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  • 1.
    Aro, Rudolf
    et al.
    Örebro University, School of Science and Technology.
    Carlsson, Pernilla
    Norwegian Institute for Water Research (NIVA), Fram Centre, Tromsø, Norway.
    Vogelsang, Christian
    Norwegian Institute for Water Research (NIVA), Oslo, Norway.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Fluorine mass balance analysis of selected environmental samples from Norway2021In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 283, article id 131200Article in journal (Refereed)
    Abstract [en]

    The presence of unidentified organofluorine compounds (UOF) has been investigated in recent publication, but their environmental occurrence is still poorly understood. Fluorine mass balance analysis was performed on environmental samples from lake Mjøsa and river Alna (surface water (n = 9), sediment (n = 5) and fish liver (n = 4)) and sewage samples from Oslo (n = 5), to reveal to the fraction of UOF. In samples that had extractable organofluorine (EOF) concentrations above the limit of detection (LoD), more than 70% of their EOF could not be accounted for by the 37 PFAS monitored in this study. The surface water samples from lake Mjøsa had EOF concentrations several times higher than what has been reported elsewhere in Nordic nations. The flux of EOF in river Alna and selected sewage pipes revealed that it was 1-2 orders of magnitude higher than the flux of the measured PFAS. The elevated concentrations of EOF in all samples pose a potential health and environmental hazard, as their composition remains mostly unknown.

  • 2.
    Aro, Rudolf
    et al.
    Örebro University, School of Science and Technology.
    Eriksson, Ulrika
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Chen, Fangfang
    Man-Technology-Environment (MTM) Research Centre, School of Science and Technology, Örebro University, Örebro, Sweden.
    Wang, Thanh
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Fluorine Mass Balance Analysis of Effluent and Sludge from Nordic Countries2021In: ACS - ES & T Water, E-ISSN 2690-0637, Vol. 1, no 9, p. 2087-2096Article in journal (Refereed)
    Abstract [en]

    Recent publications have highlighted the ubiquitous presence of unidentified organofluorine compounds, whose environmental occurrence is poorly understood. In this study, wastewater treatment plant (WWTP) effluent and sludge samples from seven countries were analyzed for extractable organofluorine (EOF) and target PFAS, to evaluate which compounds are released back into the environment. Fluorine mass balance analysis of effluent samples (n = 14) revealed that on average 90% of the EOF could not be explained by the 73 PFAS monitored in this investigation. The levels of EOF in effluent (324–1460 ng of F/L) and sludge (39–210 ng of F/g of dry weight) indicate that a substantial amount of organofluorine compounds is released back into nature. A commonly overlooked PFAS class, ultra-short-chain PFCAs, accounted for 4% of EOF on average, while the remaining 71 compounds explained only a further 6% of EOF on average. The highest number of PFAS was detected in the effluent dissolved phase (37), compared to 29 and 23 PFAS in sludge and effluent particulate phase, respectively. The increased concentrations of EOF in both WWTP effluent and sludge are of concern, as the chemical species contained therein remain largely unknown, and thus, their potential health and environmental risks cannot be assessed.

  • 3.
    Aro, Rudolf
    et al.
    Örebro University, School of Science and Technology.
    Eriksson, Ulrika
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology. Man-Technology-Environment (MTM) Research Centre.
    Jakobsson, Kristina
    School of Public Health and Community Medicine, Institute of Medicine, University of Gothenburg, Gothenburg, Sweden.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Extractable organofluorine analysis: A way to screen for elevated per- and polyfluoroalkyl substance contamination in humans?2022In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 159, article id 107035Article in journal (Refereed)
    Abstract [en]

    The ubiquitous occurrence of a few per- and polyfluoroalkyl substances (PFAS) in humans and the environment has been previously reported. However, the number of PFAS humans and the environment are potentially exposed to is much higher, making it difficult to investigate every sample in detail. More importantly, recent studies have shown an increasing fraction of potentially unknown PFAS in human samples. A screening tool for identifying samples of concern that may contain high PFAS levels, to be studied more thoroughly, is needed. This study presents a simplified workflow to detect elevated PFAS levels using extractable organofluorine (EOF) analysis. A fluorine mass balance analysis on samples with high EOF, targeting 63 PFAS, can then confirm the PFAS contamination. Whole blood samples from a cohort of individuals with historical drinking water contamination from firefighting foams (n = 20) in Ronneby (Sweden) and a control group (n = 9) with background exposure were used as a case study. The average EOF concentration in the Ronneby group was 234 ng/mLF (<107-592 ng/mLF) vs 24.8 ng/mLF (17.6-37.8 ng/mL F) in the control group. The large difference (statistically significant, p < 0.05) in the EOF levels between the exposed and control groups would have made it possible to identify samples with high PFAS exposure only using EOF data. This was confirmed by target analysis, which found an average ∑PFAS concentration of 346 ng/mL in the exposed group and 7.9 ng/mL in the control group. The limit of quantification for EOF analysis (up to 107 ng/mLF using 0.5 mL whole blood) did not allow for the detection of PFAS levels in low or sub parts per billion (ng/mL) concentrations, but the results indicate that EOF analysis is a suitable screening method sensitive enough to detect elevated/significant/exposure above background levels by known or unknown PFAS.

  • 4.
    Aro, Rudolf
    et al.
    Örebro University, School of Science and Technology.
    Eriksson, Ulrika
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Jakobsson, Kristina
    School of Public Health and Community Medicine, Institute of Medicine, University of Gothenburg, Gothenburg, Sweden.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Extractable Organofluorine Analysis: a Way to Screen for Elevated Per- and Polyfluoroalkyl Substance Contamination in Humans?Manuscript (preprint) (Other academic)
  • 5.
    Aro, Rudolf
    et al.
    Örebro University, School of Science and Technology.
    Eriksson, Ulrika
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Reber, Iris
    Metrohm AG, Ionenstrasse, Herisau, Switzerland.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Combustion ion chromatography for extractable organofluorine analysis2021In: iScience, E-ISSN 2589-0042 , Vol. 24, no 9, article id 102968Article in journal (Refereed)
    Abstract [en]

    Combustion ion chromatography (CIC) has found a role in environmental analytical chemistry for fluorine content analysis. It is used for extractable organofluorine (EOF) analysis to evaluate perfluoroalkyl and polyfluoroalkyl substances (PFASs) and other organofluorine burden. The prevailing assumption has been that all PFASs are incinerated in CIC and matrix components have no impact on this process, but this has not been experimentally evaluated. In this work, the combustion efficiencies of 13 different PFASs were determined (66-110%). A notable difference was observed between calibrating the CIC with inorganic fluorine or organofluorine. Potential interferences from cations and coextracted matrix components from whole blood and surface water samples were evaluated. These observations should be acknowledged when performing EOF analysis using CIC, overlooking either non-100% combustion efficiencies or the differences in calibrating the CIC with inorganic fluorine or organofluorine could lead to underestimating EOF content and through that to misguide policy decisions.

  • 6.
    Aro, Rudolf
    et al.
    Örebro University, School of Science and Technology.
    Eriksson, Ulrika
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Reber, Iris
    Metrohm AG, Ionenstrasse, Herisau, Switzerland.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Combustion Ion Chromatography for Extractable Organofluorine AnalysisManuscript (preprint) (Other academic)
  • 7.
    Aro, Rudolf
    et al.
    Örebro University, School of Science and Technology.
    Eriksson, Ulrika
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Organofluorine Mass Balance Analysis of Whole Blood Samples in Relation to Gender and Age2021In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 55, no 19, p. 13142-13151Article in journal (Refereed)
    Abstract [en]

    Studies have highlighted the increasing fraction of unidentified organofluorine (UOF) compounds in human blood, whose health effects are not known. In this study, 130 whole blood samples from the Swedish general population were analyzed for extractable organofluorine (EOF) and selected per- and polyfluoroalkyl substances (PFAS). Organofluorine mass balance analysis revealed that 60% (0-99%) of the EOF in female samples could not be explained by the 63 monitored PFAS; in males, 41% (0-93%) of the EOF was of unidentified origin. Significant differences between both age groups and gender were seen, with the highest fraction of UOF in young females (70% UOF, aged 18-44), which is contrary to what has been reported in the literature for commonly monitored compounds (e.g., perfluorooctane sulfonic acid, PFOS). Increasing the number of monitored PFAS did not lead to a large decrease of the UOF fraction; the seven highest PFAS (C8-C11 PFCAs, C6-C8 PFSAs) accounted for 98% of sum 63 PFAS. The high fraction of UOF in human samples is of concern, as the chemical species of these organofluorine compounds remain unknown and thus their potential health risks cannot be assessed.

  • 8.
    Aro, Rudolf
    et al.
    Örebro University, School of Science and Technology.
    Eriksson, Ulrika
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Organofluorine Mass Balance Analysis of Whole Blood Samples in Relation to Gender and AgeManuscript (preprint) (Other academic)
  • 9.
    Bao, Jia
    et al.
    Sch Sci, Shenyang Univ Technol, Shenyang, Peoples R China.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    van Bavel, Bert
    Örebro University, School of Science and Technology.
    Jin, Yihe
    Sch Environm Sci & Technol, Key Lab Ind Ecol & Environm Engn MOE, Dalian Univ Technol, Dalian, Peoples R China.
    Perfluoroalkyl substances in the blood samples from a male population of Sweden2014In: Chinese Science Bulletin, ISSN 1001-6538, E-ISSN 1861-9541, Vol. 59, no 4, p. 388-395Article in journal (Refereed)
    Abstract [en]

    Temporal trends of perfluoroalkyl substances (PFASs) have been determined in the blood samples from several countries globally including a female population in Sweden recently, yet little is known about the time trends in the blood levels of these compounds in Swedish male populations over recent years. In this study, the fourteen target PFASs consisted of four perfluorosulfonates (PFSAs) and ten perfluorocarboxylates (PFCAs) in the whole blood samples, collected from 153 Swedish elderly men during the period between 2008 and 2010, were analyzed via ultra-performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS). As the dominant PFASs contaminants in the blood samples, perfluorooctane sulfonate (PFOS) showed the highest geometric mean (GM) at 8.5 ng/mL, ranging from 1.7 to 29 ng/mL, while blood perfluorooctanoic acid (PFOA) contained the GM of 1.8 ng/mL, ranging from 0.35 to 6.4 ng/mL. Both the levels of these two compounds were lower than those determined in the blood samples of Swedish elderly populations derived from the late 1990s. According to the temporal trend analysis, over the three years, the blood levels of PFOS in Swedish male populations declined 16 % per annum, while those of perfluoroundecanoic acid (PFUnDA) increased 6.1 % per annum, which were consistent with those reported previously for the populations from other countries.

