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Background: In 2012, drinking water contaminated with per- and polyfluoroalkyl substances (PFASs), foremost perfluorooctanesulfonic acid (PFOS) and perfluorohexanesulfonic acid (PFHxS) at levels over 20ng/L and 40ng/L, respectively, was confirmed in Uppsala, Sweden., Objectives: We assessed how a longitudinally sampled cohort's temporal trend in PFAS plasma concentration was influenced by their residential location and determined the plausible association or disparity between the PFASs detected in the drinking water and the trend in the study cohort., Methods: The Prospective Investigation of the Vasculature in Uppsala Seniors (PIVUS) cohort provided plasma samples three times from 2001 to 2014. Individuals maintaining the same zip code throughout the study (n = 399) were divided into a reference (no known PFAS exposure), low, intermediate and high exposure area depending on the proportion of contaminated drinking water received. Eight PFASs detected in the majority (75%) of the cohort's plasma samples were evaluated for significant changes in temporal PFAS concentrations using a random effects (mixed) model., Results: PFHxS plasma concentrations continued to significantly increase in individuals living in areas receiving the largest percentage of contaminated drinking water (p < 0.0001), while PFOS showed an overall decrease. The temporal trend of other PFAS plasma concentrations did not show an association to the quality of drinking water received., Conclusions: The distribution of contaminated drinking water had a direct effect on the trend in PFHxS plasma levels among the different exposure groups, resulting in increased concentrations over time, especially in the intermediate and high exposure areas. PFOS and the remaining PFASs did not show the same relationship, suggesting other sources of exposure influenced these PFAS plasma trends., (Copyright © 2017 Elsevier Inc. All rights reserved.)

Background and Objective: During recent years, some persistent organic pollutants (POPs) have been linked to atherosclerosis. One group of POPs, the poly- and perfluoroalkyl substances (PFASs) have not been investigated with regard to atherosclerotic plaques., Methods: Carotid artery atherosclerosis was assessed by ultrasound in 1016 subjects aged 70 years in the Prospective Investigation of the Vasculature in Uppsala Seniors (PIVUS) study. Eight PFASs were detected in >75% of participants' plasma by ultra-performance liquid chromatography coupled to tandem mass spectrometry (UPLC-MS/MS)., Results: No significant linear associations were observed between the PFASs and intima-media thickness (IMT), or the echogenicity in the intima-media complex (IM-GSM, a marker of lipid infiltration in the artery) when men and women were analyzed together. Neither was occurrence of carotid plaques related to PFASs levels. However, highly significant interactions were observed between some PFASs and sex regarding both IM-GSM and plaque prevalence. Perfluorononanoic acid (PFNA), perfluorodecanoic acid (PFDA), and perfluoroundecanoic acid (PFUnDA), were all related to IM-GSM in a positive fashion in women (p=0.002-0.003), while these relationships were negative in men. The levels of PFUnDA were significantly related to carotid plaque in women (OR 1.59, 95%CI 1.03-2.43, p=0.03), but not in men (OR 0.93, 95%CI 0.62-1.42, p=0.75)., Conclusions: In this cross-sectional study, a pronounced gender difference was observed regarding associations between some PFASs, especially the long-chain PFUnDA, and markers of atherosclerosis, with more pronounced relationships found in women. These findings suggest a sex-specific role for PFASs in atherosclerosis., (Copyright © 2016 The Authors. Published by Elsevier Inc. All rights reserved.)

Background: In our daily life, we are exposed to perfluoroalkyl substances (PFAS) with possible health implications. The main exposure route for these substances is diet but comparative studies on how dietary habits influence exposure are lacking., Objectives: To examine the relations between blood levels of PFAS and adherence to three predefined dietary patterns (a WHO recommended diet, a Mediterranean-like diet, and a Low-Carbohydrate High-Protein (LCHP) diet) in an elderly Swedish population., Methods: Dietary data from 7-day food records and serum concentrations of PFAS were obtained from a 70-year-old Swedish population (n=844), the Prospective Investigation of the Vasculature in Uppsala Seniors (PIVUS) study. The Healthy Diet Indicator score (based on WHO recommendations), the Mediterranean Diet Score and LCHP score were used to assess adherence. Multivariate linear regression was used to assess the associations between eight major PFAS and adherence to each dietary pattern., Results: The WHO recommended diet was positively associated with perfluorohexane sulfonic acid (PFHxS). The LCHP diet was positively related to four out of eight PFAS; namely, perfluorooctane sulfonic acid (PFOS), perfluorononanoic acid (PFNA), perfluorodecanoic acid (PFDA) and perfluoroundecanoic acid (PFUnDA). The Mediterranean-like diet was positively associated with most PFAS; namely perfluorooctanoic acid (PFOA), perfluorooctane sulfonamide (PFOSA), PFHxS, PFNA, PFDA, and PFUnDA., Conclusions: All dietary patterns were positively associated with blood levels of PFAS. The highest body burden of PFAS was found in individuals with high adherence to a Mediterranean-like diet, whilst individuals who more closely followed the officially recommended diet displayed a lower body burden of these compounds., (Copyright © 2016 Elsevier Inc. All rights reserved.)

