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Comparative Assessment of the Global Fate and Transport Pathways of Long-chain Perfluorocarboxylic Acids (PFCAs) and Perfluorocarboxylates (PFCs) Emitted from Direct Sources
Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
2009 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 43, no 15, 5830-5836 p.Article in journal (Refereed) Published
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.

Place, publisher, year, edition, pages
American Chemical Society , 2009. Vol. 43, no 15, 5830-5836 p.
National Category
Natural Sciences Earth and Related Environmental Sciences
URN: urn:nbn:se:su:diva-25784DOI: 10.1021/es900753yOAI: diva2:200512
Part of urn:nbn:se:su:diva-8571Available from: 2009-03-05 Created: 2009-02-19 Last updated: 2011-03-18Bibliographically approved
In thesis
1. Modeling the global fate and transport of perfluoroalkylated substances (PFAS)
Open this publication in new window or tab >>Modeling the global fate and transport of perfluoroalkylated substances (PFAS)
2009 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Perfluoroalkylated substances (PFAS) are persistent contaminants that are widely distributed in the global environment. Despite the fact that these chemicals have been manufactured and used for over 50 years, there has been little scientific and regulatory interest until very recently. An important research priority over the past decade has been to gain a better understanding of the mechanisms and pathways explaining the presence of these compounds in remote regions. One explanation is related to the use and release of volatile precursor compounds which undergo atmospheric transport and are also susceptible to degradation to PFAS through gas phase reactions with radical species. The main purpose of this doctoral thesis was to investigate an alternative explanation, namely the long-range transport (LRT) of PFAS themselves, which have been released into the environment in substantial quantities during manufacturing and product use. Papers I – III explore the LRT potential of perfluorocarboxylic acids and perfluorocarboxylates and demonstrate that both oceanic and atmospheric transport are efficient pathways of dispersion from source to remote regions of the Northern Hemisphere. Oceanic transport of perfluorooctane sulfonate (PFOS) was shown to be an important process in Paper IV as well. The role of precursor transport and degradation to PFOS was also examined in this paper. The most interesting aspect of the fate and transport of PFOS precursors is the rapid response in ambient concentrations exhibited by these compounds in the model simulations following production phase-out. Since precursor compounds are known to degrade to PFOS in vivo, the modeling results demonstrate that this exposure pathway is a plausible explanation for the declining trends in PFOS concentrations reported for marine mammals in some remote environments.

Place, publisher, year, edition, pages
Stockholm: Institutionen för tillämpad miljövetenskap (ITM), 2009. 32 p.
perfluoroalkylated substances, global-scale, fate and transport
National Category
Environmental Sciences
Research subject
Applied Environmental Science
urn:nbn:se:su:diva-8571 (URN)978-91-7155-812-1 (ISBN)
Public defence
2009-03-27, Nordenskiöldsalen, Geovetenskapens hus, Svante Arrhenius väg 8 C, Stockholm, 10:00
Available from: 2009-03-05 Created: 2009-02-19Bibliographically approved

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Armitage, James MMacleod, MatthewCousins, Ian T
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