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  • 1.
    Johansson, Jana
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Stockholm University.
    Sources, transport and fate of perfluoroalkyl acids in the atmosphere2017Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Perfluoroalkyl acids (PFAAs) are man-made chemicals which have been observed in the global environment, even in locations far away from where they are emitted. These persistent substances are taken up in humans and biota and may have toxic effects. Knowledge about how PFAAs are dispersed in the environment is needed to discern strategies to manage their sources and to evaluate the efficacy of adopted legislation. This thesis aimed to increase our understanding of the sources of PFAAs to the atmosphere and how PFAAs are transported in air. The results of Paper I demonstrated that gaseous perfluorooctanoic acid (PFOA) sorbs to typical glass fibre filters (GFFs) used in high-volume air sampling of PFAAs. As a consequence, the fraction of gaseous PFOA present in sampled air is underestimated, while the fraction of PFOA associated with aerosols is overestimated. Replacing GFFs with filters deactivated through silanisation and siliconisation did not eliminate this sampling artefact and is therefore not recommended as a means to determine the gas-particle partitioning of PFAAs. In Paper II, monitoring of the mass of PFOA transferred from water solutions of pH 0.2-5.5 demonstrated that the acid dissociation constant of linear PFOA and the four most ubiquitous branched PFOA isomers is around or below 1. Furthermore, the results demonstrated that the presence of counter ions and organic matter in water retarded, rather than enhanced, the volatilisation of PFOA. Therefore, volatilisation of all isomers of PFOA from environmental waters is expected to be negligible. To further study the transfer of PFAAs from environmental waters to air, Paper III simulated the process of sea spray generation in the laboratory. Strong enrichment of PFAAs was observed from bulk water to the surface microlayer and to aerosols. The enrichment increased with PFAA chain length, indicating that this process is of greater importance for more surface active substances. The highest enrichment was observed in aerosols < 1.6 µm, which can travel over long distances if not rained out. Based on the measured aerosol enrichment factors we estimated that approximately 70 metric tonnes of PFAAs are aerosolised from the global oceans yearly and that 3% of this mass is deposited in terrestrial environments. Paper IV reported the occurrence of branched PFOA isomers in deposition sampled in five geographical locations. The presence of these isomers demonstrated that atmospheric transformation of fluorotelomer alcohols is not the only ongoing source of PFAAs to air. We hypothesised that, additionally, both sea spray aerosols and direct emissions from manufacturing sources contributed to the contamination of the precipitation on different spatial scales. Although further research is required to determine the relative importance of different sources to the atmosphere locally and globally, this thesis has substantially advanced the state-of-the-science by i) demonstrating the significance of an air sampling artefact discussed as an uncertainty in the scientific literature over the past decade, ii) definitively ruling out volatilisation from environmental waters as a source of PFOA to air, iii) demonstrating transfer of PFAAs from seawater to air via sea spray aerosols and thus quantifying the environmental importance of this process, and iv) ultimately demonstrating that several types of sources of PFAAs impact the global atmosphere and thus PFAA contamination patterns in precipitation.

  • 2.
    Johansson, Jana H.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Berger, Urs
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Can the use of deactivated glass fibre filters eliminate sorption artefacts associated with active air sampling of perfluorooctanoic acid?2017In: Environmental Pollution, ISSN 0269-7491, E-ISSN 1873-6424, Vol. 224, p. 779-786Article in journal (Refereed)
    Abstract [en]

    Experimental work was undertaken to test whether gaseous perfluorooctanoic acid (PFOA) sorbs to glassfibre filters (GFFs) during air sampling, causing an incorrect measure of the gas-particle equilibriumdistribution. Furthermore, tests were performed to investigate whether deactivation by siliconisationprevents sorption of gaseous PFOA to filter materials. An apparatus was constructed to closely simulate ahigh-volume air sampler, although with additional features allowing introduction of gaseous test compoundsinto an air stream stripped from particles. The set-up enabled investigation of the sorption ofgaseous test compounds to filter media, eliminating any contribution from particles. Experiments wereperformed under ambient outdoor air conditions at environmentally relevant analyte concentrations.The results demonstrate that gaseous PFOA sorbs to GFFs, but that breakthrough of gaseous PFOA on theGFFs occurs at trace-level loadings. This indicates that during high volume air sampling, filters do notquantitatively capture all the PFOA in the sampled air. Experiments with siliconised GFFs showed thatthis filter pre-treatment reduced the sorption of gaseous PFOA, but that sorption still occurred atenvironmentally relevant air concentrations. We conclude that deactivation of GFFs does not allow forthe separation of gaseous and particle bound perfluorinated carboxylic acids (PFCAs) during active airsampling. Consequently, the well-recognised theory that PFCAs do not prevail as gaseous species in theatmosphere may be based on biased measurements. Caution should be taken to ensure that this artefactwill not bias the conclusions of future field studies.