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 (C6-11) of fourteen (C4-13) 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., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

Per- and polyfluoroalkyl substances (PFASs) are a class of compounds with unique chemical properties that have been shown useful in a wide variety of applications because they provide materials with reduced surface tension and exceptional non-stick properties. PFASs are commonly found in impregnation materials, coatings of papers and textiles, fire-fighting foams, pesticides, and cleaning agents. The potential for human exposure to PFASs is high because of their widespread distribution. The aim of this study was to investigate levels of PFASs in men and women from Sweden and to assess the influence of gender and parity among women. Levels of 13 PFASs were determined in plasma samples collected during 2001-2004 from 1016 (507 women) 70year-old participants from the population-based Prospective Study of the Vasculature in Uppsala Seniors (PIVUS). The PFASs studied were nine perfluorinated carboxylic acids (PFCAs), four perfluorinated sulfonic acids (PFSAs) and perfluorooctane sulfonamide (PFOSA). In addition, structural isomers of perfluorooctane sulfonic acid (PFOS) were determined in a subset of 398 individuals. The detection rates were high and the majority of the studied compounds were detected in more than 75% of the participants. Levels of the selected analytes were found to be similar to other studies of non-occupationally exposed populations. Gender differences were observed in levels of PFHpA which was higher in men, while PFHxS was higher in women. Parity among women was shown to have a minor effect on PFAS concentrations and we found primi- and multiparous women to have slightly lower levels of PFUnDA when compared to nulliparous women., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Aims/hypothesis: Several environmental contaminants, such as polychlorinated biphenyls, dioxins, bisphenol A and phthalates, have been linked to diabetes. We therefore investigated whether other kinds of contaminants, perfluoroalkyl substances (PFAS), also called perfluorinated compounds (PFCs), are also associated with diabetes., Methods: The Prospective Investigation of the Vasculature in Uppsala Seniors (PIVUS) study investigated 1,016 men and women aged 70 years. Seven PFAS were detected in almost all participant sera by ultra-high performance liquid chromatograph/tandem mass spectrometry. Diabetes was defined as use of hypoglycaemic agents or fasting glucose >7.0 mmol/l., Results: 114 people had diabetes. In the linear analysis, no significant relationships were seen between the seven PFAS and prevalent diabetes. However, inclusion of the quadratic terms of the PFAS revealed a significant non-linear relationship between perfluorononanoic acid (PFNA) and diabetes, even after adjusting for multiple confounders (OR 1.96, 95% CI 1.19, 3.22, p = 0.008 for the linear term and OR 1.25, 95% CI 1.08, 1.44, p = 0.002 for the quadratic term). Perfluorooctanoic acid (PFOA) also showed such a relationship (p = 0.01). PFOA was related to the proinsulin/insulin ratio (a marker of insulin secretion), but none of the PFAS was related to the HOMA-IR (a marker of insulin resistance) following adjustment for multiple confounders., Conclusions/interpretation: PFNA was related to prevalent diabetes in a non-monotonic fashion in this cross-sectional study, supporting the view that this perfluoroalkyl substance might influence glucose metabolism in humans at the level of exposure seen in the general elderly population.

Perfluorinated alkyl acids (PFAAs) are emerging environmental contaminants. Possible health effects for humans include increased risk for cancer but the knowledge is limited. In this study serum concentrations of certain perfluorinated sulfonates (PFHxS and PFOS) and carboxylates (PFOA, PFNA, PFDA, PFUnDA) were analyzed among 201 cases with prostate cancer and 186 population based control subjects. All blood samples were collected during 2007-2011 and no case had been treated with radio- or chemotherapy before enrolment in the study. The blood concentrations did not differ statistically significant between cases and controls except for PFDA with higher concentration among the cases (p=0.03). Analyses based on Gleason score and prostate specific antigen (PSA) level did not change the results. Heredity was a risk factor for prostate cancer yielding odds ratio (OR)=1.8, 95% confidence interval (CI)=1.01-3.1. The analyzed PFAAs yielded statistically significant higher ORs in cases with a first degree relative reporting prostate cancer, e.g., PFOA gave OR=2.6, 95% CI=1.2-6.0 and PFOS gave OR=2.7, 95% CI=1.04-6.8. The results showed a higher risk for prostate cancer in cases with heredity as a risk factor. In further studies interaction between gene and environment should be considered., (© 2013.)

