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Temporal trends of perfluoroalkane sulfonic acids and their sulfonamide-based precursors in herring from the Swedish west coast 1991–2011 including isomer-specific considerations
Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
(English)Manuscript (preprint) (Other academic)
Abstract [en]

A method was developed for simultaneous analysis of perfluoroalkane sulfonic acids (PFSAs) and their sulfonamide-based precursors (perfluoroalkane sulfonamidoacetic acids (FASAAs), sulfonamides (FASAs), and sulfonamidoethanols (FASEs)) in fish muscle. Extraction was performed with acetonitrile followed by a clean-up and fractionation step and instrumental analysis by UPLC/MS/MS and GC/MS. Time trends of PFSAs and their precursors in herring muscle samples originating from the Kattegat at the west coast of Sweden were investigated covering the years 1991-2011. PFSAs, FOSA and alkyl-FOSAAs were detected at pg/g levels, all with decreasing or unchanged trends between 1991 and 2011. The highest concentrations were found for PFOS and FOSA around the turn of the century. Shorter disappearance half-lives were observed for precursors compared to PFSAs. Assuming that these trend differences are representative for fish consumed by the general Swedish population, this observation suggests that the relative contribution of precursors to total human exposure to PFOS via fish intake has decreased in Sweden over the study period. PFOS precursors in fish may have constituted a significant indirect exposure pathway for PFOS in the 1990s. Isomer-specific analysis of PFOS and FOSA revealed diverging patterns and temporal trends from what is commonly found in human serum. In combination with literature data on isomer patterns in other edible fish species and on isomer-specific human toxicokinetics, our results suggest that fish consumption alone cannot account for the PFOS isomer patterns and trends observed in humans.

Keyword [en]
Temporal trends, herring muscle, PFOS, perfluorooctane sulfonamides, precursor, human exposure
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
URN: urn:nbn:se:su:diva-93742OAI: oai:DiVA.org:su-93742DiVA: diva2:648351
Available from: 2013-09-15 Created: 2013-09-15 Last updated: 2013-09-16Bibliographically approved
In thesis
1. Improved analytical methods for perfluoroalkyl acids (PFAAs) and their precursors – a focus on human dietary exposure
Open this publication in new window or tab >>Improved analytical methods for perfluoroalkyl acids (PFAAs) and their precursors – a focus on human dietary exposure
2013 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Per- and polyfluoroalkyl substances are a large group of global environmental contaminants. They can be divided into two sub-groups, 1) perfluoroalkyl acids (PFAAs) and 2) so called precursors, i.e. compounds that can potentially be transformed to form PFAAs. PFAAs are today ubiquitous in wildlife and humans. Food and drinking water are assumed to be the dominant human exposure pathways for PFAAs.

The main aim of this doctoral thesis was to develop highly sensitive and fully validated analytical methods for the determination of a range of PFAAs and selected precursors in dietary samples. The methods were based on liquid chromatography coupled to mass spectrometry. Samples were extracted by solvent extraction followed by a cleanup step employing solid phase extraction. The cleanup step could at the same time be used as a fractionation of ionic PFAAs and neutral precursors.

Paper I and II describe the development of methods for simultaneous analysis of three groups of PFAAs including perfluoroalkyl phosphonic acids (PFPAs) in drinking water and food. Methyl piperidine was used as ion pairing agent, leading to highly sensitive analysis of PFPAs. A first screening of tap water samples and different food items revealed that human dietary exposure to PFPAs in Europe is currently not of concern.

A novel method for simultaneous analysis of perfluoroalkyl carboxylic acids (PFCAs) and polyfluoroalkyl phosphate esters (PAPs) in food and packaging materials is described in paper III. Targeted food samples and their packaging were analyzed. The results showed that PAPs may contribute to human exposure to PFCAs. In paper IV temporal trends (1991-2011) of perfluorooctane sulfonic acid (PFOS) and its precursors in herring were investigated. Rapidly decreasing trends were found for precursors, whereas PFOS did not show a significant change over time. Precursors in fish may have played an important role for human exposure to PFOS in the 1990s but are probably negligible today.

Place, publisher, year, edition, pages
Stockholm: Department of Applied Environmental Science (ITM), Stockholm University, 2013. 47 p.
Keyword
Environmental Science, PFASs, PFAAs, PFOA, PFOS, Precursor, FOSA, PAPs, Method development, LC-MS, SPE, Dietary sample, Drinking water, Human exposure
National Category
Environmental Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-93719 (URN)978-91-7447-753-5 (ISBN)
Public defence
2013-10-25, Nordenskiöldsalen, Geovetenskapens hus, Svante Arrhenius väg 12, Stockholm, 10:00 (English)
Opponent
Supervisors
Projects
PERFOOD project (KBBE-227525)
Funder
EU, FP7, Seventh Framework Programme, KBBE-227525
Note

At the time of the doctoral defense, the following paper was unpublished and had a status as follows: Paper 4: Manuscript.

Available from: 2013-10-03 Created: 2013-09-13 Last updated: 2014-01-31Bibliographically approved

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