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  • 1. Anderson, J. K.
    et al.
    Brecher, R. W.
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    DeWitt, J.
    Fiedler, H.
    Kannan, K.
    Kirman, C. R.
    Lipscomb, J.
    Priestly, B.
    Schoeny, R.
    Seed, J.
    Verner, M.
    Hays, S. M.
    Grouping of PFAS for human health risk assessment: Findings from an independent panel of experts2022In: Regulatory toxicology and pharmacology, ISSN 0273-2300, E-ISSN 1096-0295, Vol. 134, article id 105226Article in journal (Refereed)
    Abstract [en]

    An expert panel was convened to provide insight and guidance on per-and polyfluoroalkyl substances (PFAS) grouping for the purposes of protecting human health from drinking water exposures, and how risks to PFAS mixtures should be assessed. These questions were addressed through multiple rounds of blind, independent responses to charge questions, and review and comments on co-panelists responses. The experts agreed that the lack of consistent interpretations of human health risk for well-studied PFAS and the lack of information for the vast majority of PFAS present significant challenges for any mixtures risk assessment approach. Most experts agreed that all PFAS should not be grouped together, persistence alone is not sufficient for grouping PFAS for the purposes of assessing human health risk, and that the definition of appropriate subgroups can only be defined on a case-by-case manner. Most panelists agreed that it is inappropriate to assume equal toxicity/potency across the diverse class of PFAS. A tiered approach combining multiple lines of evidence was presented as a possible viable means for addressing PFAS that lack analytical and/or toxicological studies. Most PFAS risk assessments will need to employ assumptions that are more likely to overestimate risk than to underestimate risk, given the choice of assumptions regarding dose-response model, uncertainty factors, and exposure information.

  • 2.
    Armitage,
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Cousins,
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Prevedouros, Kostas
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Macleod, M.
    Russell, M.H.
    Buck, R.C.
    Global-Scale Fate and Transport of Perfluorocarboxylates and Perfluorocarboxylic Acids Emitted from Direct Sources using a Spatially-Resolved Multi-Species Model.2007In: SETAC 17:th Annual Meeting in Europe, Porto, Portugal: 20-24 May, 2007Conference paper (Other (popular science, discussion, etc.))
  • 3.
    Armitage,
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Cousins,
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Prevedouros, Kostas
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Macleod, M.
    Russell, M.H.
    Buck, R.C.
    Modelling the fate and transport of PFCAs emitted from direct sources using a global-scale chemical fate model.2007In: SETAC North America 28th Annual Meeting, in Milwaukee, Wisconsin, USA.: 11-15 November, 2007Conference paper (Other (popular science, discussion, etc.))
  • 4.
    Armitage, J
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Cousins, I
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    MacLeod, M.
    Modelling the long-term fate and transport of PFO(A) emitted from direct sources using a two-dimensional global-scale model2008In: Organohalogen Compd., Vol. 70, p. 1438-1441Article in journal (Refereed)
  • 5.
    Armitage, J
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Cousins, I
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    MacLeod, M.
    Modelling the long-term fate and transport of PFO(A) emitted from direct sources using a two-dimensional global-scale model2008In: Dioxin 2008: 17-22 August, Birmingham, UK, 2008Conference paper (Refereed)
  • 6.
    Armitage, J
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Cousins, I
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Persson, N.J.
    Gustafsson, Ö
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Cornelissen, G
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Saloranta, T.
    Broman, D
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Næs, K.
    Black Carbon-Inclusive Modeling Approaches for Estimating the Aquatic Fate of Dibenzo-p-dioxins and Dibenzofurans2008In: Environ. Sci. Technol., Vol. 42, p. 3697-3703Article in journal (Refereed)
  • 7.
    Armitage, J
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Franco, A.
    Gomez, S.
    Cousins, I
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Modeling the Potential Influence of Particle Deposition on the Accumulation of Organic Contaminants by Submerged Aquatic Vegetation2008In: Environ. Sci. Technol., Vol. 42, p. 4052-4059Article in journal (Refereed)
  • 8.
    Armitage, James
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Cousins, Ian
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Hauck, M.
    Harbers, J.V.
    Huijbregts, M.A.J.
    Empirical evaluation of spatial and non-spatial European-scale multimedia fate models: Results and implications for chemical risk assessment.2007In: J. Environ. Monit., Vol. 9, p. 572-581Article in journal (Refereed)
  • 9.
    Armitage, James M
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Macleod, Matthew
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Cousins, Ian T
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Additions and corrections to “Modeling the global fate and transport of perfluorooctanoic acid (PFOA) and perfluorooctanoate (PFO) emitted from direct sources using a multispecies mass balance model”2009Other (Refereed)
  • 10.
    Armitage, James M
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Macleod, Matthew
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Cousins, Ian T
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Comparative Assessment of the Global Fate and Transport Pathways of Long-chain Perfluorocarboxylic Acids (PFCAs) and Perfluorocarboxylates (PFCs) Emitted from Direct Sources2009In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 43, no 15, p. 5830-5836Article in journal (Refereed)
    Abstract [en]

    A global-scale multispecies mass balance model was used to simulate the long-term fate and transport of perfluorocarboxylic acids (PFCAs) with eight to thirteen carbons (C8−C13) and their conjugate bases, the perfluorocarboxylates (PFCs). The main purpose of this study was to assess the relative long-range transport (LRT) potential of each conjugate pair, collectively termed PFC(A)s, considering emissions from direct sources (i.e., manufacturing and use) only. Overall LRT potential (atmospheric + oceanic) varied as a function of chain length and depended on assumptions regarding pKa and mode of entry. Atmospheric transport makes a relatively higher contribution to overall LRT potential for PFC(A)s with longer chain length, which reflects the increasing trend in the air−water partition coefficient (KAW) of the neutral PFCA species with chain length. Model scenarios using estimated direct emissions of the C8, C9, and C11 PFC(A)s indicate that the mass fluxes to the Arctic marine environment associated with oceanic transport are in excess of mass fluxes from indirect sources (i.e., atmospheric transport of precursor substances such as fluorotelomer alcohols and subsequent degradation to PFCAs). Modeled concentrations of C8 and C9 in the abiotic environment are broadly consistent with available monitoring data in surface ocean waters. Furthermore, the modeled concentration ratios of C8 to C9 are reconcilable with the homologue pattern frequently observed in biota, assuming a positive correlation between bioaccumulation potential and chain length. Modeled concentration ratios of C11 to C10 are more difficult to reconcile with monitoring data in both source and remote regions. Our model results for C11 and C10 therefore imply that either (i) indirect sources are dominant or (ii) estimates of direct emission are not accurate for these homologues.

  • 11.
    Armitage, James M
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McLachlan, Michael
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Cousins, Ian T
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Modeling the Global Fate and Transport of Perfluorooctanoic Acid (PFOA) and Perfluorooctanoate (PFO) Emitted from Direct Sources Using a Multispecies Mass Balance Model2009In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 43, no 4, p. 1134-1140Article in journal (Refereed)
    Abstract [en]

    The global-scale fate and transport processes of perfluorooctanoic acid (PFOA) and perfluorooctanoate (PFO) emitted from direct sources were simulated using a multispecies mass balance model over the period 1950 to 2010. The main goal of this study was to assess the atmospheric and oceanic long-range transport potential of direct source emissions and the implications for the contamination of terrestrial and marine systems worldwide. Consistent with previous modeling studies, ocean transport was found to be the dominant pathway for delivering PFO(A) associated with direct sources to the Arctic marine environment, regardless of model assumptions. The modeled concentrations for surface ocean waters were insensitive to assumptions regarding physical−chemical properties and emission mode of entry and were in reasonable agreement with available monitoring data from the Northern Hemisphere. In contrast, model outputs characterizing atmospheric transport potential were highly sensitive to model assumptions, especially the assumed value of the acid dissociation constant (pKa). However, the complete range of model results for scenarios with different assumptions about partitioning and emissions provide evidence that the atmospheric transport of directly emitted PFO(A) can deliver this substance to terrestrial environments distant from sources. Additional studies in remote or isolated terrestrial systems may provide further insight into the scale of contamination actually attributable to direct sources.

  • 12.
    Armitage, James M
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Schenker, Urs
    Scheringer, Martin
    Martin, Jonathan W
    Macleod, Matthew
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Cousins, Ian T
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Modeling the Global Fate and Transport of Perfluorooctane Sulfonate (PFOS) and Precursor Compounds in Relation to Temporal Trends in Wildlife Exposure.2009In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 43, no 24, p. 9274-80Article in journal (Refereed)
    Abstract [en]

    A global-scale fate and transport model was applied to investigate the historic and future trends in ambient concentrations of perfluorooctane sulfonate (PFOS) and volatile perfluorooctane sulfonyl fluoride (POSF)-based precursor compounds in the environment. First, a global emission inventory for PFOS and its precursor compounds was estimated for the period 1957-2010. We used this inventory as input to a global-scale contaminant fate model and compared modeled concentrations with field data. The main focus of the simulations was to examine how modeled concentrations of PFOS and volatile precursor compounds respond to the major production phase-out that occurred in 2000-2002. Modeled concentrations of PFOS in surface ocean waters are generally within a factor of 5 of field data and are dominated by direct emissions of this substance. In contrast, modeled concentrations of the precursor compounds considered in this study are lower than measured concentrations both before and after the production phase-out. Modeled surface ocean water concentrations of PFOS in source regions decline slowly in response to the production phase-out while concentrations in remote regions continue to increase until 2030. In contrast, modeled concentrations of precursor compounds in both the atmosphere and surface ocean water compartment in all regions respond rapidly to the production phase-out (i.e., decline quickly to much lower levels). With respect to wildlife biomonitoring data, since precursor compounds are bioavailable and degrade to PFOS in vivo, it is at least plausible that declining trends in PFOS body burdens observed in some marine organisms are attributable to this exposure pathway. The continued increases in PFOS body burdens observed in marine organisms inhabiting other regions may reflect exposure primarily to PFOS itself, present in the environment due to production and use of this compound as well as degradation of precursor compounds.