This study investigates the influence of biological and environmental factors on the concentrations of perfluoroalkyl acids (PFAAs) in a top predator; the American mink. Perfluorobutane sulfonate (PFBS), perfluorohexane sulfonate (PFHxS), perfluorooctane sulfonate (PFOS) and perfluoroalkyl carboxylates (PFCAs) with C8-C13 perfluorinated carbon chains were analyzed in livers from wild male mink liver (n=101) from four areas in Sweden representing two inland environments (rural and highly anthropogenic, respectively) and two different coastal environments. Mean PFOS concentrations were 1250ng/g wet weight and some mink from the urban inland area had among the highest PFOS concentrations ever recorded in mink (up to 21 800ng/g wet weight). PFBS was detected in 89% of the samples, but in low concentrations (mean 0.6ng/g ww). There were significant differences in PFAA concentrations between the geographical areas (p<0.001-0.01). Age, body condition and body weight did not influence the concentrations significantly, but there was a seasonal influence on the concentrations of perfluorodecanoic acid (PFDA) and perfluoroundecanoic acid (PFUnDA) (p<0.01 and p<0.05, respectively), with lower concentrations in autumn samples than in samples taken in the winter and spring. It is thus recommended to take possible seasonal differences into account when using mink exposure data. The overall results suggest that the mink is a suitable sentinel species for assessing and monitoring environmental levels of PFAAs., (© 2013. Published by Elsevier Ltd. All rights reserved.)

To facilitate high-throughput analysis suitable for large epidemiological studies we developed an automated column-switching ultra-performance liquid chromatography-tandem mass spectrometry (HPLC-MS/MS) method for determination of perfluorocarboxylic acids (PFCAs; C5, C6, C7, C8, C9, C10, C11, C12, and C13), perfluoroalkyl sulfonic acids (PFSAs; C4, C6, C8, and C10), perfluorooctane sulfonamide (PFOSA), and five groups of structural perfluorooctane sulfonic acid (PFOS) isomers in human serum or plasma. The analytical procedure involves rapid protein precipitation using 96-well plates followed by an automated sample clean-up using an on-line trap column removing many potentially interfering sample components while through the mobile phase gradient the target analytes are eluted onto the analytical column for further separation and subsequent mass detection. The method was linear (R(2)<0.995) at concentrations ranging from 0.01 to 60ngmL(-1) with method detection limits ranging between 0.01 and 0.17ngmL(-1) depending on the analyte. The developed method was precise, with repeatability (n=7) and reproducibility (n=103) coefficients of variation between 2% and 20% for most compounds including PFOS (2% and 8%) and its structural isomers (2-6% and 4-8%). The method was in conformity with a standard reference material. The column-switching HPLC-MS/MS method has been successfully applied for the determination of perfluoroalkyl substances including structural PFOS isomers in human plasma from an epidemiological study., (Copyright © 2013 Elsevier B.V. All rights reserved.)

Previous reports show that professional ski waxers have elevated blood levels of perfluorinated substances (PFAS) such as perfluorooctanoate (PFOA) and are exposed to very high concentrations of PFAS in air during ski waxing. Aerosol exposure increases the risk of cardiovascular disease, and PFOA is a potential hormonal disruptor and carcinogen, and can affect the fatty acid metabolism. Animal studies have shown that 8:2 FTOH can undergo biotransformation to PFOA. For the first time, this study presents an occupational scenario of professional ski waxers who are exposed to extremely high dust levels as well as per- and polyfluorinated compounds. Personal and fixed measurements of total aerosol, inhalable and respirable fractions were performed during World Cup events 2007-2010. The occupational exposure limit (OEL) is exceeded in 37% of the personal measurements with concentrations up to 15 mg m(-3) in air. There are differences between personal and area total aerosol concentrations with levels from personal measurements twice as high as those from the area measurements. The personal levels for FTOH ranged up to 996 μg m(-3) (mean = 114 μg m(-3)) and for PFOA up to 4.89 μg m(-3) (mean = 0.53 μg m(-3)) in ENV+ sorbent samples as compared to the general exposure levels from air reaching only low ng m(-3) (<30 ng m(-3)) levels. FTOHs were not detected in aerosols but PFOA showed an average level of 12 μg m(-3) (range = 1.2-47 μg m(-3)). The ski waxers' exposure to paraffin fumes and PFAS is not in compliance with the occupational exposure standards and by far exceed the general populations' exposure. Preventive measures must be taken to minimize the exposure in this occupational group.

