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  • 1.
    Balk, Fabian G. P.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Swiss Federal Institute of Aquatic Science and Technology, Switzerland.
    Winkens Pütz, Kerstin
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Swedish Museum of Natural History, Sweden.
    Ribbenstedt, Anton
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Gomis, Melissa I.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Université Paris-Saclay, France.
    Filipovic, Marko
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. NIRAS Sweden AB, Sweden.
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Children's exposure to perfluoroalkyl acids - a modelling approach2019In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 11, p. 1875-1886Article in journal (Refereed)
    Abstract [en]

    Adults are mainly exposed to per- and polyfluoroalkyl substances (PFASs) via ingestion of food, inhalation of air and ingestion of dust, whereas for children the exposure to PFASs is largely unknown. This study aimed to reconstruct the serum concentrations of perfluorooctanoic acid (PFOA), perfluorooctane sulfonic acid (PFOS) and perfluorohexane sulfonic acid (PFHxS) in children after infancy up to 10.5 years of age and to test if dietary intake is the major exposure pathway for children to PFOA, PFOS and PFHxS after infancy. For this work, a dataset from a Finnish child cohort study was available, which comprised serum concentrations of the studied perfluoroalkyl acids (PFAAs) and PFAS concentration measurements in dust and air samples from the children's bedrooms. The calculated PFAA intakes were used in a pharmacokinetic model to reconstruct the PFAA serum concentrations from 1 to 10.5 years of age. The calculated PFOA and PFOS intakes were close to current regulatory intake thresholds and diet was the major exposure medium for the 10.5 year-olds. The one-compartment PK model reconstructed median PFOA and PFOS serum concentrations well compared to corresponding measured median serum concentrations, while the modelled PFHxS serum concentrations showed a constant underestimation. The results imply that children's exposure to PFOA and PFOS after breastfeeding and with increasing age resembles the exposure of adults. Further, the children in the Finnish cohort experienced a rather constant exposure to PFOA and PFOS between 1 and 10.5 years of age. The PFHxS exposure sources and respective pharmacokinetic parameter estimations need further investigation.

  • 2. Chirikona, Florah
    et al.
    Filipovic, Marko
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Ooko, Seline
    Orata, Francis
    Perfluoroalkyl acids in selected wastewater treatment plants and their discharge load within the Lake Victoria basin in Kenya2015In: Environmental Monitoring & Assessment, ISSN 0167-6369, E-ISSN 1573-2959, Vol. 187, no 5, article id 238Article in journal (Refereed)
    Abstract [en]

    A major ecological challenge facing Lake Victoria basin is the influx of chemical contaminants from domestic, hospital, and industrial effluents. Determined levels of perfluoroalkyl acids (PFAAs) in wastewater and sludge from selected wastewater treatment plants (WWTPs) in Kenya are presented and their daily discharge loads calculated for the first time within the Lake Victoria basin. Samples were extracted and separated using solid-phase extraction and ultra-performance liquid chromatography (UPLC)-MS/MS or LC-MS/MS methodology. All sewage sludge and wastewater samples obtained from the WWTPs contained detectable levels of PFAAs in picogram per gram dry weight (d.w.) and in nanogram per liter, respectively. There was variability in distribution of PFAAs in domestic, hospital, and industrial waste with domestic WWPTs observed to contain higher levels. Almost all PFAA homologues of chain length C-6 and above were detected in samples analyzed, with long-chain PFAAs (C-8 and above chain length) being dominant. The discharge from hospital contributes significantly to the amounts of PFAAs released to the municipal water systems and the lake catchment. Using the average output of wastewater from the five WWTPs, a mass load of 1013 mg day(-1) PFAAs per day discharged has been calculated, with the highest discharge obtained at Kisumu City (656 mg day(-1)). The concentration range of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) in wastewater was 1.3-28 and 0.9-9.8 ng L-1 and in sludge samples were 117-673 and 98-683 pg g(-1), respectively.