  • 13. Arnot, Jon A.
    et al.
    Armitage, James M.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    McCarty, Lynn S.
    Wania, Frank
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Toose-Reid, Liisa
    Toward a Consistent Evaluative Framework for POP Risk Characterization2011In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 45, no 1, p. 97-103Article in journal (Refereed)
    Abstract [en]

    The purpose of Annex E in the Stockholm Convention (SC) on Persistent Organic Pollutants (POPs) is to assess whether a chemical is likely, as a result of its long-range environmental transport, to lead to significant adverse human health or environmental effects, such that global action is warranted. To date, risk profiles for nominated POPs have not consistently selected assessment endpoints or completed mandated risk characterizations. An assessment endpoint hierarchy is proposed to facilitate risk characterization for the implementation of the SC. The framework is illustrated for a nominated POP, hexabromocyclododecane (HBCD), using three risk estimation methods. Based on current monitoring and toxicity data, the screening-level results indicate that humans and ecological receptors in remote regions such as the Arctic are unlikely to experience significant adverse effects (i.e., low risk) due to long-range environmental transport of HBCD. The results for birds are more uncertain than the results for fish and mammals due to the paucity of avian toxicity data. Risk characterization results for HBCD and for some listed POPs are compared to illustrate how the proposed methods can further assist decision-making and chemical management.

  • 14.
    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.

  • 15. Boucher, Justin M.
    et al.
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Scheringer, Martin
    Hungerbühler, Konrad
    Wang, Zhanyun
    Toward a Comprehensive Global Emission Inventory of C-4-C-10 Perfluoroalkanesulfonic Acids (PFSAs) and Related Precursors: Focus on the Life Cycle of C-6- and C-10-Based Products2019In: Environmental Science and Technology Letters, E-ISSN 2328-8930, Vol. 6, no 1, p. 1-7Article in journal (Refereed)
    Abstract [en]

    A first global emission inventory of C-4-C-10 perfluoroalkanesulfonic acids (PFSAs) released during the life cycle of perfluorohexanesulfonyl fluoride (PHxSF)- and perfluorodecanesulfonyl fluoride (PDSF)-based products is presented. This study complements previous research on emissions of PFSAs that focused largely on the life cycle of perfluorooctanesulfonyl fluoride (POSF) and its derivatives. It reviews and integrates existing information about the life cycle of PHxSF, PDSF, and their derivatives; the limited data available in the public domain point to potentially significant global production, uses, and releases of these substances. Between 1958 and 2015, ranges of total emissions of perfluorohexanesulfonic acid (PFHxS) and perfluorodecanesulfonic acid (PFDS) are estimated to be 120-1022 and 38-378 metric tons, respectively. With the new emission estimates as inputs in a global multimedia environmental fate model (CliMoChem), the model-derived environmental concentrations well capture the reported field concentrations, providing strong support for the plausibility of the developed emission inventories. The results highlight the ongoing environmental exposure to these substances and the need for more detailed data in the public domain about their production levels and uses.

  • 16. Brack, Werner
    et al.
    Ait-Aissa, Selim
    Backhaus, Thomas
    Birk, Sebastian
    Barcelo, Damia
    Burgess, Rob
    Cousins, Ian
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Dulio, Valeria
    Escher, Beate I.
    Focks, Andreas
    van Gils, Jos
    Ginebreda, Antoni
    Hering, Daniel
    Hewitt, L. Mark
    Hilscherova, Klara
    Hollender, Juliane
    Hollert, Henner
    Kock, Marianne
    Kortenkamp, Andreas
    Lopez de Alda, Miren
    Mueller, Christin
    Posthuma, Leo
    Schueuermann, Gerrit
    Schymanski, Emma
    Segner, Helmut
    Sleeuwaert, Frank
    Slobodnik, Jaroslav
    Teodorovic, Ivana
    Umbuzeiro, Gisela
    Voulvoulis, Nick
    van Wezel, Annemarie
    Altenburger, Rolf
    Strengthen the European collaborative environmental research to meet European policy goals for achieving a sustainable, non-toxic environment2019In: Environmental Sciences Europe, ISSN 2190-4707, E-ISSN 2190-4715, Vol. 31, no 1, article id 63Article in journal (Refereed)
    Abstract [en]

    To meet the United Nations (UN) sustainable development goals and the European Union (EU) strategy for a non-toxic environment, water resources and ecosystems management require cost-efficient solutions for prevailing complex contamination and multiple stressor exposures. For the protection of water resources under global change conditions, specific research needs for prediction, monitoring, assessment and abatement of multiple stressors emerge with respect to maintaining human needs, biodiversity, and ecosystem services. Collaborative European research seems an ideal instrument to mobilize the required transdisciplinary scientific support and tackle the large-scale dimension and develop options required for implementation of European policies. Calls for research on minimizing society's chemical footprints in the water-food-energy-security nexus are required. European research should be complemented with targeted national scientific funding to address specific transformation pathways and support the evaluation, demonstration and implementation of novel approaches on regional scales. The foreseeable pressure developments due to demographic, economic and climate changes require solution-oriented thinking, focusing on the assessment of sustainable abatement options and transformation pathways rather than on status evaluation. Stakeholder involvement is a key success factor in collaborative projects as it allows capturing added value, to address other levels of complexity, and find smarter solutions by synthesizing scientific evidence, integrating governance issues, and addressing transition pathways. This increases the chances of closing the value chain by implementing novel solutions. For the water quality topic, the interacting European collaborative projects SOLUTIONS, MARS and GLOBAQUA and the NORMAN network provide best practice examples for successful applied collaborative research including multi-stakeholder involvement. They provided innovative conceptual, modelling and instrumental options for future monitoring and management of chemical mixtures and multiple stressors in European water resources. Advancement of EU water framework directive-related policies has therefore become an option.

  • 17. Brack, Werner
    et al.
    Altenburger, Rolf
    Schueuermann, Gerrit
    Krauss, Martin
    Herraez, David Lopez
    van Gils, Jos
    Slobodnik, Jaroslav
    Munthe, John
    Gawlik, Bernd Manfred
    van Wezel, Annemarie
    Schriks, Merijn
    Hollender, Juliane
    Tollefsen, Knut Erik
    Mekenyan, Ovanes
    Dimitrov, Saby
    Bunke, Dirk
    Cousins, Ian
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Posthuma, Leo
    van den Brink, Paul J.
    Lopez de Alda, Miren
    Barcelo, Damia
    Faust, Michael
    Kortenkamp, Andreas
    Scrimshaw, Mark
    Ignatova, Svetlana
    Engelen, Guy
    Massmann, Gudrun
    Lemkine, Gregory
    Teodorovic, Ivana
    Walz, Karl-Heinz
    Dulio, Valeria
    Jonker, Michiel T. O.
    Jaeger, Felix
    Chipman, Kevin
    Falciani, Francesco
    Liska, Igor
    Rooke, David
    Zhang, Xiaowei
    Hollert, Henner
    Vrana, Branislav
    Hilscherova, Klara
    Kramer, Kees
    Neumann, Steffen
    Hammerbacher, Ruth
    Backhaus, Thomas
    Mack, Juliane
    Segner, Helmut
    Escher, Beate
    Umbuzeiro, Gisela de Aragao
    The SOLUTIONS project: Challenges and responses for present and future emerging pollutants in land and water resources management2015In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 503, p. 22-31Article in journal (Refereed)
    Abstract [en]

    SOLUTIONS (2013 to 2018) is a European Union Seventh Framework Programme Project (EU-FP7). The project aims to deliver a conceptual framework to support the evidence-based development of environmental policies with regard to water quality. SOLUTIONS will develop the tools for the identification, prioritisation and assessment of those water contaminants that may pose a risk to ecosystems and human health. To this end, a new generation of chemical and effect-based monitoring tools is developed and integrated with a full set of exposure, effect and risk assessment models. SOLUTIONS attempts to address legacy, present and future contamination by integrating monitoring and modelling based approaches with scenarios on future developments in society, economy and technology and thus in contamination. The project follows a solutions-oriented approach by addressing major problems of water and chemicals management and by assessing abatement options. SOLUTIONS takes advantage of the access to the infrastructure necessary to investigate the large basins of the Danube and Rhine as well as relevant Mediterranean basins as case studies, and puts major efforts on stakeholder dialogue and support. Particularly, the EU Water Framework Directive (WFD) Common Implementation Strategy (CIS) working groups, International River Commissions, and water works associations are directly supported. with consistent guidance for the early detection, identification, prioritisation, and abatement of chemicals in the water cycle. SOLUTIONS will give a specific emphasis on concepts and tools for the impact and risk assessment of complex mixtures of emerging pollutants, their metabolites and transformation products. Analytical and effect-based screening tools will be applied together with ecological assessment tools for the identification of toxicants and their impacts. The SOLUTIONS approach is expected to provide transparent and evidence-based candidates or River Basin Specific Pollutants in the case study basins and to assist future review of priority pollutants under the WFD as well as potential abatement options.