Levels of perfluorocarboxylates (PFCAs) in biological compartments have been known for some time but their transport routes and distribution patterns are not properly elucidated. The opinions diverge whether the exposure of the general population occurs indirect through precursors or direct via PFCAs. Previous results showed that ski wax technicians are exposed to levels up to 92 000 ng/m(3) of 8:2 fluorotelomer alcohol (FTOH) via air and have elevated blood levels of PFCAs. Blood samples were collected in 2007-2011 and analyzed for C(4)-C(18) PFCAs, 6:2, 8:2 and 10:2 unsaturated fluorotelomer acids (FTUCAs) and 3:3, 5:3 and 7:3 fluorotelomer acids (FTCAs) using UPLC-MS/MS. Perfluorooctanoic acid (PFOA) was detected in levels ranging from 1.90 to 628 ng/mL whole blood (wb). Metabolic intermediates 5:3 and 7:3 FTCA were detected in all samples at levels up to 6.1 and 3.9 ng/mL wb. 6:2, 8:2 and 10:2 FTUCAs showed maximum levels of 0.07, 0.64 and 0.11 ng/mL wb. Also, for the first time levels of PFHxDA and PFOcDA were detected in the human blood at mean concentrations up to 4.22 ng/mL wb and 4.25 ng/mL wb respectively. The aim of this study was to determine concentrations of PFCAs and FTOH metabolites in blood from ski wax technicians., (Copyright © 2012 Elsevier Ltd. All rights reserved.)

In this study, the concentrations of 15 perfluorinated compounds (PFCs) were analyzed in 30 water samples collected in Catalonia (Spain) at three stages of the drinking water treatment process in several water purification plants. In addition, the concentrations of 13 PFCs were determined in samples of fish and shellfish collected from coastal areas of Catalonia. The intake of PFCs through both pathways, drinking water intake and fish and shellfish consumption, was also estimated. In water samples, the highest mean concentrations corresponded to perfluorooctane sulfonate (PFOS) and perfluorooctanoate (PFOA) (1.81 and 2.40 ng/L, respectively), whereas perfluorodecanosulfonate (PFDS) and perfluorotetradecanoic acid (PFTDA) were under their respective limits of detection in all analyzed samples. The results show that although the current treatment processes caused slight reductions in PFC concentrations, these processes did not mean significant changes in the amounts of PFCs already contained in the raw water. Among the analyzed PFCs in fish and shellfish, only seven compounds could be detected in at least one composite sample. PFOS showed the highest mean concentration (2.70 ng/g fw), being detected in all species with the exception of mussels. With regard to PFOA (mean, 0.074 ng/g fw), the highest concentrations were detected in prawn and hake (0.098 and 0.091 ng/g fw, respectively). The current exposure to PFCs through consumption of fish and shellfish indicates that it should not be of concern for the consumers. The amounts ingested are well below the recommended tolerable daily intakes, at least for those PFCs for which information is available.

Temporal variations in concentrations of perfluorinated carboxylic acids (PFCAs) and sulfonic acids (PFSAs), including perfluorooctane sulfonate (PFOS) and perfluorooctanoate (PFOA) structural isomers, were examined in livers of pilot whale (Globicephala melas), ringed seal (Phoca hisida), minke whale (Balaenoptera acutorostrata), harbor porpoise (Phocoena phocoena), hooded seal (Cystophora cristata), Atlantic white-sided dolphin (Lagenorhynchus acutus) and in muscle tissue of fin whales (Balaenoptera physalus). The sampling spanned over 20 years (1984-2009) and covered a large geographical area of the North Atlantic and West Greenland. Liver and muscle samples were homogenized, extracted with acetonitrile, cleaned up using hexane and solid phase extraction (SPE), and analyzed by liquid chromatography with negative electrospray tandem mass spectrometry (LC-MS/MS). In general, the levels of the long-chained PFCAs (C9-C12) increased whereas the levels of PFOS remained steady over the studied period. The PFOS isomer pattern in pilot whale liver was relatively constant over the sampling years. However, in ringed seals there seemed to be a decrease in linear PFOS (L-PFOS) with time, going from 91% in 1984 to 83% in 2006., (Copyright © 2011 Elsevier Ltd. All rights reserved.)

Perfluorinated compounds (PFCs) have been determined in 21 samples of selected food and beverages such as meat, fish, bread, vegetables, milk, drinking water and tea from the Norwegian marked. Up to 12 different PFCs were detected in the samples. Perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS) were found in concentrations similar to or lower than what has been observed in other studies world-wide. Differences in the relative proportion of PFOA and PFOS between samples of animal origin and samples of non-animal origin were observed and support findings that PFOS has a higher bioaccumulation potential in animals than PFOA. Based on these 21 measurements and consumption data for the general Norwegian population, a rough estimate of the total dietary intake of PFCs was found to be around 100 ng d(-1). PFOA and PFOS contributed to about 50% of the total intake. When dividing the population in gender and age groups, estimated intakes were decreasing with increasing age and were higher in males than females. The estimated intakes of PFOS and PFOA in the present study are lower than what has been reported in studies from Spain, Germany, United Kingdom, Canada and Japan. This study illustrates that by improving the analytical methods for determination of PFC in food samples, a broad range of compounds can be detected, which is important when assessing dietary exposure., (Copyright (c) 2010 Elsevier Ltd. All rights reserved.)