  • 10. Berger, Urs
    et al.
    Kaiser, Mary A.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Barber, Jonathan L.
    van Leeuwen, Stefan P. J.
    Recent developments in trace analysis of poly- and perfluoroalkyl substances2011In: Analytical and Bioanalytical Chemistry, ISSN 1618-2642, E-ISSN 1618-2650, Vol. 400, no 6, p. 1625-1635Article in journal (Refereed)
    Abstract [en]

     Recent developments, improvements, and trends in the ultra-trace determination of per- and polyfluoroalkyl substances (PFASs) in environmental and human samples are highlighted and the remaining challenges and uncertainties are outlined and discussed. Understanding the analytical implications of such things as adsorption of PFASs to surfaces, effects of differing matrices, varying PFAS isomer response factors, potential bias effects of sampling, sample preparation, and analysis is critical to measuring highly fluorinated compounds at trace levels. These intricate analytical issues and the potential consequences of ignoring to deal with them correctly are discussed and documented with examples. Isomer-specific analysis and the development of robust multi-chemical methods are identified as topical trends in method development for an ever-increasing number of PFASs of environmental and human interest. Ultimately, the state-of-the-art of current analytical method accuracy is discussed on the basis of results from interlaboratory comparison studies.

  • 11.
    Bjurlid, Filip
    et al.
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Ricklund, Niklas
    Department of Occupational and Environmental Medicine, Örebro University Hospital, Örebro, Sweden.
    Hagberg, Jessika
    Örebro University, School of Science and Technology. Department of Occupational and Environmental Medicine, Faculty of Medicine and Health, Örebro University, Örebro, Sweden.
    Occurrence of brominated dioxins in a study using various firefighting methods2017In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 599-600, p. 1213-1221Article in journal (Refereed)
    Abstract [en]

    The use of different firefighting methods influences how fast a fire is extinguished and how fast the temperature drops in the area affected by the fire. These differences may also influence the formation of harmful pollutants during firefighting of an accidental fire. The aim was to study occurrence of brominated dibenzo-p-dioxins and furans (PBDD/Fs) in gas and soot during five fire scenarios resembling a small apartment fire and where different firefighting methods were used. Samples of gas and soot were taken both during the buildup of the fire and during the subsequent extinguishing of the fire while using different firefighting methods (nozzle, compressed air foam system, cutting extinguisher) and an extinguishing additive. New containers equipped with identical sets of combustible material were used for the five tests. The use of different firefighting methods and extinguishing additive induced variations in concentration and congener profiles of detected PBDD/Fs. The concentration range of Sigma PBDD/Fs in gas was 4020-18,700 pg/m(3), and in soot 76-4092 pg/m(2). PBDFs were the predominant congeners and 1,2,3,4,6,7,8-HpBDF was the most abundant congener. Chlorinated dibenzo-p-dioxins and furans (PCDD/Fs) were also monitored. The PBDD/Fs contributed with in average 97% to the total (PCDD/Fs plus PBDD/Fs) toxic equivalents, in soot and gas. During extinguishing, the shorter time the temperature was around 300 degrees C, the lower occurrence of PBDD/Fs. In the study the firefighting methods showed a difference in how effectively they induced a temperature decrease below 300 degrees C in the fire zone during quenching, where cutting extinguishing using additive and the compressed air foam system showed the fastest drop in temperature.

  • 12.
    Björnsdotter, Maria
    et al.
    Örebro University, School of Science and Technology.
    Hartz, William F.
    Department of Earth Sciences, University of Oxford, Oxford, United Kingdom; Department of Arctic Geology, University Centre in Svalbard (UNIS), Longyearbyen, Svalbard, Norway.
    Kallenborn, Roland
    Faculty of Chemistry, Biotechnology and Food Sciences (KBM), Norwegian University of Life Sciences (NMBU), Ås, Norway; Department of Arctic Technology, University Centre in Svalbard (UNIS), Longyearbyen, Svalbard, Norway.
    Ericson Jogsten, Ingrid
    Örebro University, School of Science and Technology.
    Humby, Jack D.
    Ice Dynamics and Paleoclimate, British Antarctic Survey, Cambridge, United Kingdom.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Levels and seasonal trends of C1-C4 perfluoroalkyl acids and the discovery of trifluoromethane sulfonic acid in surface snow in the ArcticManuscript (preprint) (Other academic)
  • 13.
    Björnsdotter, Maria
    et al.
    Örebro University, School of Science and Technology.
    Hartz, William F.
    Department of Earth Sciences, University of Oxford, South Parks Road, Oxford, United Kingdom; Department of Arctic Geology, University Centre in Svalbard (UNIS), Longyearbyen, Svalbard, Norway.
    Kallenborn, Roland
    Faculty of Chemistry, Biotechnology and Food Sciences (KBM), Norwegian University of Life Sciences (NMBU), Ås, Norway; Department of Arctic Technology, University Centre in Svalbard (UNIS), Longyearbyen, Svalbard, Norway.
    Ericson Jogsten, Ingrid
    Örebro University, School of Science and Technology.
    Humby, Jack D.
    Ice Dynamics and Paleoclimate, British Antarctic Survey, High Cross, Cambridge, United Kingdom.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Levels and Seasonal Trends of C1-C4 Perfluoroalkyl Acids and the Discovery of Trifluoromethane Sulfonic Acid in Surface Snow in the Arctic2021In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 55, no 23, p. 15853-15861Article in journal (Refereed)
    Abstract [en]

    C1-C4 perfluoroalkyl acids (PFAAs) are highly persistent chemicals that have been found in the environment. To date, much uncertainty still exists about their sources and fate. The importance of the atmospheric degradation of volatile precursors to C1-C4 PFAAs were investigated by studying their distribution and seasonal variation in remote Arctic locations. C1-C4 PFAAs were measured in surface snow on the island of Spitsbergen in the Norwegian Arctic during January-August 2019. Trifluoroacetic acid (TFA), perfluoropropanoic acid (PFPrA), perfluorobutanoic acid (PFBA), and trifluoromethane sulfonic acid (TFMS) were detected in most samples, including samples collected at locations presumably receiving PFAA input solely from long-range processes. The flux of TFA, PFPrA, PFBA, and TFMS per precipitation event was in the ranges of 22-1800, 0.79-16, 0.19-170, and 1.5-57 ng/m2, respectively. A positive correlation between the flux of TFA, PFPrA, and PFBA with downward short-wave solar radiation was observed. No correlation was observed between the flux of TFMS and solar radiation. These findings suggest that atmospheric transport of volatile precursors and their subsequent degradation plays a major role in the global distribution of C2-C4 perfluoroalkyl carboxylic acids and their consequential deposition in Arctic environments. The discovery of TFMS in surface snow at these remote Arctic locations suggests that TFMS is globally distributed. However, the transport mechanism to the Arctic environment remains unknown.

  • 14.
    Björnsdotter, Maria
    et al.
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Ericson Jogsten, Ingrid
    Örebro University, School of Science and Technology.
    Challenges in the analytical determination of ultra-short-chain perfluoroalkyl acids and implications for environmental and human health2020In: Analytical and Bioanalytical Chemistry, ISSN 1618-2642, E-ISSN 1618-2650, Vol. 412, p. 4785-4796Article, review/survey (Refereed)
    Abstract [en]

    Ultra-short-chain perfluoroalkyl acids have recently gained attention due to increasing environmental concentrations being observed. The most well-known ultra-short-chain perfluoroalkyl acid is trifluoroacetic acid (TFA) which has been studied since the 1990s. Potential sources and the fate of ultra-short-chain perfluoroalkyl acids other than TFA are not well studied and data reporting their environmental occurrence is scarce. The analytical determination of ultra-short-chain perfluoroalkyl acids is challenging due to their high polarity resulting in low retention using reversed-phase liquid chromatography. Furthermore, recent studies have reported varying extraction recoveries in water samples depending on the water matrix and different methods have been suggested to increase the extraction recovery. The present review gives an overview of the currently used analytical methods and summarizes the findings regarding potential analytical challenges. In addition, the current state of knowledge regarding TFA and other ultra-short-chain perfluoroalkyl acids, namely perfluoropropanoic acid, trifluoromethane sulfonic acid, perfluoroethane sulfonic acid, and perfluoropropane sulfonic acid‚ are reviewed. Both known and potential sources as well as environmental concentrations are summarized and discussed together with their fate and the environmental and human implications.

  • 15.
    Björnsdotter, Maria
    et al.
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Ericson Jogsten, Ingrid
    Örebro University, School of Science and Technology.
    Mass balance of perfluoroalkyl acids including trifluoroacetic acid in a freshwater lakeManuscript (preprint) (Other academic)
  • 16.
    Björnsdotter, Maria
    et al.
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Ericson Jogsten, Ingrid
    Örebro University, School of Science and Technology.
    Mass Balance of Perfluoroalkyl Acids, Including Trifluoroacetic Acid, in a Freshwater Lake2022In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 56, no 1, p. 251-259Article in journal (Refereed)
    Abstract [en]

    Perfluoroalkyl acids (PFAAs) are highly persistent chemicals that are ubiquitously found in the environment. The atmospheric degradation of precursor compounds has been identified as a source of PFAAs and might be an important pathway for contamination. Lake Vättern is one of Sweden's largest lakes and is an important source for drinking water. In addition to contamination via atmospheric deposition, the lake is subject to several potential contamination sources via surface water inflow. The relevance of different sources is not well understood. A mass balance of selected PFAAs was assembled based on measured concentrations in atmospheric deposition, surface water from streams that constitute the main inflow and outflow, and surface water in the lake. The largest input was seen for trifluoroacetic acid (150 kg/year), perfluoropropanoic acid (1.6 kg/year), perfluorobutanoic acid (4.0 kg/year), and perfluoro-octanoic acid (1.5 kg/year). Both atmospheric deposition and surface water inflow was found to be important input pathways. There was a positive correlation between the input of most perfluoroalkyl carboxylic acids via atmospheric deposition and global radiation and between the input via surface water inflow and catchment area. These findings highlight the importance of atmospheric oxidation of volatile precursor compounds for contamination in surface waters.

  • 17.
    Björnsdotter, Maria
    et al.
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Ericson Jogsten, Ingrid
    Örebro University, School of Science and Technology.
    Ultra-Short-Chain Perfluoroalkyl Acids Including Trifluoromethane Sulfonic Acid in Water Connected to Known and Suspected Point Sources in Sweden2019In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 53, no 19, p. 11093-11101Article in journal (Refereed)
    Abstract [en]

    Data presenting the environmental occurrence of ultra-short-chain perfluoroalkyl acids (PFAAs) are scarce and little is known about the potential sources. In this study, ultra-short-chain PFAAs were analyzed in water connected to potential point sources using supercritical fluid chromatography coupled with tandem mass spectrometry. Samples (n = 34) were collected in connection with firefighting training sites, landfills, and a hazardous waste management facility. Ultra-short-chain PFAAs were detected in all samples at concentrations up to 84 000 ng/L (∑C1-C3), representing up to 69% of the concentration of 29 per- and polyfluoroalkyl substances (PFASs). Trifluoroacetic acid (TFA), perfluoropropanoic acid (PFPrA), trifluoromethane sulfonic acid (TFMS), perfluoroethane sulfonic acid (PFEtS), and perfluoropropane sulfonic acid (PFPrS) were detected at concentrations up to 14 000, 53 000, 940, 1700, and 15 000 ng/L, respectively. Principal component analysis suggests that TFA is associated with landfills. PFPrS was associated with samples collected close to the source at all types of sites included in this study. These findings reveal the presence of high concentrations of ultra-short-chain PFAAs released into the environment from various sources and emphasize the large fraction of ultra-short-chain PFAAs to the total concentration of PFASs in water.