  • 18. Brack, Werner
    et al.
    Dulio, Valeria
    Ågerstrand, Marlene
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Allan, Ian
    Altenburger, Rolf
    Brinkmann, Markus
    Bunke, Dirk
    Burgess, Robert M.
    Cousins, Ian
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Escher, Beate I.
    Hernandez, Felix J.
    Hewitt, L. Mark
    Hilscherova, Klara
    Hollender, Juliane
    Hollert, Henner
    Kase, Robert
    Klauer, Bernd
    Lindim, Claudia
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Herraez, David Lopez
    Miege, Cecil
    Munthe, John
    O'Toole, Simon
    Posthuma, Leo
    Ruedel, Heinz
    Schaefer, Ralf B.
    Sengl, Manfred
    Smedes, Foppe
    van de Meent, Dik
    van den Brink, Paul J.
    van Gils, Jos
    van Wezel, Annemarie P.
    Vethaak, A. Dick
    Vermeirssen, Etienne
    von der Ohe, Peter C.
    Vrana, Branislav
    Towards the review of the European Union Water Framework Directive: Recommendations for more efficient assessment and management of chemical contamination in European surface water resources2017In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 576, p. 720-737Article, review/survey (Refereed)
    Abstract [en]

    Water is a vital resource for natural ecosystems and human life, and assuring a high quality of water and protecting it from chemical contamination is a major societal goal in the European Union. The Water Framework Directive (WFD) and its daughter directives are the major body of legislation for the protection and sustainable use of European freshwater resources. The practical implementation of the WFD with regard to chemical pollution has faced some challenges. In support of the upcoming WFD review in 2019 the research project SOLUTIONS and the European monitoring network NORMAN has analyzed these challenges, evaluated the state-of-the-art of the science and suggested possible solutions. We give 10 recommendations to improve monitoring and to strengthen comprehensive prioritization, to foster consistent assessment and to support solution-oriented management of surface waters. The integration of effect-based tools, the application of passive sampling for bioaccumulative chemicals and an integrated strategy for prioritization of contaminants, accounting for knowledge gaps, are seen as important approaches to advance monitoring. Including all relevant chemical contaminants in more holistic chemical status assessment, using effect-based trigger values to address priority mixtures of chemicals, to better consider historical burdens accumulated in sediments and to use models to fill data gaps are recommended for a consistent assessment of contamination. Solution-oriented management should apply a tiered approach in investigative monitoring, to identify toxicity drivers, strengthen consistent legislative frameworks and apply solutions-oriented approaches that explore risk reduction scenarios before and along with risk assessment.

  • 19.
    Bui, Thuy T.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. IVL Swedish Environmental Research Institute, Sweden.
    Alves, Andreia
    Palm-Cousins, Anna
    Voorspoels, Stefan
    Covaci, Adrian
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Estimating uptake of phthalate ester metabolites into the human nail plate using pharmacokinetic modelling2017In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 100, p. 148-155Article in journal (Refereed)
    Abstract [en]

    There is a lack of knowledge regarding uptake of phthalate esters (PEs) and other chemicals into the human nail plate and thus, clarity concerning the suitability of human nails as a valid alternative matrix for monitoring longterm exposure. In particular, the relative importance of internal uptake of phthalate metabolites (from e.g. blood) compared to external uptake pathways is unknown. This study provides first insights into the partitioning of phthalate-metabolites between blood and nail using pharmacokinetic (PK) modelling and biomonitoring data from a Norwegian cohort. A previously published PK model (Lorber PK model) was used in combination with measured urine data to predict serum concentrations of DEHP and DnBP/DiBP metabolites at steady state. Then, partitioning between blood and nail was assessed assuming equilibrium conditions and treating the nail plate as a tissue, assuming a fixed lipid and water content. Although calculated as a worst-case scenario at equilibrium, the predicted nail concentrations of metabolites were lower than the biomonitoring data by factors of 44 to 1300 depending on the metabolite. It is therefore concluded that internal uptake of phthalate metabolites from blood into nail is a negligible pathway and does not explain the observed nail concentrations. Ingtead, external uptake pathways are more likely to dominate, possibly through deposition of phthalates onto the skin/nail and subsequent metabolism. Modelling gaseous diffusive uptake of PEs from air to nail revealed that this pathway is unlikely to be important. Experimental quantification of internal and external uptake pathways of phthalates and their metabolites into the human nail plate is needed to verify these modelling results. However, based on this model, human nails are not a good indicator of internal human exposure for the phthalate esters studied.

  • 20.
    Bui, Thuy T.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. IVL Swedish Environmental Research Institute, Sweden.
    Giovanoulis, Georgios
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. IVL Swedish Environmental Research Institute, Sweden.
    Palm Cousins, Anna
    Magnér, Jörgen
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    de Wit, Cynthia A.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Human exposure, hazard and risk of alternative plasticizers to phthalate esters2016In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 541, p. 451-467Article in journal (Refereed)
    Abstract [en]

    Alternative plasticizers to phthalate esters have been used for over a decade, but data regarding emissions, human exposure and health effects are limited. Here we review 20 alternative plasticizers in current use and their human exposure, hazard and risk. Physicochemical properties are collated for these diverse alternatives and log K-OW values range over 15 orders of magnitude and log K-AW and log K-OA values over about 9 orders of magnitude. Most substances are hydrophobic with low volatility and are produced in high volumes for use in multiple applications. There is an increasing trend in the total use of alternative plasticizers in Sweden compared to common phthalate esters in the last 10 years, especially for DINCH. Evaluative indoor fate modeling reveals that most alternatives are distributed to vertical surfaces (e.g. walls or ceilings). Only TXIB and GTA are predicted to be predominantly distributed to indoor air. Human exposure data are lacking and clear evidence for human exposure only exists for DEHT and DINCH, which show increasing trends in body burdens. Human intake rates are collected and compared with limit values with resulting risk ratios below 1 except for infant's exposure to ESBO. PBT properties of the alternatives indicate mostly no reasons for concern, except that TEHPA is estimated to be persistent and TCP toxic. A caveat is that non-standard toxicological endpoint results are not available and, similar to phthalate esters, the alternatives are likely pseudo-persistent. Keydata gaps for more comprehensive risk assessment are identified and include: analytical methods to measure metabolites in biological fluids and tissues, toxicological information regarding non-standard endpoints such as endocrine disruption and a further refined exposure assessment in order to consider high risk groups such as infants, toddlers and children.

  • 21.
    Bui, Thuy T.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. IVL Swedish Environmental Research Institute, Sweden.
    Xu, Fuchao
    Van den Eede, Nele
    Palm Cousins, Anna
    IVL Swedish Environmental Research Institute, Sweden.
    Covaci, Adrian
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Probing the relationship between external and internal human exposure of organophosphate flame retardants using pharmacokinetic modelling2017In: Environmental Pollution, ISSN 0269-7491, E-ISSN 1873-6424, Vol. 230, p. 550-560Article in journal (Refereed)
    Abstract [en]

    Human external exposure (i.e. intake) of organophosphate flame retardants (PFRs) has recently been quantified, but no link has yet been established between external and internal exposure. In this study, we used a pharmacokinetic (PK) model to probe the relationship between external and internal exposure data for three PFRs (EHDPHP, TNBP and TPHP) available for a Norwegian cohort of 61 individuals from 61 different households. Using current literature on metabolism of PFRs,, we predicted the metabolite serum/urine concentrations and compared it to measured data from the study population. Unavailable parameters were estimated using a model fitting approach (least squares method) after assigning reasonable constraints on the ranges of fitted parameters. Results showed an acceptable comparison between PK model estimates and measurements (<10-fold deviation) for EHDPHP. However, a deviation of 10-1000 was observed between PM model estimates and measurements for TNBP and TPHP. Sensitivity and uncertainty analysis on the PK model revealed that EHDPHP results showed higher uncertainty than TNBP or TPHP. However, there are indications that (1) current biomarkers of exposure (i.e. assumed metabolites) for TNBP and TPHP chemicals might not be specific and ultimately affecting the outcome of the modelling and (2) some exposure pathways might be missing. Further research, such as in vivo laboratory metabolism experiments of PFRs including identification of better biomarkers will reduce uncertainties in human exposure assessment.