A time trend study focusing on ski waxing technicians' exposure to perfluorinated chemicals (PFCs) from fluorinated wax fumes was performed in 2007/2008. Levels of eight perfluorocarboxylates and three perfluorosulfonates were analyzed in monthly blood samples from eight technicians. Samples were collected before the ski season, i.e., preseason, then at four FIS World Cup competitions in cross country skiing, and finally during an unexposed 5-month postseason period. The perfluorinated carboxylates perfluoroheptanoic acid (PFHpA), perfluorooctanoic acid (PFOA), perfluorononanoic acid (PFNA), perfluorodecanoic acid (PFDA), and perfluoroundecanoic acid (PFUnDA) bioaccumulate, and continued exposure may contribute to elevated levels in ski technicians compared to the general population. The wax technicians' median blood level of PFOA is 112 ng/mL compared to 2.5 ng/mL in the general Swedish population. A significant correlation was found between number of working years and levels of perfluorocarboxylates. The PFOA levels in three technicians with "low" initial levels of PFOA (<10.0 ng/mL in preseason blood) increased by 254, 134, and 120%, whereas five technicians with "high" initial levels (>100 ng/mL in preseason sample) were at steady state. PFHxA is suggested to have a short half-life in humans relative the other perfluorocarboxylates. The levels of perfluorosulfonates were unaffected by the wax exposure.

Background, Aim and Scope: Perfluorinated compounds (PFCs) are global environmental pollutants that bioaccumulate in wildlife and humans. Laboratory experiments have revealed toxic effects such as delayed development, humoral suppression, and hepatotoxicity. Although numerous human blood levels have been reported, little is known about distribution in the human body. Knowledge about PFC distribution and accumulation in the human body is crucial to understanding uptake and subsequent effects as well as to conduct risk assessments. The present study reports PFC levels in human liver and breast milk from a general population living in Catalonia, Spain. Liver and milk levels are compared to previously reported levels in blood from the same geographic area as well as to other existing reports on human liver and milk levels in other countries., Materials and Methods: Human liver (n = 12) and milk (n = 10) samples were collected in 2007 and 2008 in Catalonia, Spain. Liver samples were taken postmortem from six males and six females aged 27-79 years. Milk samples were from healthy primipara women (30-39 years old). Both liver and milk were analyzed by solid-phase extraction and ultra-performance liquid chromatography tandem mass spectrometry., Results: Six PFCs were detected in liver, with perfluorooctanesulfonate (PFOS, 26.6 ng/g wet weight) being the chemical with the highest mean concentration. Other PFCs such as perfluorohexanesulfonate (PFHxS), perfluorooctanoic acid (PFOA), and acids with chain lengths up to C11 were also detected, with mean levels ranging between 0.50 and 1.45 ng/g wet weight. On the other hand, PFOS and PFHxS were the only PFCs detected in human milk, with mean concentrations of 0.12 and 0.04 ng/mL, respectively., Discussion: While milk concentrations were similar to reported levels from other countries, liver samples contained more PFCs above quantification limits and higher PFOS concentrations compared to the only two other reports found in the literature. Differences between the results of the present study and those concerning previous investigations can be due to declining levels of some PFCs, which have been reported for the USA. The relationship between PFC concentrations in human liver, milk, and blood was assessed using blood concentrations previously determined in Catalonia. Those levels resulted in liver/serum ratios of 1.7:1, 1.4:1, and 2.1:1 for PFOS, perfluorodecanoic acid, and perfluoroundecanoic acid, respectively. Accumulation in liver is suggested for PFOS and the perfluorocarboxylic acids with carbon chain lengths C9, C10, and C11. For PFOA and PFHxS, fivefold and 14-fold higher concentrations, respectively, were seen in serum as compared to liver. The mean concentration of PFOS and PFHxS in milk was only 0.8% and 0.6% of the reported mean serum level, respectively., Conclusions: The results of the present study show that several PFCs could be detected in human liver samples of subjects living in Tarragona. Concerning human milk, the mechanism by which PFCs are transferred from mother's blood to breast milk is still unclear. Considering that PFCs are strongly bound to the protein fraction in blood, the possibility of PFCs entering the milk and accumulating to levels observed in maternal plasma is limited., Recommendations and Perspectives: Interestingly, the potential accumulation difference for PFCs with different chain lengths might be of great importance for risk assessment. Continuing studies on the distribution of different PFCs in human tissue are therefore justified.

