOA. The analyses presented support site-specific risk assessments as well as product stewardship initiatives for current and future short-chain fluorotelomer-based products.

Abstract  Organic compounds could be taken up by plants via different pathways, depending on chemical properties and biological species, which is important for the risk assessment and risk control. To investigate the transport pathways of perfluoroalkyl acids (PFAAs) by wheat (Triticum acstivnm L.), the uptake of five perfluoroalkyl carboxylic acids (PFCAs): TFA (C2), PFPrA (C3), PFBA (C4), PFHxA (C6), PFOA (C8), and a perfluoroalkyl sulfonic acid: PFOS (C8)) were studied using hydroponic experiments. Various inhibitors including a metabolic inhibitor (Na3VO4), two anion channel blockers (9-AC, DIDS), and two aquaporin inhibitors (AgNO3, glycerol) were examined. The wheat root and shoot showed different concentration trends with the carbon chain length of PFAAs. The uptake of TFA was inhibited by Na3VO4 and 9-AC whereas PFPrA was inhibited by Na3VO4, AgNO3 and 9-AC. For the other four PFAAs, only Na3VO4 was effective. These results together with the result of concentration-dependent uptake, which followed the Michaelis-Menten model, indicate that the uptake of PFAAs by wheat is mainly an energy-dependent active process mediated by carriers. For the ultra-short chain PFCAs (C2 and C3), aquaporins and anion channels may also be involved. A competition between TFA and PFPrA was determined during the plant uptake but no competition was observed between these two shorter chain analogues with other analogues, neither between PFBA and PFHxA, PFBA and PFBS, PFOA and PFOS.

Abstract  Perfluoroalkyl acids (PFAAs) are a group of emerging persistent organic pollutants (POPs), which have been ubiquitously detected in the environmental media. However, national scale investigations on their occurrence and distribution in drinking water are still insufficient. In this study, we detected the 17 priority PFAAs in drinking water from 79 cities of 31 provincial-level administrative regions throughout China, and investigated their occurrence and distribution. Additionally, we also analyzed the influencing factors on their profiles, such as the existence of industrial sources, socioeconomic factors (population density and GDP), and assessed levels of risk associated with contaminated drinking water. On the national scale, the sum concentrations of the 17 PFAAs (∑17PFAAs) in drinking water was in a range of 4.49-174.93 ng/L with a mean value of 35.13 ng/L. Among the 17 individual PFAAs, perfluorobutanoic acids (PFBA) was the most abundant individual PFAAs with the median concentration of 17.87 ng/L, followed by perfluorooctanoic acid (PFOA, 0.74 ng/L), perfluorononanoic acid (PFNA, 0.40 ng/L) and perfluorooctane sulfonic acid (PFOS, 0.25 ng/L). The geographic distribution characteristic of ∑17PFAAs in drinking water was in a descending order of Southwestern China (57.67 ng/L) > Eastern coastal China (32.85 ng/L) > Middle China (29.89 ng/L) > Northwestern China (28.49 ng/L) > Northeastern China (22.03 ng/L), and in general, the existence of the industrial sources could positively affect the contamination levels of PFAAs in drinking water. The pollution level of PFAAs in drinking water also varied among the three different city levels (medium-sized city > big city > town). In towns, the positive correlations were observed between the population density and the ∑17PFAAs (R2 = 0.45, p < 0.01), and the individual concentration of PFHxA, PFBS, and PFOA (p < 0.01). Moreover, besides PFAAs in Yunnan, Jiangsu, and Jiangxi, concentrations of related PFAAs in drinking water from 28 provinces were less than the suggested drinking water advisories. The relatively higher concentrations of PFAAs in Yunnan, Jiangsu, and Jiangxi suggest that further studies focusing on their sources and potential health risk to humans are needed.

Abstract  In this perspective, we evaluate key and emerging epidemiological and toxicological data concerning immunotoxicity of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) and seek to reconcile conflicting conclusions from two reviews published in 2016. We summarize ways that immunosuppression and immunoenhancement are defined and explain how specific outcomes are used to evaluate immunotoxicity in humans and experimental animals. We observe that different approaches to defining immunotoxicological outcomes, particularly those that do not produce clinical disease, may lead to different conclusions from epidemiological and toxicological studies. The fundamental point that we make is that aspects of epidemiological studies considered as limitations can be minimized when data from toxicological studies support epidemiological findings. Taken together, we find that results of epidemiological studies, supported by findings from toxicological studies, provide strong evidence that humans exposed to PFOA and PFOS are at risk for immunosuppression.