  • 22.
    Bui, Tuong Thuy
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Xu, Fuchao
    Van den Eede, Nele
    Palm Cousins, Anna
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Covaci, Adrian
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Probing the relationship between external and internal human exposure of organophosphate flame retardants using pharmacokinetic modellingManuscript (preprint) (Other academic)
    Abstract [en]

    Human external exposure (i.e. intake) of organophosphate flame retardants (PFRs) has recently been quantified, but no link has yet been established between external and internal exposure. In this study, we used a pharmacokinetic (PK) model to probe the relationship between external and internal exposure data for three PFRs (EHDPHP, TNBP and TPHP) available for a Norwegian cohort of 61 individuals from 61 different households. Using current literature on metabolism of PFRs, we predicted the human body burden and compared it to the measured serum and urine data for the PFRs metabolites. Unavailable parameters were estimated using a model fitting approach (least squares method) after assigning reasonable constraints on the ranges of fitted parameters. Results showed an acceptable comparison between PK model estimates and measurements (< 10-fold deviation) for EHDPHP. However, a deviation of 10-1000 was observed between PK model estimates and measurements for TNBP and TPHP. Sensitivity and uncertainty analysis on the PK model revealed that EHDPHP results showed higher uncertainty than TNBP or TPHP. However, there are indications that (1) current biomarkers of exposure (i.e. assumed metabolites) for TNBP and TPHP chemicals might not be specific and ultimately affecting the outcome of the modeling, (2) some exposure pathways might be missing. Further research, such as in vivo laboratory metabolism experiments of PFRs including identification of better biomarkers will reduce uncertainties in human exposure assessment.

  • 23. Carlsson, Pernilla
    et al.
    Breivik, Knut
    Brorström-Lundén, Eva
    Cousins, Ian
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Christensen, Jesper
    Grimalt, Joan O.
    Halsall, Crispin
    Kallenborn, Roland
    Abass, Khaled
    Lammel, Gerhard
    Munthe, John
    MacLeod, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Øyvind Odland, Jon
    Pawlak, Janet
    Rautio, Arja
    Reiersen, Lars-Otto
    Schlabach, Martin
    Stemmler, Irene
    Wilson, Simon
    Wöhrnschimmel, Henry
    Polychlorinated biphenyls (PCBs) as sentinels for the elucidation of Arctic environmental change processes: a comprehensive review combined with ArcRisk project results2018In: Environmental Science and Pollution Research, ISSN 0944-1344, E-ISSN 1614-7499, Vol. 25, no 23, p. 22499-22528Article, review/survey (Refereed)
    Abstract [en]

    Polychlorinated biphenyls (PCBs) can be used as chemical sentinels for the assessment of anthropogenic influences on Arctic environmental change. We present an overview of studies on PCBs in the Arctic and combine these with the findings from ArcRisk-a major European Union-funded project aimed at examining the effects of climate change on the transport of contaminants to and their behaviour of in the Arctic-to provide a case study on the behaviour and impact of PCBs over time in the Arctic. PCBs in the Arctic have shown declining trends in the environment over the last few decades. Atmospheric long-range transport from secondary and primary sources is the major input of PCBs to the Arctic region. Modelling of the atmospheric PCB composition and behaviour showed some increases in environmental concentrations in a warmer Arctic, but the general decline in PCB levels is still the most prominent feature. 'Within-Arctic' processing of PCBs will be affected by climate change-related processes such as changing wet deposition. These in turn will influence biological exposure and uptake of PCBs. The pan-Arctic rivers draining large Arctic/sub-Arctic catchments provide a significant source of PCBs to the Arctic Ocean, although changes in hydrology/sediment transport combined with a changing marine environment remain areas of uncertainty with regard to PCB fate. Indirect effects of climate change on human exposure, such as a changing diet will influence and possibly reduce PCB exposure for indigenous peoples. Body burdens of PCBs have declined since the 1980s and are predicted to decline further.

  • 24.
    Cornelissen, G
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Cousins, I
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Wiberg, K.
    Tysklind, M.
    Holmström, H.
    Broman, D
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Black carbon-dominated PCDD/Fs sorption to soils at a former wood impregnation site2008In: Chemosphere, Vol. 72, p. 1455-1461Article in journal (Refereed)
  • 25.
    Cousins, I
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Berger, U
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Overview of Research on Perfluorinated Compounds at ITM2008In: Naturvårdsverket: 27 May, 2008Conference paper (Refereed)
  • 26.
    Cousins, Ian
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Johansson, Jana H.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Salter, Matthew E.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Sha, Bo
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Scheringer, Martin
    Outside the Safe Operating Space of a New Planetary Boundary for Per- and Polyfluoroalkyl Substances (PFAS)2022In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 56, no 16, p. 11172-11179Article in journal (Refereed)
    Abstract [en]

    It is hypothesized that environmental contamination by per- and polyfluoroalkyl substances (PFAS) defines a separate planetary boundary and that this boundary has been exceeded. This hypothesis is tested by comparing the levels of four selected perfluoroalkyl acids (PFAAs) (i.e., perfluorooctanesulfonic acid (PFOS), perfluorooctanoic acid (PFOA), perfluorohexanesulfonic acid (PFHxS), and perfluorononanoic acid (PFNA)) in various global environmental media (i.e., rainwater, soils, and surface waters) with recently proposed guideline levels. On the basis of the four PFAAs considered, it is concluded that (1) levels of PFOA and PFOS in rainwater often greatly exceed US Environmental Protection Agency (EPA) Lifetime Drinking Water Health Advisory levels and the sum of the aforementioned four PFAAs (Σ4 PFAS) in rainwater is often above Danish drinking water limit values also based on Σ4 PFAS; (2) levels of PFOS in rainwater are often above Environmental Quality Standard for Inland European Union Surface Water; and (3) atmospheric deposition also leads to global soils being ubiquitously contaminated and to be often above proposed Dutch guideline values. It is, therefore, concluded that the global spread of these four PFAAs in the atmosphere has led to the planetary boundary for chemical pollution being exceeded. Levels of PFAAs in atmospheric deposition are especially poorly reversible because of the high persistence of PFAAs and their ability to continuously cycle in the hydrosphere, including on sea spray aerosols emitted from the oceans. Because of the poor reversibility of environmental exposure to PFAS and their associated effects, it is vitally important that PFAS uses and emissions are rapidly restricted.

  • 27.
    Cousins, Ian
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Kong, Deguo
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Vestergren, Robin
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Reconciling measurement and modelling studies of the sources and fate of perfluorinated carboxylates2011In: Environmental Chemistry, ISSN 1448-2517, E-ISSN 1449-8979, Vol. 8, no 4, p. 339-354Article, review/survey (Refereed)
    Abstract [en]

    This study critically evaluates the recently published measurement and modelling studies of the sources and fate of perfluorinated carboxylates (PFCAs). It is concluded that modelling studies provide support to the 'direct hypothesis' for PFOA and PFNA (i.e. the global dominance of direct sources (mainly from fluoropolymer manufacturing)). Empirical evidence for the importance of direct sources of PFOA and PFNA is provided by PFNA : PFOA ratios and isomer profiles of PFOA in ocean water. However, homologue patterns of long-chain PFCAs in biota from remote regions suggest that indirect sources (mainly from precursor degradation) are proportionally more important for PFCAs with more than 10 carbons. Temporal data in biotic and abiotic media are reviewed and an increasing trend to 2000 is observed for all PFCAs, with discrepancies in time trends reported after that period. Some studies on temporal patterns report a levelling off or decline in the latter part of the 2000s for PFOA and PFNA, whereas others show a continual increase throughout the study period. Differences in temporal patterns result from the fact that some environments respond faster to emission changes than others and may thus be useful to elucidate the importance of direct and indirect sources to different regions.

  • 28.
    Cousins, Ian T.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Balan, Simona A.
    Scheringer, Martin
    Weber, Roland
    Wang, Zhanyun
    Blum, Arlene
    Diamond, Miriam
    Fletcher, Tony
    Goldenman, Gretta
    Higgins, Christopher
    Lindeman, Avery E.
    Peaslee, Graham
    Trier, Xenia
    de Voogt, Pim
    Comment on “Fluorotechnology Is Critical to Modern Life: The FluoroCouncil Counterpoint to the Madrid Statement”2015In: Journal of Environmental Health Perspectives, ISSN 0091-6765, E-ISSN 1552-9924, Vol. 123, no 7, p. A170-A170Article in journal (Other academic)
  • 29.
    Cousins, Ian T.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    De Witt, Jamie C.
    Glüge, Juliane
    Goldenman, Gretta
    Herzke, Dorte
    Lohmann, Rainer
    Miller, Mark
    Ng, Carla A.
    Patton, Sharyle
    Scheringer, Martin
    Trier, Xenia
    Wang, Zhanyun
    Finding essentiality feasible: common questions and misinterpretations concerning the "essential-use" concept2021In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 23, no 8, p. 1079-1087Article, review/survey (Refereed)
    Abstract [en]

    The essential-use concept is a tool that can guide the phase-out of per- and polyfluoroalkyl substances (PFAS) and potentially other substances of concern. This concept is a novel approach to chemicals management that determines whether using substances of concern, such as PFAS, is truly essential for a given functionality. To assess the essentiality of a particular use case, three considerations need to be addressed: (1) the function (chemical, end use and service) that the chemical provides in the use case, (2) whether the function is necessary for health and safety and critical for the functioning of society and (3) if the function is necessary, whether there are viable alternatives for the chemical for this particular use. A few illustrative examples of the three-step process are provided for use cases of PFAS. The essential-use concept takes chemicals management away from a substance-by-substance approach to a group approach. For PFAS and other substances of concern, it offers a more rapid pathway toward effective management or phase-out. Parts of the concept of essential use have already been widely applied in global treaties and international regulations and it has also been recently used by product manufacturers and retailers to phase out substances of concern from supply chains. Herein some of the common questions and misinterpretations regarding the practical application of the essential-use concept are reviewed, and answers and further clarifications are provided.