  • 3.
    Johansson, Jana H.
    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).
    Vestergren, Robin
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM). Norwegian Institute for Air Resarch NILU, Norway.
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Bignert, Anders
    Glynn, Anders
    Darnerud, Per Ola
    Temporal trends (1999-2010) of perfluoroalkyl acids in commonly consumed food items2014In: Environmental Pollution, ISSN 0269-7491, E-ISSN 1873-6424, Vol. 188, p. 102-108Article in journal (Refereed)
    Abstract [en]

    The aim of this study was to determine how dietary exposure to PFAAs has changed over the period when major production changes occurred. Archived samples (1999-2010) of eggs, milk and farmed rainbow trout were analyzed by ultra performance liquid chromatography coupled to tandem mass spectrometry. Statistically significant decreasing trends were observed for concentrations of perfluorooctane sulfonic acid (PFOS) and perfluorohexane sulfonic acid (PFHxS) in fish (p < 0.002 and p < 0.032, respectively) and eggs (p < 0.001 for both compounds). Concentrations of PFOS in fish and eggs decreased by a factor of 10 and 40, respectively. In eggs there was also a statistically significant decreasing trend in concentrations of perfluorooctanoic acid (PFOA). The results of this study demonstrate that PFAA concentrations in food items from agricultural food chains and aquatic food chains close to sources respond rapidly to changes in environmental emissions. Implications for the overall understanding of human exposure are discussed.

  • 4.
    Johansson, Jana H.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Salter, Matthew E.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Acosta Navarro, Juan Camilo
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Leck, Caroline
    Stockholm University, Faculty of Science, Department of Meteorology .
    Nilsson, E. Douglas
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Global transport of perfluoroalkyl acids via sea spray aerosol2019In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 4, p. 635-649Article in journal (Refereed)
    Abstract [en]

    Perfluoroalkyl acids (PFAAs) are persistent organic pollutants found throughout the world's oceans. Previous research suggests that long-range atmospheric transport of these substances may be substantial. However, it remains unclear what the main sources of PFAAs to the atmosphere are. We have used a laboratory sea spray chamber to study water-to-air transfer of 11 PFAAs via sea spray aerosol (SSA). We observed significant enrichment of all PFAAs relative to sodium in the SSA generated. The highest enrichment was observed in aerosols with aerodynamic diameter < 1.6 mm, which had aerosol PFAA concentrations up to similar to 62 000 times higher than the PFAA water concentrations in the chamber. In surface microlayer samples collected from the sea spray chamber, the enrichment of the substances investigated was orders of magnitude smaller than the enrichment observed in the aerosols. In experiments with mixtures of structural isomers, a lower contribution of branched PFAA isomers was observed in the surface microlayer compared to the bulk water. However, no clear trend was observed in the comparison of structural isomers in SSA and bulk water. Using the measured enrichment factors of perfluorooctanoic acid and perfluorooctane sulfonic acid versus sodium we have estimated global annual emissions of these substances to the atmosphere via SSA as well as their global annual deposition to land areas. Our experiments suggest that SSA may currently be an important source of these substances to the atmosphere and, over certain areas, to terrestrial environments.