In this study, the concentrations of 13 perfluorinated compounds (PFCs) (PFBuS, PFHxS, PFOS, THPFOS, PFHxA, PFHpA, PFOA, PFNA, PFDA, PFUnDA, PFDoDA, PFTDA, and PFOSA) were analyzed in municipal drinking water samples collected at 40 different locations from 5 different zones of Catalonia, Spain. Detection limits ranged between 0.02 (PFHxS) and 0.85 ng/L (PFOA). The most frequent compounds were PFOS and PFHxS, which were detected in 35 and 31 samples, with maximum concentrations of 58.1 and 5.30 ng/L, respectively. PFBuS, PFHxA, and PFOA were also frequently detected (29, 27, and 26 samples, respectively), with maximum levels of 69.4, 8.55, and 57.4 ng/L. In contrast, PFDoDA and PFTDA could not be detected in any sample. The most contaminated water samples were found in the Barcelona Province, whereas none of the analyzed PFCs could be detected in two samples (Banyoles and Lleida), and only one PFC could be detected in four of the samples. Assuming a human water consumption of 2 L/day, the maximum daily intake of PFOS and PFOA from municipal drinking water would be, for a subject of 70 kg of body weight, 1.7 and 1.6 ng/kg/day. This is clearly lower than the respective Tolerable Daily Intake set by the European Food Safety Authority. In all samples, PFOS and PFOA also showed lower levels than the short-term provisional health advisory limit for drinking water (200 ng PFOS/L and 400 ng PFOA/L) set by the US Environmental Protection Agency. Although PFOS and PFOA concentrations found in drinking water in Catalonia are not expected to pose human health risks, safety limits for exposure to the remaining PFCs are clearly necessary, as health-based drinking water concentration protective for lifetime exposure is set to 40 ng/L for PFOA.

Perfluorinated chemicals (PFCs) are analyzed in laboratories worldwide to determine human blood levels and exposure pathways. The development of the analytical technique has been rapid in the last 10 years, and prerequisites for accurate and precise determination of PFCs in human blood at low ng/g concentrations are today readily available. The main contributing factors are the improved LC-MS instrumentations, the increased availability of native and mass labeled PFC standards, and new column materials available for chromatographic separations. The results of the first international interlaboratory study (ILS) in 2005 on PFCs revealed relatively better analytical results for human blood analyses when compared to analyses of a number of environmental matrices. The representative accuracy for the analyses of PFCs in human matrixes reported in recent years was established in the second human serum ILS in 2006. Interlaboratory standard deviations for the two human serum samples one low level concentration and one medium level concentration were found to be 12% and 16% for PFOS, respectively, and 47% and 21% for PFOA, respectively. Reported detections for all PFCs followed a frequency of PFOS>PFOA>PFHxS>PFNA>PFDA>>PFDoA>>PFDS>>PFHxA. Due to the small number of reported values for the other perfluorosulfonates and perfluorocarboxylates, standard deviations were not established.

Background, Aim, and Scope: In recent years, due to a high persistence, biomagnification in food webs, presence in remote regions, and potential toxicity, perfluorochemicals (PFCs) have generated a considerable interest. The present study was aimed to determine the levels of perfluorooctane sulfonate (PFOS), perfluorooctanoic acid (PFOA), and other PFCs in drinking water (tap and bottled) and river water samples from Tarragona Province (Catalonia, Spain)., Materials and Methods: Municipal drinking (tap) water samples were collected from the four most populated towns in the Tarragona Province, whereas samples of bottled waters were purchased from supermarkets. River water samples were collected from the Ebro (two samples), Cortiella, and Francolí Rivers. After pretreatment, PFC analyses were performed by HPLC-MS. Quantification was done using the internal standard method, with recoveries between 68% and 118%., Results: In tap water, PFOS and PFOA levels ranged between 0.39 and 0.87 ng/L (0.78 and 1.74 pmol/L) and between 0.32 and 6.28 ng/L (0.77 and 15.2 pmol/L), respectively. PFHpA, PFHxS, and PFNA were also other detected PFCs. PFC levels were notably lower in bottled water, where PFOS could not be detected in any sample. Moreover, PFHpA, PFHxS, PFOA, PFNA, PFOS, PFOSA, and PFDA could be detected in the river water samples. PFOS and PFOA concentrations were between <0.24 and 5.88 ng/L (<0.48 and 11.8 pmol/L) and between <0.22 and 24.9 ng/L (<0.53 and 60.1 pmol/L), respectively., Discussion: Assuming a human water consumption of 2 L per day, the daily intake of PFOS and PFOA by the population of the area under evaluation was calculated (0.78-1.74 and 12.6 ng, respectively). It was found that drinking water might be a source of exposure to PFCs as important as the dietary intake of these pollutants., Conclusions: The contribution of drinking water (tap and bottled) to the human daily intake of various PFCs has been compared for the first time with data from dietary intake of these PFCs. It was noted that in certain cases, drinking water can be a source of exposure to PFCs as important as the dietary intake of these pollutants although the current concentrations were similar or lower than those reported in the literature for surface water samples from a number of regions and countries., Recommendations and Perspectives: Further studies should be carried out in order to increase the knowledge of the role of drinking water in human exposure to PFCs.