  • 30.
    Cousins, Ian T.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    DeWitt, Jamie C.
    Glüge, Juliane
    Goldenman, Gretta
    Herzke, Dorte
    Lohmann, Rainer
    Miller, Mark
    Ng, Carla A.
    Scheringer, Martin
    Vierke, Lena
    Wang, Zhanyun
    Strategies for grouping per- and polyfluoroalkyl substances (PFAS) to protect human and environmental health2020In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 22, no 7, p. 1444-1460Article, review/survey (Refereed)
    Abstract [en]

    Grouping strategies are needed for per- and polyfluoroalkyl substances (PFAS), in part, because it would be time and resource intensive to test and evaluate the more than 4700 PFAS on the global market on a chemical-by-chemical basis. In this paper we review various grouping strategies that could be used to inform actions on these chemicals and outline the motivations, advantages and disadvantages for each. Grouping strategies are subdivided into (1) those based on the intrinsic properties of the PFAS (e.g.persistence, bioaccumulation potential, toxicity, mobility, molecular size) and (2) those that inform risk assessment through estimation of cumulative exposure and/or effects. The most precautionary grouping approach of those reviewed within this article suggests phasing out PFAS based on their high persistence alone (the so-called P-sufficient approach). The least precautionary grouping approach reviewed advocates only grouping PFAS for risk assessment that have the same toxicological effects, modes and mechanisms of action, and elimination kinetics, which would need to be well documented across different PFAS. It is recognised that, given jurisdictional differences in chemical assessment philosophies and methodologies, no one strategy will be generally acceptable. The guiding question we apply to the reviewed grouping strategies is: grouping for what purpose? The motivation behind the grouping (e.g.determining use in productsvs.setting guideline levels for contaminated environments) may lead to different grouping decisions. This assessment provides the necessary context for grouping strategies such that they can be adopted as they are, or built on further, to protect human and environmental health from potential PFAS-related effects.

  • 31.
    Cousins, Ian T.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    DeWitt, Jamie C.
    Glüge, Juliane
    Goldenman, Gretta
    Herzke, Dorte
    Lohmann, Rainer
    Ng, Carla A.
    Scheringer, Martin
    Wang, Zhanyun
    The high persistence of PFAS is sufficient for their management as a chemical class2020In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 22, no 12, p. 2307-2312Article, review/survey (Refereed)
    Abstract [en]

    Per- and polyfluoroalkyl substances (PFAS) are a class of synthetic organic substances with diverse structures, properties, uses, bioaccumulation potentials and toxicities. Despite this high diversity, all PFAS are alike in that they contain perfluoroalkyl moieties that are extremely resistant to environmental and metabolic degradation. The vast majority of PFAS are therefore either non-degradable or transform ultimately into stable terminal transformation products (which are still PFAS). Under the European chemicals regulation this classifies PFAS as very persistent substances (vP). We argue that this high persistence is sufficient concern for their management as a chemical class, and for all non-essential uses of PFAS to be phased out. The continual release of highly persistent PFAS will result in increasing concentrations and increasing probabilities of the occurrence of known and unknown effects. Once adverse effects are identified, the exposure and associated effects will not be easily reversible. Reversing PFAS contamination will be technically challenging, energy intensive, and costly for society, as is evident in the efforts to remove PFAS from contaminated land and drinking water sources.

  • 32.
    Cousins, Ian T.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Goldenman, Gretta
    Herzke, Dorte
    Lohmann, Rainer
    Miller, Mark
    Ng, Carla A.
    Patton, Sharyle
    Scheringer, Martin
    Trier, Xenia
    Vierke, Lena
    Wang, Zhanyun
    DeWitt, Jamie C.
    The concept of essential use for determining when uses of PFASs can be phased out2019In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 11, p. 1803-1815Article, review/survey (Refereed)
    Abstract [en]

    Because of the extreme persistence of per- and polyfluoroalkyl substances (PFASs) and their associated risks, the Madrid Statement argues for stopping their use where they are deemed not essential or when safer alternatives exist. To determine when uses of PFASs have an essential function in modern society, and when they do not, is not an easy task. Here, we: (1) develop the concept of essential use based on an existing approach described in the Montreal Protocol, (2) apply the concept to various uses of PFASs to determine the feasibility of elimination or substitution of PFASs in each use category, and (3) outline the challenges for phasing out uses of PFASs in society. In brief, we developed three distinct categories to describe the different levels of essentiality of individual uses. A phase-out of many uses of PFASs can be implemented because they are not necessary for the betterment of society in terms of health and safety, or because functional alternatives are currently available that can be substituted into these products or applications. Some specific uses of PFASs would be considered essential because they provide for vital functions and are currently without established alternatives. However, this essentiality should not be considered as permanent; rather, constant efforts are needed to search for alternatives. We provide a description of several ongoing uses of PFASs and discuss whether these uses are essential or non-essential according to the three essentiality categories. It is not possible to describe each use case of PFASs in detail in this single article. For follow-up work, we suggest further refining the assessment of the use cases of PFASs covered here, where necessary, and expanding the application of this concept to all other uses of PFASs. The concept of essential use can also be applied in the management of other chemicals, or groups of chemicals, of concern.

  • 33.
    Cousins, Ian T.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Ng, Carla A.
    Wang, Zhanyun
    Scheringer, Martin
    Why is high persistence alone a major cause of concern?2019In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 5, p. 781-792Article, review/survey (Refereed)
    Abstract [en]

    Persistence is a hazard criterion for chemicals enshrined in chemical regulation worldwide. In this paper, we argue that the higher the persistence of a chemical, the greater the emphasis that it should be given in chemicals assessment and decision making. We provide case studies for three classes of highly persistent chemicals (chlorofluorocarbons, polychlorinated biphenyls, and per-and polyfluoroalkyl substances) to exemplify problems unique to highly persistent chemicals, despite their otherwise diverse properties. Many well-known historical chemical pollution problems were the result of the release of highly persistent chemicals. Using evaluative modeling calculations, we demonstrate that if a chemical is highly persistent, its continuous release will lead to continuously increasing contamination irrespective of the chemical's physical-chemical properties. We argue that these increasing concentrations will result in increasing probabilities of the occurrence of known and unknown effects and that, once adverse effects are identified, it will take decades, centuries or even longer to reverse contamination and therefore effects. Based on our findings we propose that high persistence alone should be established as a sufficient basis for regulation of a chemical, which we term the P-sufficient approach. We argue that regulation on high persistence alone is not over-precautionary given the historical and ongoing problems that persistent chemicals have caused. Regulation of highly persistent chemicals, for example by restriction of emissions, would not only be precautionary, but would serve to prevent poorly reversible future impacts.

  • 34.
    Cousins, Ian T.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Vestergren, Robin
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Wang, Zhanyun
    Scheringer, Martin
    McLachlan, Michael S.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    The precautionary principle and chemicals management: The example of perfluoroalkyl acids in groundwater2016In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 94, p. 331-340Article, review/survey (Refereed)
    Abstract [en]

    Already in the late 1990s microgram-per-liter levels of perfluorooctane sulfonate (PFOS) were measured in water samples from areas where fire-fighting foams were used or spilled. Despite these early warnings, the problems of groundwater, and thus drinking water, contaminated with perfluoroalkyl and polyfluoroalkyl substances (PFASs) including PFOS are only beginning to be addressed. It is clear that this PFAS contamination is poorly reversible and that the societal costs of clean-up will be high. This inability to reverse exposure in a reasonable timeframe is a major motivation for application of the precautionary principle in chemicals management. We conclude that exposure can be poorly reversible; 1) due to slow elimination kinetics in organisms, or 2) due to poorly reversible environmental contamination that leads to continuous exposure. In the second case, which is relevant for contaminated groundwater, the reversibility of exposure is not related to the magnitude of a chemical's bioaccumulation potential. We argue therefore that all PFASs entering groundwater, irrespective of their perfluoroalkyl chain length and bioaccumulation potential, will result in poorly reversible exposures and risks as well as further clean-up costs for society. To protect groundwater resources for future generations, society should consider a precautionary approach to chemicals management and prevent the use and release of highly persistent and mobile chemicals such as PFASs. (C) 2016 Elsevier Ltd. All rights reserved.