  • 18.
    Blanc, Mélanie
    et al.
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Kukučka, Petr
    Örebro University, School of Science and Technology.
    Scherbak, Nikolai
    Örebro University, School of Science and Technology.
    Keiter, Steffen
    Örebro University, School of Science and Technology.
    Mixture-specific gene expression in zebrafish (Danio rerio) embryos exposed to perfluorooctane sulfonic acid (PFOS), perfluorohexanoic acid (PFHxA) and 3,3′,4,4′,5-pentachlorobiphenyl (PCB126)2017In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 590-591, p. 249-257Article in journal (Refereed)
    Abstract [en]

    Perfluorooctane sulfonic acid (PFOS) and 3,3′,4,4′,5-pentachlorobiphenyl (PCB126) are persistent organic pollutants of high concern because of their environmental persistence, bioaccumulation and toxic properties. Besides, the amphiphilic properties of fluorinated compounds such as PFOS and perfluorohexanoic acid (PFHxA) suggest a role in increasing cell membrane permeability and solubilizing chemicals. The present study aimed at investigating whether PFOS and PFHxA are capable of modifying the activation of PCB126 toxicity-related pathways. For this purpose, zebrafish embryos were exposed in semi-static conditions to 7.5 μg/L of PCB126 alone, in the presence of 25 mg/L of PFOS, 15.7 mg/L of PFHxA or in the presence of both PFOS and PFHxA. Quantitative PCR was performed on embryos aged from 24 h post fertilization (hpf) to 96 hpf to investigate expression changes of genes involved in metabolism of xenobiotics (ahr2, cyp1a), oxidative stress (gpx1a, tp53), lipids metabolism (acaa2, osbpl1a), and epigenetic mechanisms (dnmt1, dnmt3ba). Cyp1a and ahr2 expression were significantly induced by the presence of PCB126. However, after 72 and 78 h of exposure, induction of cyp1a expression was significantly lower when embryos were co-exposed to PCB126 + PFOS + PFHxA when compared to PCB126-exposed embryos. Significant upregulation of gpx1a occurred after exposure to PCB126 + PFHxA and to PCB126 + PFOS + PFHxA at 30 and 48 hpf. Besides, embryos appeared more sensitive to PCB126 + PFOS + PFHxA at 78 hpf: acaa2 and osbpl1a were significantly downregulated; dnmt1 was significantly upregulated. While presented as environmentally safe, PFHxA demonstrated that it could affect gene expression patterns in zebrafish embryos when combined to PFOS and PCB126, suggesting that such mixture may increase PCB126 toxicity. This is of particular relevance since PFHxA is persistent and still being ejected into the environment. Moreover, it provides additional information as to the importance to integrate mixture effects of chemicals in risk assessment and biomonitoring frameworks.

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  • 19.
    Cormier, Bettie
    et al.
    Örebro University, School of Science and Technology. Bordeaux University, EPOC, Talence, France.
    Borchet, Flora
    RWTH Aachen, Institut für Umweltforschung (Biologie V), Aachen, Germany.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Szot, Marta
    School of Science and Technology, Örebro University, Sweden.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Keiter, Steffen
    Örebro University, School of Science and Technology.
    Sorption and desorption kinetics of PFOS to pristine microplastic2022In: Environmental Science and Pollution Research, ISSN 0944-1344, E-ISSN 1614-7499, Vol. 29, no 3, p. 4497-4507Article in journal (Refereed)
    Abstract [en]

    The sorption processes of persistent organic pollutants on microplastics particles are poorly understood. Therefore, the present study investigated the sorption processes of perfluorooctanesulfonate (PFOS) on polyethylene (PE) microplastic particles (MPs) which are representing a prominent environmental pollutant and one of the most abundant microplastic polymers in the aquatic environment, respectively. The focus was set on the investigation of the impact of the particle size on PFOS sorption using four different PE MPs size ranges. The sorption kinetics for 6 months was studied with one selected size range of PE MPs. Besides, the desorption of PFOS from PE MPs under simulated digestive conditions was carried out by using artificial gut fluid mimicking the intestinal juice of fish. The investigation of the size effects of particles over 6 months demonstrated a linear increase of PFOS concentration sorbed onto PE with a decrease of the particle size. Thus, our findings implicate efficient sorption of PFOS onto PE MPs of different sizes. The results showed that PFOS desorbed from the PE MPs into the artificial gut fluid with a rate of 70 to 80%. Besides, a longer exposure of PE MPs to PFOS leads to a higher concentration adsorbed by PE MPs, which may favor the ingestion of higher concentration of PFOS, and thus represents a higher risk to transfer relevant concentrations of PFOS during digestion.

  • 20.
    Cormier, Bettie
    et al.
    Örebro University, School of Science and Technology. Bordeaux University, EPOC, UMR CNRS University of Bordeaux EPHE 5805, Avenue des Facultés, Talence, France.
    Gambardella, Chiara
    Institute for the study of Anthropic Impacts and Sustainability in Marine Environment - National Research Council (CNR-IAS), Genova, Italy.
    Tato, Tania
    Faculty of Marine Sciences, University of Vigo, E-36310 Vigo, Galicia, Spain.
    Perdriat, Quentin
    Bordeaux University, EPOC, UMR CNRS University of Bordeaux EPHE 5805, Avenue des Facultés, Talence, France.
    Costa, Elisa
    Institute for the study of Anthropic Impacts and Sustainability in Marine Environment - National Research Council (CNR-IAS), Genova, Italy.
    Veclin, Cloé
    CNRS/University of Pau & Pays Adour/E2S UPPA, Institut des Sciences Analytiques et de Physicochimie pour l'Environnement et les Matériaux, Pau, France.
    Le Bihanic, Florane
    Bordeaux University, EPOC, UMR CNRS University of Bordeaux EPHE 5805, Avenue des Facultés, Talence, France.
    Grassl, Bruno
    CNRS/University of Pau & Pays Adour/E2S UPPA, Institut des Sciences Analytiques et de Physicochimie pour l'Environnement et les Matériaux, Pau, France.
    Dubocq, Florian
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Van Arkel, Kim
    Race for Water Foundation, Lausanne, Switzerlan.
    Lemoine, Soazig
    Laboratoire de biologie marine, Université des Antilles, French West Indies, Campus de Fouillole, Pointe-à-Pitre, France.
    Lagarde, Fabienne
    Institut des Molécules et Matériaux du Mans (IMMM, UMR CNRS 6283), Université du Maine, Avenu Olivier Messiaen, Le Mans, France.
    Morin, Bénédicte
    Bordeaux University, EPOC, UMR CNRS University of Bordeaux EPHE 5805, Avenue des Facultés, Talence, France.
    Garaventa, Francesca
    Institute for the study of Anthropic Impacts and Sustainability in Marine Environment - National Research Council (CNR-IAS), Genova, Italy.
    Faimali, Marco
    Institute for the study of Anthropic Impacts and Sustainability in Marine Environment - National Research Council (CNR-IAS), Genova, Italy.
    Cousin, Xavier
    MARBEC, University of Montpellier, CNRS, IFREMER, IRD, Palavas-les-Flots, France; University of Paris-Saclay, AgroParisTech, INRAE, GABI, Jouy-en-Josas, France..
    Bégout, Marie-Laure
    MARBEC, University of Montpellier, CNRS, IFREMER, IRD, Palavas-les-Flots, France.
    Beiras, Ricardo
    Faculty of Marine Sciences, University of Vigo, Vigo, Galicia, Spain.
    Cachot, Jérôme
    Bordeaux University, EPOC, UMR CNRS University of Bordeaux EPHE 5805, Avenue des Facultés, Talence, France.
    Chemicals sorbed to environmental microplastics are toxic to early life stages of aquatic organisms2021In: Ecotoxicology and Environmental Safety, ISSN 0147-6513, E-ISSN 1090-2414, Vol. 208, article id 111665Article in journal (Refereed)
    Abstract [en]

    Microplastics are ubiquitous in aquatic ecosystems, but little information is currently available on the dangers and risks to living organisms. In order to assess the ecotoxicity of environmental microplastics (MPs), samples were collected from the beaches of two islands in the Guadeloupe archipelago, Petit-Bourg (PB) located on the main island of Guadeloupe and Marie-Galante (MG) on the second island of the archipelago. These samples have a similar polymer composition with mainly polyethylene (PE) and polypropylene (PP). However, these two samples are very dissimilar with regard to their contamination profile and their toxicity. MPs from MG contain more lead, cadmium and organochlorine compounds while those from PB have higher levels of copper, zinc and hydrocarbons. The leachates of these two samples of MPs induced sublethal effects on the growth of sea urchins and on the pulsation frequency of jellyfish ephyrae but not on the development of zebrafish embryos. The toxic effects are much more marked for samples from the PB site than those from the MG site. This work demonstrates that MPs can contain high levels of potentially bioavailable toxic substances that may represent a significant ecotoxicological risk, particularly for the early life stages of aquatic animals.