The aim of this study was to determine the dietary intake of perfluorinated chemicals (PFCs) by the population of Tarragona County (Catalonia, Spain). PFC levels were determined in 36 composite samples of foodstuffs randomly purchased in various locations. Exposure to PFCs through the diet was estimated for various age/gender groups. Perfluorooctane sulfonate (PFOS), perfluorocarboxylate perfluorooctanoate (PFOA), and perfluoroheptanoic acid (PFHpA) were the only detected PFCs in foodstuffs. On average, for a standard adult man (70 kg of body weight), the dietary intake of PFOS was estimated to be 62.5 or 74.2 ng/day (assuming ND=0 or ND=1/2 LOD, respectively). Fish, followed by dairy products and meats, were the main contributors to PFOS intake. For an adult man, the intake of PFOS (1.07 ng/kg/day) and those of PFOA and PFHpA were lower than that recently reported for Canada (4.0 ng/kg/day), and considerably lower than that previously found in the United Kingdom, the only two countries where, to date, results concerning this issue have been reported. A correlation between dietary intake and blood levels of PFOS is suggested. However, the current results do not justify dietary intake as the main route of exposure governing blood concentrations of other PFCs.

Human serum and plasma from Sweden (n=17), the United Kingdom (the UK) (n=13) and Australia (n=40) were analyzed by high performance liquid chromatography coupled to mass spectrometry. The objective was to identify different perfluorooctane sulfonate (PFOS) isomers. Similar isomer patterns typical for the electrochemical fluorination (ECF) process were found for all samples. The linear PFOS (L-PFOS) was the major isomer found (58-70%) followed by the monosubstituted PFOS isomers 1/6-CF(3)-PFOS (18-22%) and 3/4/5-CF(3)-PFOS (13-18%). Disubstituted isomers were also detected. The percentage of L-PFOS found in the serum and plasma samples was lower compared to a standard PFOS product (76-79%). The pattern of PFOS isomers in human serum and plasma may be suggestive concerning potential isomeric discrimination since PFOS is only produced by ECF. Possibilities for such isomer discrimination are discussed. Significant higher content of L-PFOS (68%) in Swedish samples compared to Australia and the UK (59%) was also found, which may suggest differences in exposure sources for humans.

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.

Background: Only limited data exist on lactation as an exposure source of persistent perfluorinated chemicals (PFCs) for children., Objectives: We studied occurrence and levels of PFCs in human milk in relation to maternal serum together with the temporal trend in milk levels between 1996 and 2004 in Sweden. Matched, individual human milk and serum samples from 12 primiparous women in Sweden were analyzed together with composite milk samples (25-90 women/year) from 1996 to 2004., Results: Eight PFCs were detected in the serum samples, and five of them were also above the detection limits in the milk samples. Perfluorooctanesulfonate (PFOS) and perfluorohexanesulfonate (PFHxS) were detected in all milk samples at mean concentrations of 0.201 ng/mL and 0.085 ng/mL, respectively. Perfluorooctanesulfonamide (PFOSA), perfluorooctanoic acid (PFOA), and perfluorononanoic acid (PFNA) were detected less frequently., Discussion: The total PFC concentration in maternal serum was 32 ng/mL, and the corresponding milk concentration was 0.34 ng/mL. The PFOS milk level was on average 1% of the corresponding serum level. There was a strong association between increasing serum concentration and increasing milk concentration for PFOS (r(2) = 0.7) and PFHxS (r(2) = 0.8). PFOS and PFHxS levels in composite milk samples were relatively unchanged between 1996 and 2004, with a total variation of 20 and 32% coefficient of variation, respectively., Conclusion: The calculated total amount of PFCs transferred by lactation to a breast-fed infant in this study was approximately 200 ng/day. Lactation is a considerable source of exposure for infants, and reference concentrations for hazard assessments are needed.

The first worldwide interlaboratory study on the analyses of 13 perfluorinated compounds (PFCs) in three environmental and two human samples indicates a varying degree of accuracy in relation to the matrix or analyte determined. The ability of 38 participating laboratories from 13 countries to determine the analytes in the various matrices was evaluated by calculation of z-scores according to the Cofino model. The PFCs which were reported most frequently by the laboratories, and assessed with the most satisfactory agreement, were perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA). In general, the level of agreement between the participating laboratories decreased in the following order: PFC standard solution (76% satisfactory z-scores of <[2]1 for PFOS) < human blood (67%) < human plasma (63%) < fish liver extract (55%) < water (31%) < fish tissue (17%). This shows that relative good agreement between laboratories was obtained for the study of standard and human matrices. For the fish extract, most laboratories underestimated the actual PFOS concentration due to matrix effects. The results for the fish tissue and water are also poor, indicating that the extraction and cleanup steps require further improvement. It was concluded that the PFC determinations in various matrices are not yet fully mastered.