  • 35.
    Dalmijn, Joost
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Gluge, Juliane
    Scheringer, Martin
    Cousins, Ian
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Emission inventory of PFASs and other fluorinated organic substances for the fluoropolymer production industry in Europe2024In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895Article in journal (Refereed)
    Abstract [en]

    Fluoropolymers are a group of fluorinated polymers within the broad class of substances known as per- and polyfluoroalkyl substances (PFASs). During their production, a wide array of additional fluorinated organic substances (many PFASs and some not defined as PFASs) are used, formed and emitted to air and water. This study aims to assess, and make an inventory of, all emissions of PFASs and other fluorinated organic substances by the fluoropolymer production industry in Europe using available emission databases and permits. Air emissions of the fluorinated gases (i.e., chlorofluorocarbons, hydrofluorocarbons, hydrochlorofluorocarbons and perfluorocarbons (CFCs, H(C)FCs and PFCs)) by this industry have reportedly decreased between 2007 and 2021 from roughly 500 to 150 tonnes per year. Emissions of fluorosurfactants to air and water have also been reduced significantly. However, large uncertainties remain regarding the emissions of substances that are neither fluorinated gases nor fluorosurfactants but are classified as PFASs, such as polymerization by-products, chain transfer agents and fluorinated solvents. The available data indicate that the release of these substances is not decreasing but remains relatively stable. As this inventory probably underestimates emissions, further research, improved data availability and more harmonized reporting of emissions are necessary to obtain more accurate emission data for these substances. Nevertheless, based on the available data, it is clear that the emissions from fluoropolymer production plants to air and water are still significant and that the production of fluoropolymers continues to introduce persistent substances to the environment. This study assesses the environmental impact of the fluoropolymer industry in Europe by making an inventory of their emissions of PFASs and other fluorinated organic substances.

  • 36. Fang, Shuhong
    et al.
    Li, Cheng
    Zhu, Lingyan
    Yin, Hongling
    Yang, Yingchun
    Ye, Zhixiang
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Spatiotemporal distribution and isomer profiles of perfluoroalkyl acids in airborne particulate matter in Chengdu City, China2019In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 689, p. 1235-1243Article in journal (Refereed)
    Abstract [en]

    Airborne particulate matter (APM) was collected in four seasons at five different areas of the city of Chengdu, China to study the spatial and seasonal contamination pattern of perfluoroalkyl acids (PFAAs). The results showed that Sigma PFAA concentrations in Downtown Chengdu (mean value: 297 +/- 238 pg/m(3)) were higher than concentrations in suburban areas. The highest concentrations of PFAAs occurred during spring (97.5-709 pg/L; arithmetic mean concentration: 297 +/- 191 pg/L) while the lowest concentration occurred during autumn (9.27-105 pg/L; arithmetic mean concentration 41.1 +/- 24.8 pg/L). Perfluorooctanoic acid (PFOA) was the main PFAA quantified during winter, summer and autumn, and perfluorononanoic acid (PFNA) was the predominant PFAA in spring. Relative humidity (RH) and average daily precipitation (PRE) showed significant negative correlations with PFAA concentrations in winter and summer, suggesting that they played an important role in controlling PFAA concentrations in APM. The linear structural isomer of PFOA (n-PFOA) was the most abundant isomer in APM in Chengdu, with the average proportion of 85.6% +/- 6.13%, higher than the proportion in ECF PFOA commercial products (74.3-77.6%). However, the consistent fingerprint of branched PFOA in the APM implies that ECF PFOA makes a significant contribution to the PFOA in APM. PEELS in the APM collected throughout the year had a mean proportion of 54.0 +/- 8.81% of n-PFOS. This proportion of n-PFOS is lower than commercial ECF products (62.9-78.2%), suggesting an additional proportion of branched PFOS isomers in APM in Chengdu.

  • 37. Fang, Shuhong
    et al.
    Plassmann, Merle M.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Levels of per- and polyfluoroalkyl substances (PFAS) in ski wax products on the market in 2019 indicate no changes in formulation2020In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 22, no 11, p. 2142-2146Article in journal (Refereed)
    Abstract [en]

    In the summer of 2019, eleven of the best-selling fluorinated ski wax products were purchased from one of Norway's largest sports stores and soon after analysed for a suite of 26 per- and polyfluoroalkyl substances (PFAS). The waxes were shown to contain a wide range of perfluoroalkyl acids, including perfluoroalkyl carboxylic acids with up to 25 carbons. Of particular concern was the finding that perfluorooctanoic acid (PFOA) levels in nine of the eleven ski lubrication products analysed were above the EU limit values of 25 ng g(-1), which came into force on 4(th) July 2020. The ski wax with the highest PFOA levels had a concentration that was 1215 times higher than the EU restrictions. Although some of the ski wax manufacturers have indicated that they have switched to formulations that contain chemistries based on shorter perfluoroalkyl chains, the analytical results show that this is not the case.

  • 38.
    Fang, Shuhong
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. Chengdu University of Information Technology, China.
    Sha, Bo
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Yin, Hongling
    Bian, Yuxia
    Yuan, Bo
    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.
    Environment occurrence of perfluoroalkyl acids and associated human health risks near a major fluorochemical manufacturing park in southwest of China2020In: Journal of Hazardous Materials, ISSN 0304-3894, E-ISSN 1873-3336, Vol. 396, article id 122617Article in journal (Refereed)
    Abstract [en]

    Despite China being the largest global manufacturer of perfluoroalkyl acids (PFAAs), few studies have been carried out on the environmental occurrence and associated human health risks of PFAAs emitted from manufacturing sites in China. Here, river water, tap water, soil and leaf samples were collected around a major fluorochemical manufacturing park (FMP) in the southwest of China in 2019. High EPFAA concentrations (sum of 12 PFAAs) of 3817 ng/L, 3254 ng/L, 322 - 476 ng/g dw and 23401-33749 ng/g dw were measured near the FMP in river water, tap water, soil and leaves, respectively, indicating that the FMP is a point source of PFAAs. PFOA was the predominant PFAA in all samples (58.5-98.6 %) indicating the production or use of PFOA at the FMP. PFOA concentrations in most tap water samples (> 300 ng/L in 31 of 38 samples) exceeded the U.S. EPA health advisory. Proportions of branched PFOA isomers in all samples were in 5.9-47.4 %, suggesting the production or use of PFOA manufactured by electrochemical fluorination at the FMP. It is recommended to focus more attention on branched PFOA isomers in the future because otherwise health risks may be underestimated due to their relatively high proportions in China.

  • 39.
    Figuière, Romain
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Borchert, Flora
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Ågerstrand, Marlene
    Stockholm University, Faculty of Science, Department of Environmental Science.
    The essential-use concept: a valuable tool to guide decision-making on applications for authorisation under REACH?2023In: Environmental Sciences Europe, ISSN 2190-4707, E-ISSN 2190-4715, Vol. 35, article id 5Article in journal (Refereed)
    Abstract [en]

    Background In 2020, the European Commission published the Chemical Strategy for Sustainability (CSS) in which it aims to increase the level of protection for human health and the environment from hazardous chemicals. Part of the implementation of the CSS will involve a reform of the REACH authorisation and restriction processes. One option for the reform of the authorisation process is to implement the essential-use concept as a tool to guide decision-making on applications for authorisation to make the process more efficient and to align it with societal needs. The purpose of this study is to investigate whether changes in the legal text that defines the authorisation process, and of the amount and type of information that applicants should provide in an application for authorisation, are needed to enable an implementation of the essential-use concept.

    Results The results suggest that no fundamental changes in the regulatory requirements are needed and that applicants should already provide sufficient and relevant information to the authorities to determine if the use(s) applied for is (are) essential.

    Conclusions Although the REACH authorisation already provides a legal and practical basis for an implementation of the essential-use concept, the feasibility of the essentiality assessment and its potential to make the decision-making on applications more efficient are highly dependent on the quality of the information provided and the clearness of decision criteria. However, if an applicant successfully demonstrates that the risk related to the use(s) applied for is adequately controlled, it could not be legally justified for the European Commission to refuse an authorisation by arguing that the use(s) applied for is (are) non-essential.

  • 40. Franco, A.
    et al.
    Prevedouros, Costas
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Alli, R.
    Cousins, Ian
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Comparison and analysis of different approaches for estimating the human exposure to phthalate esters2007In: Environ. Internat., Vol. 33, p. 283-291Article in journal (Refereed)
  • 41.
    Gebbink, Wouter A.
    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).
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Estimating human exposure to PFOS isomers and PFCA homologues: The relative importance of direct and indirect (precursor) exposure2015In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 74, p. 160-169Article in journal (Refereed)
    Abstract [en]

    Contributions of direct and indirect (via precursors) pathways of human exposure to perfluorooctane sulfonic acid (PFOS) isomers and perfluoroalkyl carboxylic acids (PFCAs) are estimated using a Scenario-Based Risk Assessment (SceBRA) modelling approach. Monitoring data published since 2008 (including samples from 2007) are used. The estimated daily exposures (resulting from both direct and precursor intake) for the general adult population are highest for PFOS and perfluorooctanoic acid (PFOA), followed by perfluorohexanoic add (PFHxA) and perfluorodecanoic acid (PFDA), while lower daily exposures are estimated for perfluorobutanoic acid (PFBA) and perfluorododecanoic acid (PFDoDA). The precursor contributions to the individual perfluoroalkyl acid (PFAA) daily exposures are estimated to be 11-33% for PFOS, 0.1-2.5% for PFBA, 3.7-34% for PFHxA, 13-64% for PFOA, 5.2-66% for PFDA, and 0.7-25% for PFDoDA (ranges represent estimated precursor contributions in a low- and high-exposure scenario). For PFOS, direct intake via diet is the major exposure pathway regardless of exposure scenario. For PFCAs, the dominant exposure pathway is dependent on perfluoroalkyl chain length and exposure scenario. Modelled PFOS and PFOA concentrations in human serum using the estimated intakes from an intermediate-exposure scenario are in agreement with measured concentrations in different populations. The isomer pattern of PFOS resulting from total intakes (direct and via precursors) is estimated to be enriched with linear PFOS (84%) relative to technical PFOS (70% linear). This finding appears to be contradictory to the observed enrichment of branched PFOS isomers in recent human serum monitoring studies and suggests that either external exposure is not fully understood (e.g. there are unknown precursors, missing or poorly quantified exposure pathways) and/or that there is an incomplete understanding of the isomer-specific human pharmacokinetic processes of PFOS, its precursors and intermediates.