  • 21.
    De Silva, Amila O.
    et al.
    Environment and Climate Change Canada, Burlington, ON, Canada.
    Armitage, James M.
    AES Armitage Environmental Sciences, Inc., Ottawa, ON, Canada.
    Bruton, Thomas A.
    Green Science Policy Institute, Berkeley, CA, USA.
    Dassuncao, Clifton
    Eastern Research Group, Inc. (ERG), Washington, DC, USA.
    Heiger-Bernays, Wendy
    Boston University School of Public Health, Boston, MA, USA.
    Hu, Xindi C.
    Mathematica, Inc., Oakland, CA, USA.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Kelly, Barry
    Simon Fraser University, Burnaby, BC, Canada.
    Ng, Carla
    University of Pittsburgh, Pittsburgh, PA, USA.
    Robuck, Anna
    University of Rhode Island, Graduate School of Oceanography, Narragansett, RI, USA.
    Sun, Mei
    University of North Carolina at Charlotte, Charlotte, NC, USA.
    Webster, Thomas F.
    Boston University School of Public Health, Boston, MA, USA.
    Sunderland, Elsie M.
    Harvard University, Cambridge, MA, USA.
    PFAS Exposure Pathways for Humans and Wildlife: A Synthesis of Current Knowledge and Key Gaps in Understanding2021In: Environmental Toxicology and Chemistry, ISSN 0730-7268, E-ISSN 1552-8618, Vol. 40, no 3, p. 631-657Article, review/survey (Refereed)
    Abstract [en]

    Here we synthesize current understanding of the magnitudes and methods for assessing human and wildlife exposures to poly- and perfluoroalkyl substances (PFAS). Most human exposure assessments have focused on two to five legacy PFAS and wildlife assessments are typically limited to targeted PFAS (up to ~30 substances). However, shifts in chemical production are occurring rapidly and targeted methods for detecting PFAS have not kept pace with these changes. Total fluorine (TF) measurements complemented by suspect screening using high resolution mass spectrometry are thus emerging as essential tools for PFAS exposure assessment. Such methods enable researchers to better understand contributions from precursor compounds that degrade into terminal perfluoroalkyl acids (PFAA). Available data suggest that diet is the major human exposure pathway for some PFAS but there is large variability across populations and PFAS compounds. Additional data on TF in exposure media and the fraction of unidentified organofluorine are needed. Drinking water has been established as the major exposure source in contaminated communities. As water supplies are remediated, and for the general population, exposures from dust, personal care products, indoor environments and other sources may be more important. A major challenge for exposure assessments is the lack of statistically representative population surveys. For wildlife, bioaccumulation processes differ substantially between PFAS and neutral lipophilic organic compounds, prompting a revaluation of traditional bioaccumulation metrics. There is evidence that both phospholipids and proteins are important for the tissue partitioning and accumulation of PFAS. New mechanistic models for PFAS bioaccumulation are being developed that will assist in wildlife risk evaluations.

  • 22. Domingo, Jose L.
    et al.
    Ericson-Jogsten, Ingrid
    Örebro University, School of Science and Technology.
    Perello, Gemma
    Nadal, Marti
    van Bavel, Bert
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Human exposure to perfluorinated compounds in Catalonia, Spain: contribution of drinking water and fish and shellfish2012In: Journal of Agricultural and Food Chemistry, ISSN 0021-8561, E-ISSN 1520-5118, Vol. 60, no 17, p. 4408-4415Article in journal (Refereed)
    Abstract [en]

    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.

  • 23.
    Dubocq, Florian
    et al.
    Örebro University, School of Science and Technology.
    Bergdís Björk, Bergdís Björk
    Örebro University, Örebro, Sweden.
    Wang, Thanh
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Comparison of extraction and clean-up methods for comprehensive screening of organic micropollutants in fish using gas chromatography coupled to high-resolution mass spectrometry2022In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 286, no Pt 3, article id 131743Article in journal (Refereed)
    Abstract [en]

    Monitoring the vast number of micropollutants in the environment by using comprehensive chemical screening is a major analytical challenge. The aim of this study was to evaluate a comprehensive analysis method for screening purposes of fish muscle samples by comparing sample preparation methods for a broad range of mid-to non-polar contaminants. Five extraction and three clean-up methods were evaluated for the analysis of 60 compounds with a log Kow range between 0.8 and 8.3 in fish. Both fresh and freeze-dried muscle tissue and extraction sodium sulphate blanks were included to assess recoveries and matrix effects. The performance of the different methods was evaluated using both comprehensive target and nontarget analysis using high resolution mass spectrometry (HRMS). The results showed that open-column and ultrasonication extractions (recoveries mostly between 20 and 160 %) resulted in higher recoveries than accelerated solvent extraction (ASE) (recoveries mostly between 20 and 80 %) and bead mixer homogenization extractions (recoveries between 0 and 50 % for the whole Kow range). Multilayer silica was the clean-up method resulting in the lowest matrix effects and highest recoveries, however some compounds (mostly pesticides) were denatured under the acidic conditions used. The convenient and time efficient ultrasonication extraction followed by deactivated silica clean-up proved to be promising for both target and nontarget approaches. The large difference in recoveries and number of detected peaks using target and nontarget approaches between fresh and freeze-dried fish seen for all methods calls for careful consideration, and further studies are needed to improve performance for screening of mid-to non-polar compounds in freeze-dried fish.

  • 24.
    Dubocq, Florian
    et al.
    Örebro University, School of Science and Technology.
    Bjurlid, Filip
    Örebro University, School of Science and Technology.
    Ydstål, D.
    Örebro University, Örebro, Sweden.
    Titaley, I. A.
    Örebro University, Örebro, Sweden.
    Reiner, E.
    Ontario Ministry of the Environment, Conservation and Parks, Toronto, ON, Canada .
    Wang, Thanh
    Örebro University, School of Science and Technology.
    Almirall, X. O.
    Ontario Ministry of the Environment, Conservation and Parks, Toronto, ON, Canada; Queen’s University, School of Environmental Sciences, St., Kingston, ON, Canada.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Organic contaminants formed during fire extinguishing using different firefighting methods assessed by nontarget analysis2020In: Environmental Pollution, ISSN 0269-7491, E-ISSN 1873-6424, Vol. 265, article id 114834Article in journal (Refereed)
    Abstract [en]

    During a fire event, potentially hazardous chemicals are formed from the combustion of burning materials and are released to the surrounding environment, both via gas and soot particles. The aim of this investigation was to study if firefighting techniques influence the emission of chemicals in gas phase and soot particles. Five full-scale fire tests were extinguished using four different firefighting techniques. A nontarget chemical analysis approach showed that important contaminants in gas and soot separating the different tests were brominated flame retardants (BFRs), organophosphate flame retardants (OPFR), polycyclic aromatic hydrocarbons (PAHs) and linear hydrocarbons. Reproducibility was evaluated by a field replicate test and it was determined that the temperature curve during the event had a bigger impact on the released chemicals than the firefighting technique used. However, despite fire intensity being a confounding factor, multivariate statistics concluded that water mist with additive resulted in less BFR emissions compared to foam extinguishing. The analysis also showed that the conventional spray nozzle method released more PAHs compared with the water mist method. The comprehensive chemical analysis of gas and soot released during fire events was able to show that different firefighting techniques influenced the release of chemicals. 

  • 25.
    Dubocq, Florian
    et al.
    Örebro University, School of Science and Technology.
    Bæringsdóttir, Bergdís Björk
    Örebro University, Örebro, Sweden.
    Wang, Thanh
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Comparing extraction methods for comprehensive screening of organic micropollutants in fish using gas chromatography coupled to high-resolution mass spectrometryManuscript (preprint) (Other academic)
  • 26.
    Dubocq, Florian
    et al.
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Gustavsson, Jakob
    Örebro University, Örebro, Sweden.
    Wang, Thanh
    Örebro University, School of Science and Technology.
    Comprehensive chemical characterization of indoor dust by target, suspect screening and nontarget analysis using LC-HRMS and GC-HRMS2021In: Environmental Pollution, ISSN 0269-7491, E-ISSN 1873-6424, Vol. 276, article id 116701Article in journal (Refereed)
    Abstract [en]

    Since humans spend more than 90% of their time in indoor environments, indoor exposure can be an important non-dietary pathway to hazardous organic contaminants. It is thus important to characterize the chemical composition of indoor dust to assess the total contaminant exposure and estimate human health risks. The aim of this investigation was to perform a comprehensive chemical characterization of indoor dust. First, the robustness of an adopted extraction method using ultrasonication was evaluated for 85 target compounds. Thereafter, a workflow combining target analysis, suspect screening analysis (SSA) and nontarget analysis (NTA) was applied to dust samples from different indoor environments. Chemical analysis was performed using both gas chromatography and liquid chromatography coupled with high resolution mass spectrometry. Although suppressing matrix effects were prominent, target analysis enabled the quantification of organophosphate/brominated flame retardants (OPFRs/BFRs), liquid crystal monomers (LCMs), toluene diisocyanate, bisphenols, pesticides and tributyl citrate. The SSA confirmed the presence of OPFRs but also enabled the detection of polyethylene glycols (PEGs) and phthalates/parabens. The combination of hierarchical cluster analysis and scaled mass defect plots in the NTA workflow confirmed the presence of the above mentioned compounds, as well as detect other contaminants such as tetrabromobisphenol A, triclocarban, diclofenac and 3,5,6-trichloro-2-pyridinol, which were further confirmed using pure standards.

  • 27.
    Dubocq, Florian
    et al.
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Gustavsson, Jakob
    Örebro University, School of Science and Technology.
    Wang, Thanh
    Örebro University, School of Science and Technology.
    Comprehensive chemical characterization of indoor dust by target, suspect screening and nontarget analysis using liquid chromatography and gas chromatography coupled with high resolution mass spectrometryManuscript (preprint) (Other academic)
  • 28.
    Dubocq, Florian
    et al.
    Örebro University, School of Science and Technology.
    Wang, Thanh
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Sjöberg, Viktor
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Characterization of the Chemical Contents of Fluorinated and Fluorine-Free Firefighting Foams Using a Novel Workflow Combining Nontarget Screening and Total Fluorine Analysis2020In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 54, no 1, p. 245-254Article in journal (Refereed)
    Abstract [en]

    Aqueous film-forming foams (AFFFs) are widely used to extinguish liquid fires due to their film-forming properties. AFFF formulation historically contains per- and polyfluoroalkyl substances (PFASs) that can be very persistent and pose a health risk to biota and humans. Detailed analysis of the chemical composition of AFFFs can provide a better understanding on the potential environmental impact of the ingredients. In this study, a novel workflow combining target analysis, nontarget screening analysis (NTA), total fluorine (TF) analysis, and inorganic fluoride (IF) analysis was applied to disclose the chemical composition of 24 foams intended for liquid fires. Foams marketed as containing PFASs as well as fluorine-free foams were included. By comparing the sum of targeted PFASs and total organofluorine concentrations, a mass balance of known and unknown organofluorine could be calculated. Known organofluorine accounted for <1% in most fluorine-containing AFFFs, and it was confirmed that the foams marketed as fluorine-free did not contain measurable amounts of organofluorine substances. Five fluorinated substances were tentatively identified, and non-fluorinated zwitterionic betaine compounds, which are considered to be replacement substances for PFASs, were tentatively identified in the organofluorine-free foams.

  • 29.
    Dunder, Linda
    et al.
    Department of Medical Sciences, Occupational and Environmental Medicine, Uppsala University, Uppsala, Sweden.
    Lind, P. Monica
    Department of Medical Sciences, Occupational and Environmental Medicine, Uppsala University, Uppsala, Sweden.
    Salihovic, Samira
    Örebro University, School of Medical Sciences. Department of Medical Sciences.
    Stubleski, Jordan
    School of Science and Technology, Örebro University, Örebro, Sweden; Wellington Laboratories Inc, Guelph, ON, Canada.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Lind, Lars
    Department of Medical Sciences, Cardiovascular Epidemiology, Uppsala University, Uppsala, Sweden.
    Changes in plasma levels of per- and polyfluoroalkyl substances (PFAS) are associated with changes in plasma lipids: A longitudinal study over 10 years2022In: Environmental Research, ISSN 0013-9351, E-ISSN 1096-0953, Vol. 211, article id 112903Article in journal (Refereed)
    Abstract [en]

    BACKGROUND: Associations between per- and polyfluoroalkyl substances (PFAS), mainly PFOS and PFOA, and increased blood lipids have been reported primarily from cross-sectional studies. The aim of the present study was to investigate associations between multiple PFAS and blood lipids in a longitudinal fashion.