  • 3.
    Filipovic, Marko
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Fate of perfluoroalkyl acids in the aquatic environment with a focus on mass balance studies2015Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Perfluoroalkyl substances (PFASs) are man-made chemicals. Their unique properties make them beneficial for a wide range of industrial and consumer product applications, such as in aqueous film forming foam (AFFF), durable water repellent clothing, hydraulic oils and food packaging materials. Perfluoroalkyl acids (PFAAs), a class of PFASs, are highly persistent in the environment, and long chain PFAAs are bioaccumulative and toxic. International regulation and voluntary actions by the industry have been implemented and led to a recent reduction of primary emissions of PFAAs to the environment. However, point sources such as AFFF training sites as well as diffuse sources continue to contaminate water bodies, soil and biota. Reducing environmental pollution with PFAAs has therefore become a regulatory priority. Designing successful measures to reduce the PFAA contamination requires an understanding of the sources, transport and fate of PFAAs in the environment.

    Four scientific publications are included in this PhD thesis, which aimed at increasing the holistic understanding of the fate of PFAAs in aquatic systems. This was achieved by chemical trace analysis combined with mass balance modeling. The following topics were covered: Dispersion and fate of PFAAs from an AFFF-impacted site (Paper I), recirculation of PFAAs in the aquatic environment with focus on waste water treatment plants (WWTPs, Paper II), mass balance of PFAAs in the Baltic Sea (Paper III) and transport and fate of PFAAs in two pristine boreal stream catchments (Paper IV).

    Results from Paper I showed that AFFF-impacted sites at a former military airfield, which was abandoned for more than 30 years, continue to be point sources of PFAAs to recipients. The sum of PFAAs in the ground water and surface waters ranged from 740 to 51000 ng L-1 and <0.5 to 79 ng L-1, respectively. PFOS in muscle tissue of European perch from a nearby lake ranged from 77 to 370 ng g-1 wet weight, representing among the highest values reported worldwide for fish muscle. In Paper II the relative importance of environmental recirculation of PFAAs versus new releases from the technosphere was investigated for PFAAs in WWTP influents. It was shown that tap water can be an important source of PFAAs to WWTPs in areas with elevated environmental levels. This needs to be taken into account when calculating emissions via WWTP effluents. PFAA mass balances over the WWTPs suggested that PFHxA and PFOA were formed from precursor compounds within the plants. Assembled PFAA mass balances for the Baltic Sea (Paper III) showed that river inflow and atmospheric deposition were the dominant input pathways, while wastewater treatment plant (WWTP) effluents discharging directly into the Baltic Sea made a minor contribution. The inputs of PFAAs were estimated to be higher than the outputs, suggesting a current increase of the PFAA inventory in the Baltic Sea. Also the mass balance study of PFAAs in two remote stream catchments presented in Paper IV revealed that inputs dominated over outputs for both catchments, indicating that a considerable portion of the PFAAs deposited from the atmosphere is retained in soil or in deep ground water and may be released to surface and marine water environments in the future

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  • 4.
    Filipovic, Marko
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Mass balance of perfluoroalkyl acids in the Baltic Sea2013Licentiate thesis, comprehensive summary (Other academic)
    Abstract [en]