  • 42.
    Giovanoulis, Georgios
    et al.
    Stockholm University.
    Bui, Thuy
    Stockholm University.
    Xu, Fuchao
    Papadopoulou, Eleni
    Padilla-Sanchez, Juan A.
    Covaci, Adrian
    Haug, Line S.
    Palm Cousins, Anna
    Magnér, Jörgen
    Cousins, Ian
    Stockholm University, Faculty of Science, Department of Environmental Science.
    de Wit, Cynthia A.
    Stockholm University, Faculty of Science, Department of Environmental Science.
    Corrigendum to “Multi-pathway human exposure assessment of phthalate esters and DINCH” [Environ. Int. 112 (2018) 115–126]2020In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 143, p. 106071-106071, article id 106071Article in journal (Refereed)
  • 43.
    Giovanoulis, Georgios
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Bui, Tuong Thuy
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Xu, Fuchao
    Covaci, Adrian
    Palm Cousins, Anna
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Magnér, Jörgen
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    de Wit, Cynthia A.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Multi-pathway human exposure assessment of phthalate esters and DINCHManuscript (preprint) (Other academic)
    Abstract [en]

    Phthalate esters are substances mainly used as plasticizers in various applications. Some have been restricted and phased out due to their adverse health effects and ubiquitous presence, leading to the introduction of alternative plasticizers, such as DINCH. Using a comprehensive dataset from a Norwegian study population, human exposure to DMP, DEP, DnBP, DiBP, BBzP, DEHP, DINP, DIDP, DPHP and DINCH was assessed by measuring their presence in external exposure media, allowing an estimation of the total intake, as well as the relative importance of different uptake pathways. Intake via different uptake routes, in particular inhalation, dermal absorption, and oral uptake was estimated and total intake based on all uptake pathways was compared to the back-calculated intake from biomonitoring data. Hand wipe results were used to determine dermal uptake and compared to other exposure sources such as air, dust and personal care products. Results showed that the calculated total intakes were similar, but slightly higher than those based on biomonitoring methods by 1.1 to 2.8 times (median), indicating a good understanding of important uptake pathways. The relative importance of different uptake pathways was comparable to other studies, where inhalation was important for lower molecular weight phthalates, and negligible for the higher molecular weight phthalates and DINCH. Dietary intake was the predominant exposure route for all analyzed substances. The dermal uptake assessed by hand wipes was much lower (median up to 2000 times) than the sum of dermal uptake via air, dust and personal care products and unlikely represents an integrative dermal exposure. Dermal uptake is not a well-studied exposure pathway and several research gaps (e.g. absorption fractions) remain. Based on calculated intakes, the exposure risk for the Norwegian participants to the phthalates and DINCH was lower than health based limit values. Nevertheless, exposure to alternative plasticizers, such as DPHP and DINCH, is expected to increase in the future and continuous monitoring is required.

  • 44.
    Giovanoulis, Georgios
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. IVL Swedish Environmental Research Institute, Sweden.
    Xu, Fuchao
    Papadopoulou, Eleni
    Padilla-Sanchez, Juan A.
    Covaci, Adrian
    Haug, Line S.
    Palm Cousins, Anna
    Magnér, Jörgen
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    de Wit, Cynthia A.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Multi-pathway human exposure assessment of phthalate esters and DINCH2018In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 112, p. 115-126Article in journal (Refereed)
    Abstract [en]

    Phthalate esters are substances mainly used as plasticizers in various applications. Some have been restricted and phased out due to their adverse health effects and ubiquitous presence, leading to the introduction of alternative plasticizers, such as DINCH. Using a comprehensive dataset from a Norwegian study population, human exposure to DMP, DEP, DnBP, DiBP, BBzP, DEHP, DINP, DIDP, DPHP and DINCH was assessed by measuring their presence in external exposure media, allowing an estimation of the total intake, as well as the relative importance of different uptake pathways. Intake via different uptake routes, in particular inhalation, dermal absorption, and oral uptake was estimated and total intake based on all uptake pathways was compared to the calculated intake from biomonitoring data. Hand wipe results were used to determine dermal uptake and compared to other exposure sources such as air, dust and personal care products. Results showed that the calculated total intakes were similar, but slightly higher than those based on biomonitoring methods by 1.1 to 3 times (median), indicating a good understanding of important uptake pathways. The relative importance of different uptake pathways was comparable to other studies, where inhalation was important for lower molecular weight phthalates, and negligible for the higher molecular weight phthalates and DINCH. Dietary intake was the predominant exposure route for all analyzed substances. Dermal uptake based on hand wipes was much lower (median up to 2000 times) than the total dermal uptake via air, dust and personal care products. Still, dermal uptake is not a well-studied exposure pathway and several research gaps (e.g. absorption fractions) remain. Based on calculated intakes, the exposure for the Norwegian participants to the phthalates and DINCH was lower than health based limit values. Nevertheless, exposure to alternative plasticizers, such as DPHP and DINCH, is expected to increase in the future and continuous monitoring is required.

  • 45. Glüge, Juliane
    et al.
    London, Rachel
    Cousins, Ian
    Stockholm University, Faculty of Science, Department of Environmental Science.
    DeWitt, Jamie
    Goldenman, Gretta
    Herzke, Dorte
    Lohmann, Rainer
    Miller, Mark
    Ng, Carla A.
    Patton, Sharyle
    Trier, Xenia
    Wang, Zhanyun
    Scheringer, Martin
    Information Requirements under the Essential-Use Concept: PFA Case Studies br2022In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 56, no 10, p. 6232-6242Article in journal (Refereed)
    Abstract [en]

    Per- and polyfluoroalkyl substances (PFAS) are a class of substances for which there are widespread concerns about their extreme persistence in combination with toxic effects. It has been argued that PFAS should only be employed in those uses that are necessary for health or safety or are critical for the functioning of society and where no alternatives are available (“essential-use concept”). Implementing the essential-use concept requires a sufficient understanding of the current uses of PFAS and of the availability, suitability, and hazardous properties of alternatives. To illustrate the information requirements under the essential-use concept, we investigate seven different PFAS uses, three in consumer products and four industrial applications. We investigate how much information is available on the types and functions of PFAS in these uses, how much information is available on alternatives, their performance and hazardous properties and, finally, whether this information is sufficient as a basis for deciding on the essentiality of a PFAS use. The results show (i) the uses of PFAS are highly diverse and information on alternatives is often limited or lacking; (ii) PFAS in consumer products often are relatively easy to replace; (iii) PFAS uses in industrial processes can be highly complex and a thorough evaluation of the technical function of each PFAS and of the suitability of alternatives is needed; (iv) more coordination among PFAS manufacturers, manufacturers of alternatives to PFAS, users of these materials, government authorities, and other stakeholders is needed to make the process of phasing out PFAS more transparent and coherent.

  • 46. Glüge, Juliane
    et al.
    Scheringer, Martin
    Cousins, Ian
    Stockholm University, Faculty of Science, Department of Environmental Science.
    DeWitt, Jamie C.
    Goldenman, Gretta
    Herzke, Dorte
    Lohmann, Rainer
    Ng, Carla A.
    Trier, Xenia
    Wang, Zhanyun
    An overview of the uses of per- and polyfluoroalkyl substances (PFAS)2020In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 22, no 12, p. 2345-2373Article in journal (Refereed)
    Abstract [en]

    Per- and polyfluoroalkyl substances (PFAS) are of concern because of their high persistence (or that of their degradation products) and their impacts on human and environmental health that are known or can be deduced from some well-studied PFAS. Currently, many different PFAS (on the order of several thousands) are used in a wide range of applications, and there is no comprehensive source of information on the many individual substances and their functions in different applications. Here we provide a broad overview of many use categories where PFAS have been employed and for which function; we also specify which PFAS have been used and discuss the magnitude of the uses. Despite being non-exhaustive, our study clearly demonstrates that PFAS are used in almost all industry branches and many consumer products. In total, more than 200 use categories and subcategories are identified for more than 1400 individual PFAS. In addition to well-known categories such as textile impregnation, fire-fighting foam, and electroplating, the identified use categories also include many categories not described in the scientific literature, including PFAS in ammunition, climbing ropes, guitar strings, artificial turf, and soil remediation. We further discuss several use categories that may be prioritised for finding PFAS-free alternatives. Besides the detailed description of use categories, the present study also provides a list of the identified PFAS per use category, including their exact masses for future analytical studies aiming to identify additional PFAS.