    METHODS: A total of 864 men and women aged 70 years and free from lipid medication were included from the PIVUS study, 614 and 404 of those were reinvestigated at age 75 and 80. At all three occasions, eight PFAS were measured in plasma using ultra-performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS). Total cholesterol, triglycerides, low-density lipoprotein cholesterol (LDL-C) and high-density lipoprotein cholesterol (HDL-C) were also measured in plasma at all three occasions. Mixed-effects linear regression models were used to examine the relationship between the changes in PFAS levels and changes in lipid levels.

    RESULTS: Changes in plasma levels of six out of the eight investigated PFAS were positively associated with changes in plasma lipids after adjustment for sex, change in body mass index (BMI), smoking, physical activity, statin use (age was the same in all subjects), and correction for multiple testing. For example, changes in perfluorodecanoic acid (PFDA) were positively associated with the changes in total cholesterol (β: 0.23, 95% confidence interval (CI): 0.14 to 0.32), triglycerides (β: 0.08, 95% CI: 0.04-0.12) and HDL-cholesterol (β: 0.08, 95% CI: 0.04-0.11).

    CONCLUSION: In this longitudinal study with three measurements over 10 years of both plasma PFAS and lipids, changes in six out of the eight investigated PFAS were positively associated with changes in plasma lipids, giving further support for a role of PFAS exposure in human lipid metabolism.

  • 30.
    Ericson Jogsten, Ingrid
    et al.
    Örebro University, School of Science and Technology.
    Perelló, Gemma
    Laboratory of Toxicology and Environmental Health, School of Medicine, Institut d’Investigacions Sanitàries Pere Virgili, “Rovira i Virgili” University, Sant Llorenç 21, 43201 Reus, Spain.
    Llebaria, Xavier
    Health Protection Agency, Department of Health, Generalitat de Catalunya, Roc Boronat 81-95, Barcelona, Spain.
    Bigas, Esther
    Health Protection Agency, Department of Health, Generalitat de Catalunya, Roc Boronat 81-95, Barcelona, Spain.
    Martí-Cid, Roser
    Laboratory of Toxicology and Environmental Health, School of Medicine, Institut d’Investigacions Sanitàries Pere Virgili, “Rovira i Virgili” University, Sant Llorenç 21, 43201 Reus, Spain.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Domingo, José L.
    Laboratory of Toxicology and Environmental Health, School of Medicine, Institut d’Investigacions Sanitàries Pere Virgili, “Rovira i Virgili” University, Sant Llorenç 21, 43201 Reus, Spain.
    Exposure to perfluorinated compounds in Catalonia, Spain, through consumption of various raw and cooked foodstuffs, including packaged food2009In: Food and Chemical Toxicology, ISSN 0278-6915, E-ISSN 1873-6351, Vol. 47, no 7, p. 1577-1583Article in journal (Refereed)
    Abstract [en]

    In this study, the role that some food processing and packaging might play as a source of perfluorinated compounds (PFCs) through the diet was assessed. The levels of PFCs were determined in composite samples of veal steak (raw, grilled, and fried), pork loin (raw, grilled, and fried), chicken breast (raw, grilled, and fried), black pudding (uncooked), liver lamb (raw), marinated salmon (home-made and packaged), lettuce (fresh and packaged), pate of pork liver, foie gras of duck, frankfurt, sausages, chicken nuggets (fried), and common salt. Among the 11 PFCs analyzed, only PFHxS, PFOS, PFHxA, and PFOA were detected in at least one composite sample, while the levels of the remaining PFCs (PFBuS, PFHpA, PFNA, PFDA, PFUnDA, and PFDoDA) were under their respective detection limits. PFOS was the compound most frequently detected, being found in 8 of the 20 food items analyzed, while PFHxA was detected in samples of raw veal, chicken nuggets, frankfurt, sausages, and packaged lettuce. According to the results of the present study, it is not sufficiently clear if cooking with non-stick cookware, or packaging some foods, could contribute to a higher human exposure to PFCs.

  • 31.
    Eriksson, Ulrika
    et al.
    Örebro University, School of Science and Technology.
    Haglund, Peter
    Department of Chemistry, Umeå University, Umeå, Sweden.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Contribution of precursor compounds to the release of per- and polyfluoroalkyl substances (PFASs) from waste water treatment plants (WWTPs)2017In: Journal of Environmental Sciences(China), ISSN 1001-0742, E-ISSN 1878-7320, Vol. 61, p. 80-90Article in journal (Refereed)
    Abstract [en]

    Per- and polyfluoroalkyl substances (PFASs) are ubiquitous in sludge and water from waste water treatment plants, as a result of their incorporation in everyday products and industrial processes. In this study, we measured several classes of persistent PFASs, precursors, transformation intermediates, and newly identified PFASs in influent and effluent sewage water and sludge from three municipal waste water treatment plants in Sweden, sampled in 2015. For sludge, samples from 2012 and 2014 were analyzed as well. Levels of precursors in sludge exceeded those of perfluoroalkyl acids and sulfonic acids (PFCAs and PFSAs), in 2015 the sum of polyfluoroalkyl phosphoric acid esters (PAPs) were 15-20ng/g dry weight, the sum of fluorotelomer sulfonic acids (FTSAs) was 0.8-1.3ng/g, and the sum of perfluorooctane sulfonamides and ethanols ranged from non-detected to 3.2ng/g. Persistent PFSAs and PFCAs were detected at 1.9-3.9ng/g and 2.4-7.3ng/g dry weight, respectively. The influence of precursor compounds was further demonstrated by an observed substantial increase for a majority of the persistent PFCAs and PFSAs in water after waste water treatment. Perfluorohexanoic acid (PFHxA), perfluorooctanoic acid (PFOA), perfluorohexane sulfonic acid (PFHxS), and perfluorooctane sulfonic acid (PFOS) had a net mass increase in all WWTPs, with mean values of 83%, 28%, 37% and 58%, respectively. The load of precursors and intermediates in influent water and sludge combined with net mass increase support the hypothesis that degradation of precursor compounds is a significant contributor to PFAS contamination in the environment.

  • 32.
    Eriksson, Ulrika
    et al.
    Örebro University, School of Science and Technology.
    Haglund, Peter
    Umeå University, Umeå, Sweden.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Contribution of precursor compounds to the release of per- and polyfluoroalkyl substances (PFASs) from waste water treatment plants (WWTPs)Manuscript (preprint) (Other academic)
  • 33.
    Eriksson, Ulrika
    et al.
    Örebro University, School of Science and Technology.
    Haglund, Peter
    Umeå universitet, Kemiska institutionen.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Screening of PFASs in sludge and water from waste water treatment plants2017Report (Other academic)
    Abstract [en]

    The purpose of this study was to assess the contribution from precursor compounds to the total amount of selected PFASs in water and sludge from Swedish waste water treatment plants, as a supplemental to previous studies of two persistent PFAS-classes; perfluorocarboxylic acids (PFCAs) and perfluorosulfonic acids (PFSAs). Compound classes added in this study were fluorotelomer sulfonic acids (FTSAs), polyfluoroalkyl phosphoric acid esters (PAPs), perfluoroalkyl phosphonic and phosphinic acids (PFPAs, PFPiAs), perfluoralkane sulfonamides (FOSAs), and sulfonamido ethanols (FOSEs), and also the intermediates fluorotelomer unsaturated carboxylic acids (FTUCAs) and the stable transformation products fluorotelomer carboxylic acids (FTCAs). Three waste water treatment plants were included; Gässlösa (Borås), Henriksdal (Stockholm) and Umeå. PFAS levels in sludge from 2012. 2014, and 2015, and in filtered effluent and influent water from 2015 are reported. Precursor compounds were detected in sludge and influent water from all three WWTPs. Levels of precursor compounds in sludge samples exceeded those of persistent PFASs. Increasing PFCA levels in the effluent water compared to the influent water was observed, especially for the short-chained PFCAs. Occurrence of precursor compounds in influent water and sludge indicate degradation of precursor compounds to persistent PFASs.

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    Screening of PFASs in sludge and water from waste water treatment plants
  • 34.
    Eriksson, Ulrika
    et al.
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    World-Wide Indoor Exposure to Polyfluoroalkyl Phosphate Esters (PAPs) and other PFASs in Household Dust2015In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 49, no 24, p. 14503-14511Article in journal (Refereed)
    Abstract [en]

    Human exposure to perfluorooctanoic acid (PFOA) and other per- and polyfluoroalkyl substances (PFASs) is ongoing and in some cases increasing, despite efforts made to reduce emissions. The role of precursor compounds such as polyfluorinated phosphate esters (PAPs) has received increasing attention, but there are knowledge gaps regarding their occurrence and impact on human exposure. In this study, mono-, di-, and triPAPs, perfluorinated alkyl acids (PFAAs), saturated, and unsaturated fluorotelomer carboxylic acids (FTCA/FTUCAs), perfluoroalkane sulfonamides, and sulfonamidethanols (FOSA/FOSEs), and one fluorotelomer sulfonic acid (FTSA)) were compared in household dust samples from Canada, the Faroe Islands, Sweden, Greece, Spain, Nepal, Japan, and Australia. Mono-, di-, and triPAPs, including several diPAP homologues, were frequently detected in dust from all countries, revealing an ubiquitous spread in private households from diverse geographic areas, with significant differences between countries. The median levels of monoPAPs and diPAPs ranged from 3.7 ng/g to 1 023 ng/g and 3.6 ng/g to 692 ng/g, respectively, with the lowest levels found in Nepal and the highest in Japan. The levels of PAPs exceeded those of the other PFAS classes. These findings reveal the importance of PAPs as a source of PFAS exposure worldwide.