    Perfluoroalkyl acids (PFAAs) are man-made chemicals. Their unique properties make them beneficial for a wide range of industrial and consumer applications, such as constituents in fire fighting foams, hydraulic oils and food packaging materials.PFAAs have shown to be highly persistent in the environment, and the toxicological potential of long chain PFAA homologues is of a concern. International regulation and voluntary actions by the industry have been implemented and led to reduced primary emissions of PFAAs to the environment. However, the concentrations of some PFAAs in e.g. birds from the Baltic Sea are still very high and of ecotoxicological concern. Measures to reduce the PFAA contamination require an understanding of the sources and how the PFAAs are being transported in the environment.In this licentiate thesis a mass balance was assembled for perfluorohexanoic acid (PFHxA), perfluorooctanoic acid (PFOA), perfluorodecanoic acid (PFDA) and perfluorooctane sulfonic acid (PFOS) in the Baltic Sea. A one-box model was used including the input pathways river inflow, atmospheric deposition, wastewater discharges and inflow from the North Sea via the Danish Straits, while the loss processes considered were sediment burial, transformation of the chemicals and outflow to the North Sea via the Danish Straits. Additionally, the inventories of the four target PFAAs in the Baltic Sea were estimated. Both chemical fluxes and inventories were estimated using recently published monitoring data (2005-2010).In order to obtain a detailed perspective on the current knowledge regarding PFAAs in the Baltic Sea, challenges and uncertainties in data selection were discussed for the most dominant input pathways. This included WWTP emissions and calculation of emission factors (EFs), atmospheric deposition and riverine inflow.River inflow and atmospheric deposition were the dominant inputs, while wastewater treatment plant (WWTP) effluents made a minor contribution. The input to the Baltic Sea exceeded the output for all 4 PFAAs, suggesting that inputs were higher during 2005-2010 than during the previous 20 years despite efforts to reduce emissions of PFAAs. Comparing the difference between PFAA input and output with the PFAA inventory, the doubling time for the concentration in the Baltic Sea was estimated to be 8-94 yr for PFHxA, 12-16 yr for PFOA, 3-5 yr for PFDA and 4 yr for PFOS. The surplus of the input can be an effect of retention and delayed release of PFAAs from atmospheric deposition in the soils and groundwater of the watershed.The licentiate thesis contributes to a holistic understanding of the major input and output pathways and inventories of PFAAs in the Baltic Sea. Furthermore, it points out current knowledge gaps in our understanding of sources and fate of PFAAs in the aquatic environment.

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  • 5.
    Filipovic, Marko
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Berger, Urs
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Are perfluoroalkyl acids in waste water treatment plant effluents the result of primary emissions from the technosphere or of environmental recirculation?2014In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 129, p. 74-80Article in journal (Refereed)
    Abstract [en]

    Wastewater treatment plants (WWTP) have been suggested to be one of the major pathways of perfluoroalkyl acids (PFAAs) from the technosphere to the aquatic environment. The origin of PFAAs in WWTP influents is either from current primary emissions or a result of recirculation of PFAAs that have been residing and transported in the environment for several years or decades. Environmental recirculation can then occur when PFAAs from the environment enter the wastewater stream in, e.g., tap water. In this study 13 PFAAs and perfluorooctane sulfonamide were analyzed in tap water as well as WWTP influent, effluent and sludge from three Swedish cities: Bromma (in the metropolitan area of Stockholm), Bollebygd and Umeå. A mass balance of the WWTPs was assembled for each PFAA. Positive mass balances were observed for PFHxA and PFOA in all WWTPs, indicating the presence of precursor compounds in the technosphere. With regard to environmental recirculation, tap water was an important source of PFAAs to the Bromma WWTP influent, contributing >40% for each quantified sulfonic acid and up to 30% for the carboxylic acids. The PFAAs in tap water from Bollebygd and Umeå did not contribute significantly to the PFAA load in the WWTP influents. Our results show that in order to estimate current primary emissions from the technosphere, it may be necessary to correct the PFAA emission rates in WWTP effluents for PFAAs present in tap water, especially in the case of elevated levels in tap water.

  • 6.
    Filipovic, Marko
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Berger, Urs
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Mass Balance of Perfluoroalkyl Acids in the Baltic Sea2013In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 47, no 9, p. 4088-4095Article in journal (Refereed)
    Abstract [en]

    A mass balance was assembled for perfluorohexanoic acid (PFHxA), perfluorooctanoic acid (PFOA), perfluorodecanoic acid (PFDA), and perfluorooctanesulfonic acid (PFOS) in the Baltic Sea. Inputs (from riverine discharge, atmospheric deposition, coastal wastewater discharges, and the North Sea) and outputs (to sediment burial, transformation of the chemical, and the North Sea), as well as the inventory in the Baltic Sea, were estimated from recently published monitoring data. Formation of the chemicals in the water column from precursors was not considered. River inflow and atmospheric deposition were the dominant inputs, while wastewater treatment plant (WWTP) effluents made a minor contribution (<5%). A mass balance of the Oder River watershed was assembled to explore the sources of the perfluoroalkyl acids (PFAAs) in the river inflow. It indicated that WWTP effluents made only a moderate contribution to riverine discharge (21% for PFOA, 6% for PFOS), while atmospheric deposition to the watershed was 1-2 orders of magnitude greater than WWTP discharges. The input to the Baltic Sea exceeded the output for all four PFAAs, suggesting that inputs were higher during 2005-2010 than during the previous 20 years despite efforts to reduce emissions of PFAAs. One possible explanation is the retention and delayed release of PFAAs from atmospheric deposition in the soils and groundwater of the watershed.