  • 5.
    Johansson, Jana H.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Shi, Yali
    Salter, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Spatial variation in the atmospheric deposition of perfluoroalkyl acids: source elucidation through analysis of isomer patterns2018In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 20, no 7, p. 997-1006Article in journal (Refereed)
    Abstract [en]

    To evaluate the relevance of different proposed sources of perfluoroalkyl acids (PFAAs) to air, their isomer patterns were analyzed in deposition samples collected from five geographical locations: two urban sites in China (>360 km from known operational fluorochemical manufacturing facilities), one remote marine site in the Azores archipelago and two Swedish sites representing urban and background conditions. Despite variable contributions from linear perfluorooctanoic acid (PFOA) in the samples, the pattern of branched PFOA isomers was similar to those of technical standards manufactured using electrochemical fluorination (ECF). This indicates that atmospheric fate processes have little influence on the isomer profiles of PFOA and that the relative contribution of PFOA manufactured using ECF (typically 20-26% branched isomers) and telomerization (typically one single linear isomer) can be determined in atmospheric deposition samples by analyzing the proportions of branched and linear isomers. In Chinese samples, branched isomers contributed 15-25% to the total loading of PFOA, indicating that the samples were dominated by ECF PFOA. Samples in the Azores had 8-10% contribution from branched PFOA isomers, indicating an approximately equal influence of ECF and telomer sources. Only three of the samples collected in Sweden displayed a quantifiable contribution from branched PFOA isomers (8-13% of overall PFOA loading in the samples). One branched PFNA isomer was observed in samples from the marine sites. Direct manufacturing discharges, transport of sea spray aerosols and degradation of precursors are all suggested to be contributing sources, albeit to different extents, to PFAAs in air at the different geographical locations where precipitation was sampled.

  • 6.
    Johansson, Jana H.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Yan, Hong
    Berger, Urs
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Water-to-air transfer of branched and linear PFOA: Influence of pH, concentration and water type2017In: Emerging Contaminants, ISSN 2405-6650, E-ISSN 2405-6642, Vol. 3, no 1, p. 46-53Article in journal (Refereed)
    Abstract [en]

    The volatilisation of perfluorooctanoic acid (PFOA) was measured experimentally at a range of pH valuesusing a previously published laboratory method. Water-to-air transfer was studied for five structuralisomers, namely: the linear isomer (n-PFOA) and the four most commonly occurring branched isomers(3-, 4-, 5- and 6-PFOA). The influence of water concentration and water type on the pH-dependent waterto-air transfer was also investigated for n-PFOA. The water-to-air transfer was studied over the course of 48 h at pH values ranging from 0.2 to 5.5. Under all experimental conditions tested, the volatilisation ofPFOA was negligible at pH > 2.5. In experiments performed with MilliQ water, volatilisation increasedwith decreasing water pH. In experiments performed with tap water and lake water, maximum volatilisationwas observed at pH 1. The concentration of PFOA in water had no influence on the pH value atwhich water-to-air transfer was observed (i.e. at pH < 2.5) for the concentration range tested (0.1e50 mg/L PFOA in deionised water). Although the percentage of PFOA volatilised was significantly different forthe four branched isomers at low pH, volatilisation was not observed above pH 2.5 for any branchedisomer suggesting that all PFOA isomers have a low pKa. Overall, these laboratory results demonstratethat volatilisation of any structural isomer of PFOA from water is negligible at environmentally-relevantconditions. It is unlikely that PFOA isomers will be fractionated in the environment as a result of volatilisationbecause it is a process of negligible environmental relevance.

  • 7.
    Johansson, Jana
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Salter, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Navarro, Juan-Camilo
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Leck, Caroline
    Stockholm University, Faculty of Science, Department of Meteorology .
    Nilsson, Douglas
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Cousins, Ian
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Global transport of perfluoroalkyl acids via sea spray aerosolManuscript (preprint) (Other academic)
  • 8.
    Johansson, Jana
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Shi, Yali
    Cousins, Ian
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Spatial variation in the atmospheric deposition of perfluoroalkyl acids: source elucidation through analysis of homologue and isomer patternsManuscript (preprint) (Other academic)
    Abstract [en]