  • 47.
    Gomis Ferreira, Melissa I.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Vestergren, Robin
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Nilsson, Helena
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Contribution of Direct and Indirect Exposure to Human Serum Concentrations of Perfluorooctanoic Acid in an Occupationally Exposed Group of Ski Waxers2016In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 50, no 13, p. 7037-7046Article in journal (Refereed)
    Abstract [en]

    The contribution of direct (i.e., uptake of perfluorooctanoic acid (PFOA) itself) and indirect (i.e., uptake of 8:2 fluorotelomer alcohol (FTOH) and metabolism to PFOA) exposure to PFOA serum concentrations was investigated using a dynamic one compartment pharmacokinetic (PK) model. The PK model was applied to six occupationally exposed ski waxers for whom direct and indirect exposures via inhalation were characterized using multiple measurements with personal air sampling devices. The model was able to predict the diverging individual temporal trends of PFOA in serum with correlation coefficients of 0.82-0.94. For the four technicians with high initial concentrations of PFOA in serum (250-1050 ng/mL), the ongoing occupational exposure (both direct and indirect) was of minor importance and net depuration of PFOA was observed throughout the ski season. An estimated average intrinsic elimination half-life of 2.4 years (1.8-3.1 years accounting for variation between technicians and model uncertainty) was derived for these technicians. The remaining two technicians, who had much lower initial serum concentrations (10-17 ng/mL), were strongly influenced by exposure during the ski season with indirect exposure contributing to 45% of PFOA serum concentrations. On the basis of these model simulations, an average metabolism yield of 0.003 (molar concentration basis; uncertainty range of 0.0006-0.01) was derived for transformation of 8:2 FTOH to PFOA. An uncertainty analysis was performed, and it was determined that the input parameters quantifying the intake of PFOA were mainly responsible for the uncertainty of the metabolism yield and the initial concentration of PFOA in serum was mainly contributing to the uncertainty of estimated serum half-lives.

  • 48.
    Gomis Ferreira, Melissa Ines
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Vestergren, Robin
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. IVL Swedish Environmental Research Institute, Sweden.
    Borg, Daniel
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Comparing the toxic potency in vivo of long-chain perfluoroalkyl acids and fluorinated alternatives2018In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 113, p. 1-9Article in journal (Refereed)
    Abstract [en]

    Since 2000, long-chain perfluoroalkyl acids (PFAAs) and their respective precursors have been replaced by numerous fluorinated alternatives. The main rationale for this industrial transition was that these alternatives were considered less bioaccumulative and toxic than their predecessors. In this study, we evaluated to what extent differences in toxicological effect thresholds for PFAAs and fluorinated alternatives, expressed as administered dose, were confounded by differences in their distribution and elimination kinetics. A dynamic one-compartment toxicokinetic (TK) model for male rats was constructed and evaluated using test data from toxicity studies for perfluorobutanoic acid (PFBA), perfluorohexanoic acid (PFHxA), perfluorobutane sulfonic acid (PFBS), perfluorooctanoic acid (PFOA), perfluoroctanesulfonic acid (PFOS) and ammonium 2,3,3,3-tetrafluoro-2-(heptafluoropropoxy)-propanoate (GenX). Dose-response curves of liver enlargement from sub-chronic oral toxicity studies in male rats were converted to internal dose in serum and in liver to examine the toxicity ranking of PFAAs and fluorinated alternatives. Converting administered doses into equivalent serum and liver concentrations reduced the variability in the dose-response curves for PFBA, PFHxA, PFOA and GenX. The toxicity ranking using modeled serum (GenX>PFOA>PFHxA>PFBA) and liver (GenX>PFOA≈PFHxA≈PFBA) concentrations indicated that some fluorinated alternatives have similar or higher toxic potency than their predecessors when correcting for differences in toxicokinetics. For PFOS and perfluorobutane sulfonic acid (PFBS) the conversion from administered dose to serum concentration equivalents did not change the toxicity ranking. In conclusion, hazard assessment based on internal exposure allows evaluation of toxic potency and bioaccumulation potential independent of kinetics and should be considered when comparing fluorinated alternatives with their predecessors.

  • 49.
    Gomis, Melissa I.
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Vestergren, Robin
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry. IVL Swedish Environmental Research Institute, Sweden.
    MacLeod, Matthew
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Mueller, Jochen F.
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Historical human exposure to perfluoroalkyl acids in the United States and Australia reconstructed from biomonitoring data using population-based pharmacokinetic modelling2017In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 108, p. 92-102Article in journal (Refereed)
    Abstract [en]

    Perfluorooctanoic acid (PFOA), perfluorooctanesulfonic acid (PFOS) and perfluorohexanesulfonic acid (PFHxS) are found in the blood of humans and wildlife worldwide. Since the beginning of the 21st century, a downward trend in the human body burden, especially for PFOS and PFOA, has been observed while there is no clear temporal trend in wildlife. The inconsistency between the concentration decline in human serum and in wildlife could be indicative of a historical exposure pathway for humans linked to consumer products that has been reduced or eliminated. In this study, we reconstruct the past human exposure trends in two different regions, USA and Australia, by inferring the historical intake from cross-sectional biomonitoring data of PFOS, PFOA and PFHxS using a population-based pharmacokinetic model. For PFOS in the USA, the reconstructed daily intake peaked at 4.5 ng/kg-bw/day between 1988 and 1999 while in Australia it peaked at 4.0 ng/kg-bw/day between 1984 and 1996. For PFOA in the USA and Australia, the peak reconstructed daily intake was 1.1 ng/kg-bw/day in 1995 and 3.6 ng/kg-bw/day in 1992, respectively, and started to decline in 2000 and 1995, respectively. The model could not be satisfactorily fitted to the biomonitoring data for PFHxS within reasonable boundaries for its intrinsic elimination half-life, and thus reconstructing intakes of PFHxS was not possible. Our results indicate that humans experienced similar exposure levels and trends to PFOS and PFOA in the USA and Australia. Our findings support the hypothesis that near-field consumer product exposure pathways were likely dominant prior to the phase-out in industrialized countries. The intrinsic elimination half-life, which represents elimination processes that are common for all humans, and elimination processes unique to women (i.e., menstruation, cord-blood transfer and breastfeeding) were also investigated. The intrinsic elimination half-lives for PFOS and PFOA derived from model fitting for men were 3.8 and 2.4 years, respectively, for the USA, and 4.9 and 2 years respectively for Australia. Our results show that menstruation is a depuration pathway for PFOA for women, similarly but to a lesser extent compared to previous reports for PFOS. However menstruation, cord-blood transfer and breastfeeding together do not fully explain the apparently more rapid elimination of PFOA and PFOS by women compared to men; the intrinsic elimination half-lives in women were up to 13% lower for PFOS and up to 12% lower for PFOA compared to the corresponding half-lives in men.

  • 50.
    Gomis, Melissa Ines
    et al.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    Wang, Zhanyun
    Scheringer, Martin
    Cousins, Ian T.
    Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
    A modeling assessment of the physicochemical properties and environmental fate of emerging and novel per- and polyfluoroalkyl substances2015In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 505, p. 981-991Article in journal (Refereed)
    Abstract [en]

    Long-chain perfluoroalkyl carboxylic acids (PFCAs) and perfluoroalkane sulfonic acids (PFSAs) are persistent, bioaccumulative, and toxic contaminants that are globally present in the environment, wildlife and humans. Phase-out actions and use restrictions to reduce the environmental release of long-chain PFCAs, PFSAs and their precursors have been taken since 2000. In particular, long-chain poly- and perfluoroalkyl substances (PFASs) are being replaced with shorter-chain homologues or other fluorinated or non-fluorinated alternatives. A key question is: are these alternatives, particularly the structurally similar fluorinated alternatives, less hazardous to humans and the environment than the substances they replace? Several fluorinated alternatives including perfluoroether carboxylic acids (PFECAs) and perfluoroether sulfonic adds (PFESAs) have beet recently identified. However, the scarcity of experimental data prevents hazard and risk assessments for these substances. In this study, we use state-of-the-art in silico tools to estimate key properties of these newly identified fluorinated alternatives. [i] COSMOtherm and SPARC ate used to estimate physicochemical properties. The US EPA EPISuite software package is used to predict degradation half-lives in air, water and soil. [ii] In combination with estimated chemical properties, a fugacity-based multimedia mass-balance unit-world model the OECD Overall Persistence (Pov) and Long-Range Transport Potential (LRTP) Screening Tool is used to assess the likely environmental fate of these alternatives. Even though the fluorinated alternatives contain some structural differences, their physicochemical properties are not significantly different from those of their predecessors. Furthermore, most of the alternatives are estimated to be similarly persistent and mobile in the environment as the long-chain PFASs. The models therefore predict that the fluorinated alternatives will become globally distributed in the environment similar to their predecessors. Although such in silico methods are coupled with uncertainties, this preliminary assessment provides enough cause for concern to warrant experimental work to better determine the properties of these fluorinated alternatives.

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