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  • 7.
    Filipovic, Marko
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Laudon, Hjalmar
    McLachlan, Michael
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Berger, Urs
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Mass Balance of Perfluorinated Alkyl Acids (PFAAs) in a Pristine Boreal CatchmentManuscript (preprint) (Other academic)
    Abstract [en]

    Mass balances of ten individual PFAAs in two nested pristine catchments in Northern Sweden with different sizes and hydrological functions were assembled for 2011-2012. Concentrations of PFAAs in rain and snowmelt, as well as in stream water at the outlet of the two watersheds were measured and used to calculate PFAA inputs and outputs to the catchments. The results generally showed a great excess of PFAA inputs for both catchments. During spring flow the stream water showed PFAA patterns resembling the patterns in rain (as opposed to snowmelt) and the mass balances were roughly closed for several PFAAs, suggesting that snowmelt water infiltrating the ground had displaced water from the previous summer. Comparison of PFAA mass balances between the two catchments further suggested that atmospheric inputs of short-chain (replacement) perfluoroalkyl carboxylic acids had increased in the years before sampling, while inputs of the legacy perfluorooctane sulfonic acid had decreased. The overall positive mass balances indicate that a considerable portion of the PFAAs deposited from the atmosphere are stored in soil and may be released to surface and marine water environments in the future.

  • 8.
    Filipovic, Marko
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Laudon, Hjalmar
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Berger, Urs
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Helmholtz Centre for Environmental Research—UFZ, Germany.
    Mass Balance of Perfluorinated Alkyl Acids in a Pristine Boreal Catchment2015In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 49, no 20, p. 12127-12135Article in journal (Refereed)
    Abstract [en]

    Mass balances of ten individual perfluorinated alkyl acids (PFAAs) in two nested pristine catchments in Northern Sweden with different sizes and hydrological functions were assembled for 2011-2012. Concentrations of PFAAs in rain and snowmelt, as well as in streamwater at the outlet of the two watersheds were measured and used to calculate PFAA atmospheric inputs to and riverine outputs from the catchments. The results generally showed a great excess of PFAA inputs for both catchments over the whole study year. However, during the spring flood period, the inputs and outputs were within a factor of 2 for several PFAAs and the streamwater showed PFAA patterns resembling the patterns in rain (as opposed to snowmelt), suggesting that snowmelt water infiltrating the ground had displaced water from the previous summer. Comparison of PFAA mass balances between the two catchments further suggested that atmospheric inputs of short-chain (replacement) perfluoroalkyl carboxylic acids had increased in the years before sampling, while inputs of the legacy perfluorooctane sulfonic acid had decreased. Overall, the mass balances indicate that a considerable portion of the PFAAs deposited from the atmosphere are stored in soil and may be released to surface and marine water environments in the future.

  • 9.
    Filipovic, Marko
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Woldegiorgis, Andreas
    Norström, Karin
    Bibi, Momina
    Lindberg, Maria
    Österås, Ann-Helen
    Historical usage of aqueous film forming foam: A case study of the widespread distribution of perfluoroalkyl acids from a military airport to groundwater, lakes, soils and fish2014In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 129, p. 39-45Article in journal (Refereed)
    Abstract [en]

    Historical usage of aqueous film forming foams (AFFFs) at military airports is a potential source of perfluoroalkyl acids (PFAAs) to the nearby environment. In this study, the distribution of perfluorohexanoic acid (PFHxA), perfluorooctanoic acid (PFOA), perfluorohexane sulfonate (PFHxS) and perfluorooctane sulfonate (PFOS) in soil, groundwater, surface water, tap water well, and fish muscle was investigated at a closed down military airfield (F18) and its surroundings in Stockholm, Sweden. The presence of PFOS at AFFF training sites was inventoried.