    To evaluate the relevance of different proposed sources of perfluoroalkyl acids (PFAAs) to air, PFAA homologue and isomer patterns were analysed in precipitation collected from five geographical locations suspected to be influenced by these different types of sources. In Chinese samples, perflourooctanoic acid (PFOA) dominated the homologue patterns with concentrations exceeding those observed in European samples by a factor of 2-59. Furthermore, the isomer pattern of PFOA in Chinese samples was close to that of technical standards for PFOA manufactured using electrochemical fluorination (ECF). This finding suggests that direct manufacturing emissions of PFOA to air dominate the loading of PFOA in air in these regions of China. The PFAA homologue pattern observed in precipitation sampled in Stockholm was dominated by perfluorohexanoic acid, perfluorononanoic acid (PFNA) and PFOA. The isomer pattern of PFOA was to a large degree linear indicating that telomer-based sources, i.e. most likely atmospheric degradation of fluorotelomer alcohols, dominate in this urban area. Samples from the Azores, a group of islands located in the open Atlantic, were dominated by perfluorooctane sulfonic acid (PFOS), PFNA and PFOA, which displayed an isomer patttern suggestive of input from both ECF and telomer sources. A similar pattern was observed in precipitation collected during winter months at a rural site on the Swedish west coast, while samples taken at this site during summer displayed homologue and isomer patterns more like those observed in Stockholm. We hypothesize that the contribution from ECF PFOA observed in European samples was due to influence from sea spray aerosols and this requires further detailed investigation.

  • 9. Land, Magnus
    et al.
    de Wit, Cynthia A.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Bignert, Anders
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Herzke, Dorte
    Johansson, Jana H.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Martin, Jonathan W.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. University of Alberta, Canada.
    What is the effect of phasing out long-chain per- and polyfluoroalkyl substances on the concentrations of perfluoroalkyl acids and their precursors in the environment? A systematic review2018In: Environmental Evidence, ISSN 2047-2382, E-ISSN 2047-2382, Vol. 7, no 1, article id UNSP 4Article, review/survey (Refereed)
    Abstract [en]

    Background: There is a concern that continued emissions of man-made per-and polyfluoroalkyl substances (PFASs) may cause environmental and human health effects. Now widespread in human populations and in the environment, several PFASs are also present in remote regions of the world, but the environmental transport and fate of PFASs are not well understood. Phasing out the manufacture of some types of PFASs started in 2000 and further regulatory and voluntary actions have followed. The objective of this review is to understand the effects of these actions on global scale PFAS concentrations. Methods: Searches for primary research studies reporting on temporal variations of PFAS concentrations were performed in bibliographic databases, on the internet, through stakeholder contacts and in review bibliographies. No time, document type, language or geographical constraints were applied in the searches. Relevant subjects included human and environmental samples. Two authors screened all retrieved articles. Dual screening of 10% of the articles was performed at title/abstract and full-text levels by all authors. Kappa tests were used to test consistency. Relevant articles were critically appraised by four reviewers, with double checking of 20% of the articles by a second reviewer. Meta-analysis of included temporal trends was considered but judged to not be appropriate. The trends were therefore discussed in a narrative synthesis. Results: Available evidence suggests that human concentrations of perfluorooctane sulfonate (PFOS), perfluorodecane sulfonate (PFDS), and perfluorooctanoic acid (PFOA) generally are declining, while previously increasing concentrations of perfluorohexane sulfonate (PFHxS) have begun to level off. Rapid declines for PFOS-precursors (e.g. perfluorooctane sulfonamide, FOSA) have also been consistently observed in human studies. In contrast, limited data indicate that human concentrations of PFOS and PFOA are increasing in China where the production of these substances has increased. Human concentrations of longer-chained perfluoroalkyl carboxylic acids (PFCAs) with 9-14 carbon atoms are generally increasing or show insignificant trends with too low power to detect a trend. For abiotic and biological environmental samples there are no clear patterns of declining trends. Most substances show mixed results, and a majority of the trends are insignificant with low power to detect a trend. Conclusions: For electrochemically derived PFASs, including PFOS and PFOA, most human studies in North America and Europe show consistent statistically significant declines. This contrasts with findings in wildlife and in abiotic environmental samples, suggesting that declining PFOS, PFOS-precursor and PFOA concentrations in humans likely resulted from removal of certain PFASs from commercial products including paper and board used in food packaging. Increasing concentrations of long-chain PFCAs in most matrices, and in most regions, is likely due to increased use of alternative PFASs. Continued temporal trend monitoring in the environment with well-designed studies with high statistical power are necessary to evaluate the effectiveness of past and continuing regulatory mitigation measures. For humans, more temporal trend studies are needed in regions where manufacturing is most intense, as the one human study available in China is much different than in North America or Europe.