  • 35.
    Eriksson, Ulrika
    et al.
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Rotander, Anna
    Örebro University, School of Science and Technology.
    Mikkelsen, Bjorg
    Faroese Food & Vet Agcy, Torshavn, Faroe Islands, Denmark.
    Dam, Maria
    Environm Agcy, Argir, Faroe Islands, Denmark.
    Perfluoroalkyl substances (PFASs) in food and water from Faroe Islands2013In: Environmental Science and Pollution Research, ISSN 0944-1344, E-ISSN 1614-7499, Vol. 20, no 11, p. 7940-7948Article in journal (Refereed)
    Abstract [en]

    Diet and drinking water are suggested to be major exposure pathways for perfluoroalkyl substances (PFASs). In this study, food items and water from Faroe Islands sampled in 2011/2012 were analyzed for 11 perfluoroalkyl carboxylic acids (PFCAs) and 4 perfluoroalkane sulfonic acids (PFSAs). The food samples included milk, yoghurt, crSme fraiche, potatoes, fish, and fish feed, and the water samples included surface water and purified drinking water. In total, nine PFCAs and four PFSAs were detected. Generally, the levels of PFAS were in the lower picogram per gram range. Perfluorobutanoic acid was a major contributor to the total PFASs concentration in water samples and had a mean concentration of 750 pg/L. Perfluoroundecanoic acid (PFUnDA) was predominating in milk and wild fish with mean concentrations of 170 pg/g. Perfluorooctane sulfonic acid (PFOS) was most frequently detected in food items followed by PFUnDA, perfluorononanoic acid, and perfluorooctanoic acid (PFOA). Levels of PFUnDA and PFOA exceeded those of PFOS in milk and fish samples. Prevalence of long-chain PFCAs in Faroese food items and water is confirming earlier observations of their increase in Arctic biota. Predominance of short-chain and long-chain homologues indicates exposure from PFOS and PFOA replacement compounds.

  • 36.
    Eriksson, Ulrika
    et al.
    Örebro University, School of Science and Technology.
    Mueller, Jochen F.
    Entox, Queensland Alliance for Environmental Health Sciences, The University of Queensland, Coopers Plains, Australia.
    Toms, Leisa-Maree L.
    School of Public Health and Social Work and Institute of Health and Biomedical Innovation, Queensland University of Technology, Kelvin Grove, Australia.
    Hobson, Peter
    Sullivan and Nicolaides Pathology, Taringa, Australia.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Temporal trends of PFSAs, PFCAs and selected precursors in Australian serum from 2002 to 20132017In: Environmental Pollution, ISSN 0269-7491, E-ISSN 1873-6424, Vol. 220, no Pt A, p. 168-177Article in journal (Refereed)
    Abstract [en]

    Per- and polyfluoroalkyl substances (PFASs) are a family of compounds that includes numerous compound classes. To date, only a subset of these PFASs have been studied thoroughly in the general population. In this study, pooled serum samples from Australia collected in 2002-2013 were analyzed for PFASs according to gender and age (age categories of 0-4 years, 5-15 years, 16-30 years, 31-45 years, 46-60 years, and >60 years), in total 54 pooled samples and 4920 individuals. Compound classes included were perfluorocarboxylic acids (PFCAs), perfluorosulfonic acids (PFSAs), and two groups of PFCA precursor compounds; polyfluoroalkyl phosphate diesters (diPAPs), and fluorotelomer sulfonic acids (FTSAs). Several PFASs that were not reported in previous studies of Australian serum samples were found in this sample set including; diPAPs, FTSAs, perfluoropentane sulfonic acid (PFPeS), perfluoroheptane sulfonic acid (PFHpS), perfluoroheptane carboxylic acid (PFHpA), perfluoroundecanoic acid (PFUnDA), perfluorododecanoic acid (PFDoDA), and perfluorotridecanoic acid (PFTrDA). Various temporal trends were observed with a significant reduction (p < 0.05) between 2002 and 2013 for 8:2 FTSA, perflurohexane sulfonic acid (PFHxS), PFHpS, PFOS, and perflurooctanoic acid (PFOA). Levels of longer-chained PFDA and PFUnDA started to decrease more recently, between 2006 and 2013, while PFDoDA increased during the same time period. Higher levels in younger age groups (0-4 and 5-15 years) compared to adults (>15 years) were found for 8:2 FTSA and PFHpA, while levels of PFHpS, PFOS, PFUnDA, PFDoDA and PFTrDA were higher in adult age groups compared to younger age groups. Gender-specific patterns were seen for PFOA, PFHxS, PFHpS and PFOS, where levels were lower in women. Changes in manufacturing processes were reflected in the temporal time trends, and differences in bioaccumulation potential between homologues could be associated with age trends. Our results emphasize the importance of including emerging classes of PFASs in biomonitoring studies.

  • 37.
    Eriksson, Ulrika
    et al.
    Örebro University, School of Science and Technology.
    Mueller, Jochen F.
    University of Queensland, Coopers Plains, Australia.
    Toms, Leisa-Maree L.
    Queensland University of Technology, Kelvin Grove, Australia .
    Hobson, Peter
    Sullivan and Nicolaides Pathology, Taringa, Australia.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Temporal trends of PFSAs, PFCAs and selected precursors in Australian serum from 2002 to 2013Manuscript (preprint) (Other academic)
  • 38.
    Eriksson, Ulrika
    et al.
    Örebro University, School of Science and Technology.
    Roos, Anna
    Swedish Museum of Natural History, Stockholm, Sweden.
    Lind, Ylva
    Swedish Museum of Natural History, Stockholm, Sweden.
    Hope, Kjell
    Örebro University, School of Science and Technology.
    Ekblad, Alf
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Comparison of PFASs contamination in the freshwater and terrestrial environments by analysis of eggs from osprey (Pandion haliaetus), tawny owl (Strix aluco), and common kestrel (Falco tinnunculus)2016In: Environmental Research, ISSN 0013-9351, E-ISSN 1096-0953, Vol. 149, p. 40-47Article in journal (Refereed)
    Abstract [en]

    The level of PFAS (per- and polyfluorinated alkyl substances) contamination in freshwater and terrestrial Swedish environments in 2013/2014 was assessed by analyzing a range of perfluorinated alkyl acids, fluorotelomer acids, sulfonamides, sulfonamidoethanols and polyfluoralkyl phosphate diesters (diPAPs) in predator bird eggs. Stable isotopes ((13)C and (15)N) were analyzed to elucidate the dietary source. The tawny owl (Strix aluco, n=10) and common kestrel (Falco tinnunculus, n=40), two terrestrial species, and the osprey (Pandion haliaetus, n=30), a freshwater specie were included. In addition, a temporal trend (1997-2001, 2008-2009, 2013) in osprey was studied as well. The PFAS profile was dominated by perfluorooctane sulfonic acid (PFOS) in eggs from osprey and tawny owl, while for common kestrel perfluorinated carboxylic acids (∑PFCA) exceeded the level of PFOS. PFOS concentration in osprey eggs remained at the same level between 1997 and 2001 and 2013. For the long-chained PFCAs, there were a significant increase in concentrations in osprey eggs between 1997 and 2001 and 2008-2009. The levels of PFOS and PFCAs were about 10 and five times higher, respectively, in osprey compared to tawny owl and common kestrel. Evidence of direct exposure from PFCA precursor compounds to birds in both freshwater and terrestrial environment was observed. Low levels of diPAPs were detected in a few samples of osprey (<0.02-2.4ng/g) and common kestrel (<0.02-0.16ng/g) eggs, and 6:2 FTSA was detected in a majority of the osprey eggs (<6.3-52ng/g). One saturated telomer acid (7:3 FTCA), which is a transformation marker from precursor exposure, was detected in all species (<0.24-2.7ng/g). The (15)N data showed higher levels in osprey eggs compared to tawny owl and common kestrel, indicating that they feed on a 2-3 times higher trophic level. We conclude that ospreys are continuously exposed to PFAS at levels where adverse toxic effects have been observed in birds.

  • 39.
    Fredriksson, Felicia
    et al.
    Örebro University, School of Science and Technology.
    Eriksson, Ulrika
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Yeung, Leo
    Örebro University, School of Science and Technology.
    A Pilot Study of the Fluorinated Ingredient of Scotchgard Products and Their Levels in WWTP Sludge and Landfill Leachate from Sweden2020Report (Other academic)
    Abstract [en]

    This study performed by Örebro University on behalf of the Swedish Environmental Agency aims at assessing the occurrence and levels of the newly identified side-chain fluorinated polymers from an environmental perspective. The aims of present study are 1) to develop instrumental and extraction methods to measure the active ingredient of two Scotchgard products (two side-chain fluorinated polymers, hereafter referred to as Pre-2002 and Post-2002) in sludge and leachate samples from Swedish wastewater treatment plants and landfills; 2) to evaluate if Pre-2002 and Post-2002 may be responsible for the unidentified organofluorine in the sludge samples from our previous screening study reporting extractable organofluorine (EOF); and 3) to conduct a mass balance analysis on EOF and sum of 93 per- and polyfluoroalkyl substances (PFAS) including Pre-2002 and Post-2002 in the sludge and landfill leachate samples to assess the levels of unidentified EOF that potentially are other polymeric or non-polymeric PFAS.

    Levels of Pre-2002 and Post-2002 and EOF are reported for sludge samples from four wastewater treatment plants (Bergkvara in Torsås, Gässlösa in Borås, Henriksdal in Stockholm, and Öhn in Umeå) collected in 2015, and leachate samples from three different landfills (Atleverket in Örebro, Hässleholm Kretsloppscenter in Hässleholm, and Flishult in Vetlanda). Sludge samples from Gässlösa wastewater treatment plant collected between 2004 and 2016 (excluding 2005 and 2006) were analyzed to assess any temporal trends of the two side-chain fluorinated polymers (Pre-2002 and Post-2002). The present investigation reported levels of both Pre-2002 and Post-2002 in all sludge samples (158-2618 ng/g d.w.). Levels of Pre-2002 were always higher than those of Post-2002 in the same samples. A declining trend was observed for Pre-2002 in sludge samples from Gässlösa but no clear trend was noted for Post-2002. The concentrations of the Pre-2002 and Post-2002 in sludge were higher than the sum of 83 PFAS analyzed in the previous screening study. No relationship between number of people that the wastewater treatment plants served and the concentrations of EOF and Pre-2002 and Post-2002 could be observed. The concentrations of both EOF and Pre-2002 and Post-2002 seem to be more related to the types of industry located in that area. Only three of the five leachate samples showed detectable levels of Pre-2002. Post-2002 was not detected in any of the landfill leachates. The low levels could be due to that both compounds are strongly sorbed to particles, which indicates the fate and distribution of these compounds. For both the sludge and leachate samples, the quantified levels of Pre-2002 and Post-2002 only contributed to a minor part of the EOF. A high proportion of unknown EOF still remains and may be related to other polymeric or non-polar PFAS.