In order to evaluate blood levels of some perfluorinated chemicals (PFCs) and compare them to current levels of classical persistent organic pollutants (POPs) whole blood samples from Sweden were analyzed with respect to 12 PFCs, 37 polychlorinated biphenyls (PCBs), p,p'-dichlorodiphenyl-dichloroethylene (DDE), hexachlorobenzene (HCB), six chlordanes and three polybrominated diphenyl ethers (PBDEs). The median concentration, on whole blood basis, of the sum of PFCs was 20-50 times higher compared to the sum of PCBs and p,p'-DDE, 300-450 times higher than HCB, sum of chlordanes and sum of PBDEs. Estimations of the total body amount of PFCs and lipophilic POPs point at similar body burdens. While levels of for example PCBs and PBDEs are normalized to the lipid content of blood, there is no such general procedure for PFCs in blood. The distributions of a number of perfluorinated compounds between whole blood and plasma were therefore studied. Plasma concentrations were higher than whole blood concentrations for four perfluoroalkylated acids with plasma/whole blood ratios between 1.1 and 1.4, whereas the ratio for perflurooctanesulfonamide (PFOSA) was considerably lower (0.2). This suggests that the comparison of levels of PFCs determined in plasma with levels determined in whole blood should be made with caution. We also conclude that Swedish residents are exposed to a large number of PFCs to the same extent as in USA, Japan, Colombia and the few other countries from which data is available today.

Pooled serum samples from 3802 Australian residents were analyzed for four perfluoroalkylsulfonates, seven perfluoroalkylcarboxylates, and perfluorooctanesulfonamide (PFOSA). Serum was collected from men and women of five different age groups and from rural and urban regions in Australia. The highest mean concentration was obtained for perfluorooctane sulfonate (PFOS, 20.8 ng/mL) followed by perfluorooctanoic acid (PFOA, 7.6 ng/mL), perfluorohexane sulfonate (PFHxS, 6.2 ng/mL), perfluorononanoic acid (PFNA, 1.1 ng/mL), and PFOSA (0.71 ng/mL). Additional four PFCs were detected in 5-18% of the samples at concentrations near the detection limits (0.1-0.5 ng/mL). An increase in PFOS concentration with increasing age in both regions and genders was observed. The male pool levels of some of the age groups compared to females were higherfor PFOS, PFOA, and PFHxS. In contrast, PFNA concentrations were higher in the female pools. No substantial difference was found in levels of PFCs between the urban and rural regions. The levels are equal or higher than previously reported serum levels in Europe and Asia but lower compared to the U.S.A. These results suggest that emissions from production in the Northern Hemisphere are of less importance for human exposure.

A method for the determination of perfluorooctanesulfonate (PFOS) and perfluorooctanoic acid (PFOA) simultaneously with 10 closely related perfluorochemicals (PFCs) in human whole blood was developed and validated. PFOS and PFOA are used in various applications, for example, as surfactants and plastic additives, and are subject to environmental and health research due to their persistence. The main part of the data on PFCs in human blood is from serum samples, analyzed mainly by ion pair extraction followed by high-performance liquid chromatography (HPLC) and negative electrospray (ESI) tandem mass spectrometry (MS/MS). The analytical method developed here is suitable for human whole blood and involves solid-phase extraction (SPE) and HPLC negative electrospray single quadrupole mass spectrometry (HPLC/ES-MS). A whole blood aliquot was treated with formic acid and extracted on a octadecyl (C18) SPE column. The PFCs were isolated with methanol, and quantification was performed using single quadrupole mass spectrometry and perfluoroheptanoic acid as internal standard. Validation was performed in the range 0.3-194 ng/mL with recovery between 64 and 112% and limit of detection in the 0.1-0.5 ng/mL range for 11 of the 12 PFCs studied. We applied this method to 20 whole blood samples collected in 1997-2000 from the Swedish population in the ages 24-72. Eleven of the 12 PFCs were detected, and they were quantitatively and qualitatively confirmed using triple quadrupole LC/MS/MS analysis. PFOS, perfluorooctanesulfonamide, perfluorohexanesulfonate, PFOA and perfluorononanoic acid were quantified in all samples. In addition, perfluorohexanoic acid, perfluorodecanoic acid, perfluorodecanesulfonate, perfluoroundecanoic acid, perfluorododecanoic acid, and perfluorotetradecanoic acid were detected in some samples. This study shows that SPE and single quadrupole MS can be applied for extraction and quantification of PFCs in human whole blood, resulting in selectivity and low detection limits.