  • 10. Land, Magnus
    et al.
    de Wit, Cynthia A.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Herzke, Dorte
    Johansson, Jana
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Martin, Jonathan W.
    What is the effect of phasing out long-chain per- and polyfluoroalkyl substances on the concentrations of perfluoroalkyl acids and their precursors in the environment? A systematic review protocol2015In: Environmental Evidence, ISSN 2047-2382, E-ISSN 2047-2382, Vol. 4, article id 3Article in journal (Refereed)
    Abstract [en]

    Background

    There is a growing concern in Sweden and elsewhere that continued emissions of per- and polyfluoroalkyl substances (PFASs) may cause environmental as well as human health effects. PFASs are a broad class of man-made substances that have been produced and used in both commercial products and industrial processes for more than 60 years. Although the production and use of some PFASs has been phased-out in some parts of the world, it is not known what effect these actions to date have had on PFAS concentrations in the environment. Owing to the wide diversity of PFASs, it is difficult to generalize their properties, environmental fate and production histories. However, the strength and stability of the C-F bond renders the perfluoroalkyl moieties resistant to heat and environmental degradation. Several PFASs are now occurring even in very remote areas in large parts of the world, but the environmental transport and fate of substances within this group is not well understood. A systematic review may be able to determine whether the concentrations of these substances in different environments are changing in any particular direction with time, and whether the phase-outs have had any effects on the concentration trends.

    Methods

    Searches for primary research studies reporting on temporal variations of PFAS concentrations in the environment will be performed in the scientific literature as well as in other reports. Relevant samples include both abiotic and biological samples including humans. No particular time, document type, language or geographical constraints will be applied. Two authors will screen all retrieved articles. Double screening of about 10% of the articles will be performed by all authors at both title/abstract and full-text levels. Kappa tests will be used to test if the screening is consistent. Relevant articles will be critically appraised by four authors (double checking of 25% of the articles). Quality assessment will focus on selection bias, dating of samples, sample integrity and analytical procedures. Data synthesis will be based on statistical analysis of temporal concentration trends.

  • 11. Shatalov, Victor
    et al.
    Johansson, Jana H.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Wiberg, Karin
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Tracing the origin of dioxins in Baltic air using an atmospheric modeling approach2012In: Atmospheric Pollution Research, ISSN 1309-1042, E-ISSN 1309-1042, Vol. 3, no 4, p. 408-416Article in journal (Refereed)
    Abstract [en]

    Previous work has concluded that the sources of dioxins to the Baltic Sea are dominated by atmospheric deposition. Here, we investigate whether current emission estimates can explain Baltic air levels and deposition fluxes of four selected 2,3,7,8-substituted PCDD/F congeners using an atmospheric modeling approach. The EMEP (European Monitoring and Evaluation Programme) database of emissions for dioxins was used to provide inputs to the selected model (MSCE-POP model) and model predicted levels were compared with measurements of dioxins in air and deposition fluxes at three monitoring stations in Sweden. The model underestimated air concentrations between a factor of 5 and 30, with the level of agreement depending on congener, monitoring station and, importantly, with the compass sector from which the contaminated air mass had arrived. Additional model simulations were undertaken in which emissions were enlarged in some selected areas to optimize agreement between model predictions and measurements. A novel emission adjustment approach is used in an attempt to identify source regions where emissions were in error. The emission adjustment approach improved the agreement between model predictions and measurements for 60% of the measurements within a factor of 3 of model predicted concentrations. However, the agreement was still relatively poor when air masses originated from the SSE and SSW. The model adjustment procedure gives an indication of the magnitude of error in exiting emission estimates, but due to the poor quality of existing emission databases and few quality air monitoring data it is not currently possible to use the emission adjustment approach to accurately identify source regions of error. The approach presented here is promising, however, and could be applied to other substances where better emission and monitoring data are available. (C) Author(s) 2012. This work is distributed under the Creative Commons Attribution 3.0 License.

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