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    A Pilot Study of the Fluorinated Ingredient of Scotchgard Products and Their Levels in WWTP Sludge and Landfill Leachate from Sweden
  • 40.
    Fredriksson, Felicia
    et al.
    Örebro University, School of Science and Technology.
    Eriksson, Ulrika
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Impact of sample treatment on extractable organofluorine mass balance in sludge – an insight into the characteristics of unidentified organofluorineManuscript (preprint) (Other academic)
  • 41.
    Fredriksson, Felicia
    et al.
    Örebro University, School of Science and Technology.
    Eriksson, Ulrika
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Per- and polyfluoroalkyl substances (PFAS) in sludge from wastewater treatment plants in Sweden: First findings of novel fluorinated copolymers in Europe including temporal analysis2022In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 846, article id 157406Article in journal (Refereed)
    Abstract [en]

    Thousands of per- and polyfluoroalkyl substances (PFAS) are on the global market, while only a minor proportion is monitored regularly in the environment. Wastewater treatment plants (WWTPs) have been suggested to be a point source for PFAS to the environment due to emission of effluent and sludge. In this study, 81 PFAS including two rarely studied perfluoroalkyl sulfonamide-based (FASA) copolymers were analyzed in sludge samples to understand the usage of PFAS in the society. Sludge samples (n = 28) were collected at four WWTPs in Sweden between 2004 and 2017. The total levels of 79 measured PFAS were between 50 and 1124 ng/g d.w. All sludge samples showed detectable levels of both C8- and C4-FASA-based copolymers. The concentrations of the FASA-based copolymers were proposed to be reported in fluorinated side-chain equivalents (FSC eq.), in order to compare the levels of the copolymers with the other neutral and anionic PFAS, as no authentic standards were available. The concentrations of the FASA-based copolymers in sludge were between 1.4 and 22 ng FSC eq./g d.w. A general predomination of precursor and intermediate compounds was observed. A lower contribution of perfluoroalkyl carboxylic acids was noted for the WWTPs more influenced by domestic emission when compared with more influenced by industrial emission. An overall declining trend in the total PFAS concentration was seen between the years 2004 and 2017. The present study observed a shift from the C8-based chemistry toward shorter chain lengths, included a declining trend for C8-FASA-based copolymer over the entire study period. These findings further demonstrate the occurrence of side-chain fluorinated copolymers in Sweden and that sludge is a useful matrix to reflect the usage of PFAS in society and the potential for environmental exposure.

  • 42.
    Fredriksson, Felicia
    et al.
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Eriksson, Ulrika
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Analysis and characterization of novel fluorinated compounds used in surface treatments products2022In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 302, article id 134720Article in journal (Refereed)
    Abstract [en]

    Side-chain fluorinated polymers are speculated to be potential precursors to other non-polymeric aliphatic per- and polyfluoroalkyl acids (PFAAs). Limited knowledge of environmental occurrence of this compound class is partly due to lack of structural information and authentic standards. In this study, two novel fluorinated compounds, suspected to be side-chain fluorinated copolymers used in two commercial technical mixtures (Scotchgard™ Pre-2002 formulation and Scotchgard™ Post-2002 formulation) were analyzed and characterized in order to provide information to facilitate detection and quantification. The commercial mixtures were analyzed using tandem mass spectrometry and high-resolution mass spectrometry; besides already reported C4- and C8-fluoroalkylsulfonamido (FASA) side-chains, a proposed structure was determined for the perfluorooctane (C8) sulfonamide-urethane copolymer in the Pre-2002 formulation. Structural isomers were also observed for C4- and C8-FASA-based copolymers. Total fluorine analysis revealed that the Scotchgard™ Pre-2002 Formulation contained a fluorine content of 0.5% and 1.8% for the Scotchgard™ Post-2002 Formulation. The equivalent FASA side-chain content was determined to be 0.8% for Pre-2002 and 3.1% for Post-2002. Both C4- and C8-FASA-based copolymers underwent hydrolysis and oxidation and were transformed to their respective perfluoroalkyl side chain, which suggest that transformation products can be analyzed for example after total oxidizable precursor (TOP) assay. Both compounds were shown to strongly sorb to sediment particles, which also gives indications about their environmental fate and transport pathways.

  • 43.
    Fredriksson, Felicia
    et al.
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Eriksson, Ulrika
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Experimental and field studies of bioavailability and transformation of fluoroalkyl sulfonamide (FASA) based copolymers in earthwormsManuscript (preprint) (Other academic)
  • 44.
    Hardell, Elin
    et al.
    School of Science and Technology, Örebro University, Örebro, Sweden.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    van Bavel, Bert
    Örebro University, School of Science and Technology.
    Bao, Jia
    School of Science and Technology, Örebro University, Örebro, Sweden.
    Carlberg, Michael
    Department of Oncology, University Hospital, Örebro, Sweden.
    Hardell, Lennart
    Örebro University Hospital. Department of Oncology, Örebro University Hospital, Örebro, Sweden.
    Case-control study on perfluorinated alkyl acids (PFAAs) and the risk of prostate cancer2014In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 63, p. 35-39Article in journal (Refereed)
    Abstract [en]

    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. (C) 2013 Elsevier Ltd. All rights reserved.

  • 45.
    Hartz, William F.
    et al.
    Department of Earth Sciences, University of Oxford, South Parks Road, Oxford OX1 3AN, United Kingdom; Department of Arctic Geology, University Centre in Svalbard (UNIS), NO-9171, Longyearbyen, Svalbard, Norway.
    Björnsdotter, Maria K.
    Institute of Environmental Assessment and Water Research (IDAEA-CSIC), C/Jordi Girona, 18-26, 08034 Barcelona, Catalonia, Spain; Örebro University, Örebro, Sweden.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Hodson, Andrew
    Department of Arctic Geology, University Centre in Svalbard (UNIS), NO-9171, Longyearbyen, Svalbard, Norway; Department of Environmental Sciences, Western Norway University of Applied Sciences, NO-6851 Sogndal, Norway.
    Thomas, Elizabeth R.
    Ice Dynamics and Paleoclimate, British Antarctic Survey, High Cross, Cambridge CB3 0ET, United Kingdom.
    Humby, Jack D.
    Ice Dynamics and Paleoclimate, British Antarctic Survey, High Cross, Cambridge CB3 0ET, United Kingdom.
    Day, Chris
    Department of Earth Sciences, University of Oxford, South Parks Road, Oxford OX1 3AN, United Kingdom.
    Ericson Jogsten, Ingrid
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Kallenborn, Roland
    Faculty of Chemistry, Biotechnology and Food Sciences (KBM), Norwegian University of Life Sciences (NMBU), NO-1432 Ås, Norway; Department of Arctic Technology, University Centre in Svalbard (UNIS), NO-9171, Longyearbyen, Svalbard, Norway.
    Levels and distribution profiles of Per- and Polyfluoroalkyl Substances (PFAS) in a high Arctic Svalbard ice core2023In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 871, article id 161830Article in journal (Refereed)
    Abstract [en]

    Per- and polyfluoroalkyl substances (PFAS) are a group of persistent organic contaminants of which some are toxic and bioaccumulative. Several PFAS can be formed from the atmospheric degradation of precursors such as fluorotelomer alcohols (FTOHs) as well as hydrochlorofluorocarbons (HFCs) and other ozone-depleting chlorofluorocarbon (CFC) replacement compounds. Svalbard ice cores have been shown to provide a valuable record of long-range atmospheric transport of contaminants to the Arctic. This study uses a 12.3 m ice core from the remote Lomonosovfonna ice cap on Svalbard to understand the atmospheric deposition of PFAS in the Arctic. A total of 45 PFAS were targeted, of which 26 were detected, using supercritical fluid chromatography (SFC) tandem mass spectrometry (MS/MS) and ultra-performance liquid chromatography (UPLC) MS/MS. C2 to C11 perfluoroalkyl carboxylic acids (PFCAs) were detected continuously in the ice core and their fluxes ranged from 2.5 to 8200 ng m-2 yr-1 (9.51-16,500 pg L-1). Trifluoroacetic acid (TFA) represented 71 % of the total mass of C2 - C11 PFCAs in the ice core and had increasing temporal trends in deposition. The distribution profile of PFCAs suggested that FTOHs were likely the atmospheric precursor to C8 - C11 PFCAs, whereas C2 - C6 PFCAs had alternative sources, such as HFCs and other CFC replacement compounds. Perfluorooctanesulfonic acid (PFOS) was also widely detected in 82 % of ice core subsections, and its isomer profile (81 % linear) indicated an electrochemical fluorination manufacturing source. Comparisons of PFAS concentrations with a marine aerosol proxy showed that marine aerosols were insignificant for the deposition of PFAS on Lomonosovfonna. Comparisons with a melt proxy showed that TFA and PFOS were mobile during meltwater percolation. This indicates that seasonal snowmelt and runoff from post-industrial accumulation on glaciers could be a significant seasonal source of PFAS to ecosystems in Arctic fjords.

  • 46.
    Jiao, Enmiao
    et al.
    Key Laboratory of Yangtze River Water Environment, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China.
    Larsson, Pontus
    Örebro University, School of Science and Technology.
    Wang, Qi
    State Key Laboratory of Marine Pollution, City University of Hong Kong, Hong Kong 999077, China.
    Zhu, Zhiliang
    Key Laboratory of Yangtze River Water Environment, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China.
    Yin, Daqiang
    Key Laboratory of Yangtze River Water Environment, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    van Hees, Patrick
    Örebro University, School of Science and Technology. Eurofins Food and Feed Testing Sweden AB, Sjöhagsgatan 3, SE-531 40 Lidköping, Sweden.
    Karlsson, Patrik
    Eurofins Food and Feed Testing Sweden AB, Sjöhagsgatan 3, SE-531 40 Lidköping, Sweden.
    Qiu, Yanling
    Key Laboratory of Yangtze River Water Environment, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Further Insight into Extractable (Organo)fluorine Mass Balance Analysis of Tap Water from Shanghai, China2023In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 57, no 38, p. 14330-14339Article in journal (Refereed)
    Abstract [en]

    The ubiquitous occurrence of per- and polyfluoroalkyl substances (PFAS) and the detection of unexplained extractable organofluorine (EOF) in drinking water have raised growing concerns. A recent study reported the detection of inorganic fluorinated anions in German river systems, and therefore, in some samples, EOF may include some inorganic fluorinated anions. Thus, it might be more appropriate to use the term "extractable fluorine (EF) analysis" instead of the term EOF analysis. In this study, tap water samples (n = 39) from Shanghai were collected to assess the levels of EF/EOF, 35 target PFAS, two inorganic fluorinated anions (tetrafluoroborate (BF4-) and hexafluorophosphate (PF6-)), and novel PFAS through suspect screening and potential oxidizable precursors through oxidative conversion. The results showed that ultra-short PFAS were the largest contributors to target PFAS, accounting for up to 97% of ΣPFAS. To the best of our knowledge, this was the first time that bis(trifluoromethanesulfonyl)imide (NTf2) was reported in drinking water from China, and p-perfluorous nonenoxybenzenesulfonate (OBS) was also identified through suspect screening. Small amounts of precursors that can be oxidatively converted to PFCAs were noted after oxidative conversion. EF mass balance analysis revealed that target PFAS could only explain less than 36% of EF. However, the amounts of unexplained extractable fluorine were greatly reduced when BF4- and PF6- were included. These compounds further explained more than 44% of the EF, indicating the role of inorganic fluorinated anions in the mass balance analysis.