    One major finding of the study is that a former airfield, abandoned since 1994, may still be a point source of PFAAs to nearby recipients. PFOS and PFOA were ubiquitous in the soil samples at former AFFF training sites with concentrations ranging from 2.18 to 8520 ng g−1 dry weight and <0.12–287 ng g−1 dry weight respectively. The sum of PFAAs in the groundwater and surface waters ranged from 738 to 51 000 ng L−1 and <MDL to 79.0 ng L−1, respectively. PFOS in European perch ranged from 76.5 to 370 ng g−1 wet weight muscle tissue which is among the highest previously reported worldwide. Our results provide evidence that the historical use of AFFF at the site have contaminated an aquifer (7500 m3 d−1), that will require constant PFAA purification before being used for drinking water production. Despite the fact that the water turnover time in the investigated recipients (of 4–6 months) suggest a depletion of PFAA-contaminants over a quarter of a decade, abandoned airfields may still pose an environmental and human health concern.

  • 10.
    Magnér, Jörgen
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Filipovic, Marko
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Alsberg, Tomas
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Application of a novel solid-phase-extraction sampler and ultra-performance liquid chromatography quadrupole-time-of-flight mass spectrometry for determination of pharmaceutical residues in surface sea water2010In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 80, no 11, p. 1255-1260Article in journal (Refereed)
    Abstract [en]

    In the present study, a multi-residue method based on a bag-solid phase extraction (bag-SPE) technique was evaluated for determination of 10 pharmaceuticals in surface water close to the effluent of a sewage treatment plant (STP) and along a coastal gradient from a STP effluent.

    The 10 compounds selected were caffeine, atenolol, metoprolol, oxazepam, carbamazepine, ketoprofen, naproxen, ibuprofen, diclofenac and gemfibrozil. All analyses were performed using ultra-performance liquid chromatography (UPLC) combined with quadrupole time-of-flight (QTOF) mass spectrometry. The detection limits (LOD) ranged from 1.0 to 13 ng L−1. The method showed linear concentration ranges from 25 to 800 ng L−1 with regression coefficients (R2) better than 0.9801. The recoveries of the selected analytes ranged from 11 to 65% with relative standard deviations (RSD) of <16% and inter-day variations of less than 18%. Isotopically labeled surrogate standards were used to compensate for sampling losses and matrix effects.

    Four of the selected 10 pharmaceuticals (caffeine, metoprolol, oxazepam and carbamazepine) were quantified, at concentrations ranging from 4 to 210 ng L−1.

  • 11.
    Magnér, Jörgen
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Filipovic, Marko
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Alsberg, Tomas
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Development of a method for determination of pharmaceutical residues in surface sea water using bag-SPE and UPLC-QToFManuscript (preprint) (Other academic)
    Abstract [en]

    In the present study, a multi-residue method based on a bag –solid phase extraction (bag-SPE) technique was applied to determine the occurrence of ten pharmaceuticals in surface water close to the effluent of a sewage treatment plant (STP) and along a coastal gradient from a STP effluent.

    The ten compounds selected were caffeine, atenolol, metoprolol, oxazepam, carbamazepine, ketoprofen, naproxen, ibuprofen, diclofenac and gemfibrozil, i.e. a mixture of pharmaceuticals of different therapeutic classes having logarithmic octanol/water partitioning coefficients (Log KOW) ranging from -0.13 to 4.39.

    All analyses were performed using ultra performance liquid chromatography (UPLC) combined with quadrupole time-of-flight (QToF) mass spectrometry.

    The detection limit (LOD) of the pharmaceuticals in water ranged from 1.0-13 ng/L. The method showed consistent linear concentration ranges from 25-800 ng/L with regression coefficients (R2) better than 0.9801. The recoveries of the selected analytes ranged from 10.6-64.5 % with relative standard deviations (RSD) of < 16.4 % and inter-day variations of less than 17.7 %.

    Although the detection limits (LOD) of the analytes were low, only four of the selected ten pharmaceuticals (caffeine, metoprolol, oxazepam and carbamazepine) showed concentrations in surface water higher than the detection levels. The concentrations of the four pharmaceuticals in sea water range from 4-210 ng/L.

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