Abstract  Background Residents of a large area of the Veneto Region (North-Eastern Italy) were exposed for decades to drinking water contaminated by perfluoroalkyl substances (PFAS). PFAS have been consistently associated with raised serum lipids, mainly in cross-sectional studies and in background exposure contexts, but the shape of the dose-response relationships has been poorly investigated. The objectives of our study were to evaluate the association between serum PFAS and serum lipids and their dose-response patterns in a large exposed population. Methods A cross-sectional study was conducted in 16,224 individuals aged 20–39 years recruited in the regional health surveillance program. 15,720 subjects were analysed after excluding pregnant women (n = 327), participants reporting use of cholesterol lowering medications (n = 67) or with missing information on the selected covariates (n = 110). Twelve PFAS were measured by HPLC-MS in serum; three (PFOA, PFOS and PFHxS) were quantifiable in at least 50% of samples. Non-fasting serum total cholesterol (TC), high-density lipoprotein cholesterol (HDL-C) and triglycerides were measured by enzymatic assays in automated analysers and low-density lipoprotein cholesterol (LDL-C), non-HDL cholesterol and total/HDL cholesterol ratio were calculated. The associations between natural log (ln) transformed PFAS and lipids were assessed through generalized additive models using linear regression and smoothing thin plate splines, adjusted for potential confounders. Results There were strong positive associations between the ln-transformed PFOA, PFOS, and PFHxS and TC, HDL-C, and LDL-C, and between ln PFOA and PFHxS and triglycerides. Each ln-increase in PFOA was associated with an increase of 1.94 mg/dL (95% CI 1.48–2.41) in TC, with 4.99 mg/dL (CI 4.12–5.86) for PFOS and 2.02 mg/dL (CI 1.45–2.58) for PFHxS. Conclusions Investigation of the shape of exposure-response associations using splines showed a positive association with the largest increases per unit of PFAS in cholesterol levels occurring at the lower range of PFAS concentrations for each compound. Previous article in issueNext article in issue

Abstract  BACKGROUND: Drinking water contamination related to the use of aqueous film-forming foam (AFFF) has been documented at hundreds of military bases, airports, and firefighter training facilities. AFFF has historically contained high levels of long-chain per- and polyfluoroalkyl substances(PFAS), which pose serious health concerns. However, the composition and toxicity of legacy AFFF mixtures are unknown, presenting great uncertainties in risk assessment and affected communities. OBJECTIVES: This study aimed to determine the fluorinated and nonfluorinated chemical composition of a legacy AFFF sample and its toxicity in zebrafish embryos. METHODS: A sample of legacy AFFF (3% application formulation, manufactured before 2001) was provided by the Massachusetts Department of Environmental Protection. High resolution mass spectrometry (HRMS) was used to identify PFAS and nonfluorinated compounds, and a commercial laboratory measured 24 PFAS by a modified U.S. EPA Method 537.1. AFFF toxicity was assessed in zebrafish embryos in comparison with four major constituents: perfluorooctanesulfonic acid (PFOS); perfluorohexanesulfonic acid (PFHxS); sodium dodecyl sulfate (SDS); and sodium tetradecyl sulfate (TDS). End points included LC50 values, and sublethal effects on growth, yolk utilization, and pancreas and liver development. RESULTS: We identified more than 100 PFAS. Of the PFAS detected, PFOS was measured at the highest concentration (9,410 mg=L) followed by PFHxS (1,500 mg=L). Fourteen nonfluorinated compounds were identified with dodecyl sulfate and tetradecyl sulfate the most abundant at 547.8 and 496:4 mg=L, respectively. An LC50 of 7:41 × 10−4% AFFF was calculated, representing a dilution of the 3% formulation. TDS was the most toxic of the constituents tested but could not predict the AFFF phenotype in larval zebrafish. PFOS exposure recapitulated the reduction in length but could not predict effects on development of the liver, which was the tissue most sensitive to AFFF. DISCUSSION: To our knowledge, this research is the first characterization of the chemical composition and toxicity of legacy AFFF, which has important implications for regulatory toxicology.

Abstract  Per- and polyfluoroalkyl substances (PFASs) are today considered important constituents of the continuously growing substance group of persistent contaminants of emerging environmental concern (PCEC). Here, we report for the first time the concentrations of 12 relevant PFASs in 28 marine water samples from the Saudi Arabian coastal waters of the Red Sea. The sum levels of 12 PFASs (sigma(12)PFAS) in surface seawater ranged from

Abstract  Persistent organic pollutants (POPs) including organochlorine pesticides, polychlorinated biphenyls (PCBs), and per- and polyfluoroalkylated substances (PFASs) are suspected endocrine disruptors.

Abstract  6:2 Fluorotelomer alcohol (6:2 FTOH) is a short-chain polyfluoroalkyl substance (PFAS) in polymeric PFAS used in fast food packaging and stain- and water-resistant textiles and may be degradation products of some components of aqueous film-forming foams (AFFF). The general population is exposed to 6:2 FTOH by inhalation of evaporates from treated surfaces or ambient concentrations in air, ingestion of indoor dust, or ingestion of food packaged in materials containing PFAS. Although exposure to 6:2 FTOH is pervasive, little is known concerning human health effects of this compound. Some published risk assessments have assumed that perfluorohexanoic acid (PFHxA), a metabolite of 6:2 FTOH, adequately models the human health effects of 6:2 FTOH. Recently identified studies conducted with 6:2 FTOH and its metabolite, 5:3 acid, have provided information that enables comparison of the toxicological profiles of PFHxA and 6:2 FTOH. This article summarizes a comparative analysis of the toxicological effects of PFHxA and 6:2 FTOH in rodents to determine whether data for PFHxA adequately models potential hazards of 6:2 FTOH exposure. Our analysis demonstrates that 6:2 FTOH is significantly more toxic than PFHxA. Use of toxicological studies conducted with PFHxA to assess 6:2 FTOH exposure may significantly underestimate human health risk.