  • 47.
    Jiao, Enmiao
    et al.
    Key Laboratory of Yangtze River Water Environment, College of Environmental Science and Engineering, Tongji University, China.
    Zhu, Zhiliang
    Key Laboratory of Yangtze River Water Environment, College of Environmental Science and Engineering, Tongji University, China.
    Yin, Daqiang
    Key Laboratory of Yangtze River Water Environment, College of Environmental Science and Engineering, Tongji University, China.
    Qiu, Yanling
    Key Laboratory of Yangtze River Water Environment, College of Environmental Science and Engineering, Tongji University, China.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    A pilot study on extractable organofluorine and per- and polyfluoroalkyl substances (PFAS) in water from drinking water treatment plants around Taihu Lake, China: what is missed by target PFAS analysis?2022In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 24, no 7, p. 1060-1070Article in journal (Refereed)
    Abstract [en]

    Per- and polyfluoroalkyl substances (PFAS) have raised concerns due to their worldwide occurrence and adverse effects on both the environment and humans as well as posing challenges for monitoring. Further collection of information is required for a better understanding of their occurrence and the unknown fractions of the extractable organofluorine (EOF) not explained by commonly monitored target PFAS. In this study, eight pairs of raw and treated water were collected from drinking water treatment plants (DWTPs) around Taihu Lake in China and analyzed for EOF and 34 target PFAS. Mass balance analysis of organofluorine revealed that at least 68% of EOF could not be explained by target PFAS. Relatively higher total target concentrations were observed in 4 DWTPs (D1 to D4) when compared to other samples with the highest sum concentration up to 189 ng L-1. PFOA, PFOS and PFHxS were the abundant compounds. Suspect screening analysis identified 10 emerging PFAS (e.g., H-PFAAs, H-PFESAs and OBS) in addition to target PFAS in raw or treated water. The ratios PFBA/PFOA and PFBS/PFOS between previous and current studies showed significant replacements of short-chain to long-chain PFAS. The ratios of the measured PFAS concentrations to the guideline values showed that some of the treated drinking water exceeds guideline values, appealing for efforts on drinking water safety guarantee.

  • 48.
    Jugan, Juliann
    et al.
    Department of Environmental Toxicology, University of California, One Shields Avenue, Davis, CA, USA.
    Lind, P. Monica
    Department of Medical Sciences, Occupational and Environmental Medicine, Uppsala University, Uppsala, Sweden.
    Salihovic, Samira
    Örebro University, School of Medical Sciences.
    Stubleski, Jordan
    Wellington Laboratories Inc., Guelph, ON, Canada.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Lind, Lars
    Department of Medical Sciences, Cardiovascular Epidemiology, Uppsala University, Uppsala, Sweden.
    La Merrill, Michele A.
    Department of Environmental Toxicology, University of California, One Shields Avenue, Davis, CA, USA.
    The associations between p,p'-DDE levels and plasma levels of lipoproteins and their subclasses in an elderly population determined by analysis of lipoprotein content2020In: Lipids in Health and Disease, E-ISSN 1476-511X, Vol. 19, no 1, article id 249Article in journal (Refereed)
    Abstract [en]

    BACKGROUND: Lipoproteins at aberrant levels are known to play a role in cardiovascular disease. The metabolite of the insecticide dichlorodiphenyltrichloroethane (DDT), p,p'-dichlorodiphenyldichloroethylene (p,p'-DDE), physically associates with lipids and accumulates in adipose tissue. Little is known about which lipoproteins associate with p,p'-DDE. An association between p,p'-DDE exposure and altered levels of circulating lipids was assessed in a large human cohort using a detailed analysis of lipoprotein content.

    METHODS: Plasma samples were collected from the subset of 75-year old Swedes in the Prospective Investigation of the Vasculature of Uppsala Seniors (PIVUS) cohort who were not prescribed lipid lowering medication (n = 571). p,p'-DDE concentrations in plasma were measured using high-throughput solid phase extraction and gas chromatography-high resolution mass spectrometry. Analysis of plasma lipoprotein content was performed with nuclear magnetic resonance spectroscopy.

    RESULTS: Detectable levels of p,p'-DDE were found in the plasma samples of all subjects. Elevated p,p'-DDE levels were associated with increased concentrations of lipoproteins of all diameters, with the exception of high density lipoprotein (HDL) of diameters between 14.3 nm-10.9 nm. Of the lipoprotein constituents, triglycerides were most uniformly associated with elevated p,p'-DDE across lipoproteins. p,p'-DDE was furthermore associated with apolipoprotein B, but not apolipoprotein A1.

    CONCLUSIONS: The positive associations observed between each lipoprotein class and elevated p,p'-DDE support previous data suggesting that p,p'-DDE interacts with lipoproteins within plasma. It is speculated that both physio-chemical and biological mechanisms may explain why p,p'-DDE does not uniformly associate with lipids across lipoproteins.

  • 49.
    Järnberg, Ulf
    et al.
    Department of Applied Environmental Science, ITM, Stockholm University.
    Holmström, Katrin
    Department of Applied Environmental Science, ITM, Stockholm University.
    van Bavel, Bert
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Perfluoroalkylated acids and related compounds (PFAS) in the Swedish environment2007Report (Other academic)
    Abstract [sv]

    The perfluoroalkylated substances have gained increased attention among scientists and regulators during the last few years. In particular, perfluorooctane sulfonate (PFOS), perfluorooctanoic acid (PFOA) and similar perfluorinated alkylated acids are regarded as the most stable end products of various perfluoroalkylated substances and have been shown to be extremely stable, bioconcentrate and biomagnify and have several toxicological effects. The industrial chemistry of perfluoroalkylated substances is extremely diverse and includes almost all chemical functionalities from simple pure alkanes to complex co-polymers. Major usage of perfluoroalkylated products is related to polymeric compounds and the dominant release to the environment is from primary and secondary production plants which are lacking in the Nordic countries. The occurrence of elevated concentrations of perfluoroalkylated acids in Sweden is strongly related to urbanized areas and the most likely path into the aquatic environment is through sewage water, although atmospheric input is also possible via more volatile precursor compounds. Up to 40 times elevated concentrations were found in biota from urban areas compared to unpolluted areas. Lake Mälaren and lower parts of the river Helge å are examples of aqueous environments clearly contaminated by PFOS. One of several potential point sources in Sweden has been screened for PFOS. A firefighting training site was found to release PFOS to the local aqueous environment (wetland) where μg/l concentrations where found. Long chain (more than 8 C for sulfonates and 10 C or more for carboxylates) perfluoroalkylated acids are readily taken up by biota in aqueous environments and reach very high concentrations in predators at high trophic levels of aquatic food webs. Baltic guillemot egg showed an increasing trend in PFOS concentration from 20-30 ng/g by the end of sixties to more than 600 ng/g at present. Freshwater otter from various locations in Sweden showed concentrations similar to guillemot eggs and Baltic grey seal has extreme values up to ten times higher (21 μg/g sum of all acids 6-14 C, PFOS alone:11μg/g). Human exposure, as described by Swedish human blood levels, appears to be similar to most other countries. No extreme values were encountered which would indicate occupational exposure. An excessive consumption of freshwater fish may contribute to an increased exposure, but this could not be clearly verified. Occupational settings where exposure to precursor compounds can take place are present in Sweden and should be included in future studies. Industrial use of textile and leather impregnating formulations result in elevated concentrations of perfluorocarboylates in effluent water from sewage treatment plants. The relation between effluent and biota concentrations for an aquatic environment with this type of activity needs to be further described in particular for perfluoroalkyl carboxylates which are currently being discharged in Sweden. Exposure routes and distribution behavior are yet not completely described for many PFAS, in particular their precursors. Environmental levels, human levels and human exposure data are lacking for a wide variety of PFAS discussed in this report

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    Perfluoroalkylated acids and related compounds (PFAS) in the Swedish environment
  • 50.
    Kaiser, Andreas-Marius
    et al.
    Environment Agency Austria, Vienna, Austria; Institute of Medical Genetics, Center for Pathobiochemistry and Genetics, Medical University of Vienna, Vienna, Austria.
    Aro, Rudolf
    Örebro University, School of Science and Technology.
    Kärrman, Anna
    Örebro University, School of Science and Technology.
    Weiss, Stefan
    Environment Agency Austria, Vienna, Austria.
    Hartmann, Christina
    Environment Agency Austria, Vienna, Austria.
    Uhl, Maria
    Environment Agency Austria, Vienna, Austria.
    Forsthuber, Martin
    Institute of Medical Genetics, Center for Pathobiochemistry and Genetics, Medical University of Vienna, Vienna, Austria; Department of Environmental Health, Center for Public Health, Medical University of Vienna, Vienna, Austria.
    Gundacker, Claudia
    Institute of Medical Genetics, Center for Pathobiochemistry and Genetics, Medical University of Vienna, Vienna, Austria.
    Yeung, Leo W. Y.
    Örebro University, School of Science and Technology.
    Comparison of extraction methods for per- and polyfluoroalkyl substances (PFAS) in human serum and placenta samples-insights into extractable organic fluorine (EOF)2021In: Analytical and Bioanalytical Chemistry, ISSN 1618-2642, E-ISSN 1618-2650, Vol. 413, p. 865-876Article in journal (Refereed)
    Abstract [en]

    Since the detection of per- and polyfluoroalkyl substances (PFAS) in humans and different environmental media in the last two decades, this substance group has attracted a lot of attention as well as increasing concerns. The fluorine mass balance approach, by comparing the levels of targeted PFAS after conversion to fluorine equivalents with those of extractable organic fluorine (EOF), showed the presence of unidentified organofluorine in different environmental samples. Out of the thousands of PFAS in existence, only a very small fraction is included in routine analysis. In recent years, liquid chromatography coupled with tandem-mass spectrometry (LC-MS/MS) has demonstrated the ability to analytically cover a wide spectrum of PFAS. In contrast, conventional extraction methods developed 10 to 15 years ago were only evaluated for a limited number of PFAS. The aim of the present study was to evaluate the advantages and disadvantages of three different extraction methods, adapted from the literatures without further optimization (ion-pair liquid-liquid extraction, solid-phase extraction (SPE), using hydrophilic-lipophilic (HLB) or weak anion exchange (WAX) sorbents), for human biomonitoring of 61 PFAS in serum and placental tissue samples. In addition, levels of EOF were compared among these extraction methods via spiked samples. Results showed that performance, in terms of recovery, differed between the extraction methods for different PFAS; different extraction methods resulted in different EOF concentrations indicating that the choice of extraction method is important for target PFAS and EOF analysis. Results of maternal serum samples, analyzed in two different laboratories using two different extraction methods, showed an accordance of 107.6% (± 21.3); the detected perfluoroalkyl acids (PFAAs) in maternal and cord serum samples were in the range of 0.076 to 2.9 ng/mL.Graphical abstract.

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