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Contribution of polyfluoroalkyl phosphate esters (PAPs) and other precursor compounds to perfluoroalkyl carboxylates (PFCAs) in humans and the environment
Örebro University, School of Science and Technology, Örebro University, Sweden.
2016 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Per-and polyfluoroalkyl substances (PFAS) are anthropogenic compounds that have been spread all over the world. The use of fluorotelomer compounds, short-chained homologues, and other PFASs with perfluorinated moieties has emerged recent years. One of these emerging compound classes is polyfluoroalkyl phosphate esters (PAPs), which have the ability to degrade into persistent PFCAs.

The aim of this thesis was to assess the contribution of PAPs and other precursors to the exposure of PFCAs to humans and the environment. The main objective was to analyze a wide range of PFAS in human serum, wild bird eggs, indoor dust, waste water, and sludge. There was a significant contribution from selected precursors to the total amount of PFASs in the abiotic compartments indoor dust, waste water, and sludge. Levels of PAPs found in house dust exceeded those of PFCAs and perfluorosulfonic acids (PFSAs), revealing PAPs as a world-wide important exposure source.

A net increase was during waste water treatment was observed for several PFASs in Swedish waste water treatment plants. Together with presence of precursor compounds and intermediates in the influent water and the sludge, this suggest that degradation of PFCA precursors contributed to the increase of PFCAs. Detection of precursors in human serum, together with slow declining trends of PFCAs, revealed an ongoing exposure of PFCAs to the general population of Australia. The diPAPs and the FTSAs were also detected in raptor bird eggs from Sweden from both the terrestrial and the freshwater environment. The precursors concentrations and patterns observed reveal that current regulatory measures are insufficient for the purpose of protecting humans and the environment from PFASs exposure.

Place, publisher, year, edition, pages
Örebro: Örebro university , 2016. , 100 p.
Series
Örebro Studies in Chemistry, ISSN 1651-4270 ; 18
Keyword [en]
PAPs, precursors, PFCA, exposure, indoor dust, human serum, WWTP, bird eggs
National Category
Other Chemistry Topics
Research subject
Chemistry
Identifiers
URN: urn:nbn:se:oru:diva-52010ISBN: 978-91-7529-164-2 (print)OAI: oai:DiVA.org:oru-52010DiVA: diva2:958301
Public defence
2016-11-04, Örebro universitet, Långhuset, Hörsal 3, Fakultetsgatan 1, Örebro, 10:15 (Swedish)
Opponent
Supervisors
Available from: 2016-09-06 Created: 2016-09-06 Last updated: 2016-12-14Bibliographically approved
List of papers
1. World-Wide Indoor Exposure to Polyfluoroalkyl Phosphate Esters (PAPs) and other PFASs in Household Dust
Open this publication in new window or tab >>World-Wide Indoor Exposure to Polyfluoroalkyl Phosphate Esters (PAPs) and other PFASs in Household Dust
2015 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 49, no 24, 14503-14511 p.Article in journal (Refereed) Published
Abstract [en]

Human exposure to perfluorooctanoic acid (PFOA) and other per- and polyfluoroalkyl substances (PFASs) is ongoing and in some cases increasing, despite efforts made to reduce emissions. The role of precursor compounds such as polyfluorinated phosphate esters (PAPs) has received increasing attention, but there are knowledge gaps regarding their occurrence and impact on human exposure. In this study, mono-, di-, and triPAPs, perfluorinated alkyl acids (PFAAs), saturated, and unsaturated fluorotelomer carboxylic acids (FTCA/FTUCAs), perfluoroalkane sulfonamides, and sulfonamidethanols (FOSA/FOSEs), and one fluorotelomer sulfonic acid (FTSA)) were compared in household dust samples from Canada, the Faroe Islands, Sweden, Greece, Spain, Nepal, Japan, and Australia. Mono-, di-, and triPAPs, including several diPAP homologues, were frequently detected in dust from all countries, revealing an ubiquitous spread in private households from diverse geographic areas, with significant differences between countries. The median levels of monoPAPs and diPAPs ranged from 3.7 ng/g to 1 023 ng/g and 3.6 ng/g to 692 ng/g, respectively, with the lowest levels found in Nepal and the highest in Japan. The levels of PAPs exceeded those of the other PFAS classes. These findings reveal the importance of PAPs as a source of PFAS exposure worldwide.

Place, publisher, year, edition, pages
Washington, USA: American Chemical Society (ACS), 2015
National Category
Chemical Sciences Environmental Sciences
Research subject
Enviromental Science
Identifiers
urn:nbn:se:oru:diva-46467 (URN)10.1021/acs.est.5b00679 (DOI)000366872300072 ()26000882 (PubMedID)2-s2.0-84934903181 (Scopus ID)
Available from: 2015-11-12 Created: 2015-11-12 Last updated: 2016-10-14Bibliographically approved
2. Temporal trends of PFSAs, PFCAs and selected precursors in Australian serum from 2002 to 2013
Open this publication in new window or tab >>Temporal trends of PFSAs, PFCAs and selected precursors in Australian serum from 2002 to 2013
Show others...
(English)Manuscript (preprint) (Other academic)
National Category
Other Chemistry Topics
Research subject
Chemistry
Identifiers
urn:nbn:se:oru:diva-52953 (URN)
Available from: 2016-10-14 Created: 2016-10-14 Last updated: 2016-10-14Bibliographically approved
3. Contribution of precursor compounds to the release of per- and polyfluoroalkyl substances (PFASs) from waste water treatment plants (WWTPs)
Open this publication in new window or tab >>Contribution of precursor compounds to the release of per- and polyfluoroalkyl substances (PFASs) from waste water treatment plants (WWTPs)
(English)Manuscript (preprint) (Other academic)
National Category
Other Chemistry Topics
Research subject
Chemistry
Identifiers
urn:nbn:se:oru:diva-52964 (URN)
Available from: 2016-10-14 Created: 2016-10-14 Last updated: 2016-10-14Bibliographically approved
4. Comparison of PFASs contamination in the freshwater and terrestrial environments by analysis of eggs from osprey (Pandion haliaetus), tawny owl (Strix aluco), and common kestrel (Falco tinnunculus)
Open this publication in new window or tab >>Comparison of PFASs contamination in the freshwater and terrestrial environments by analysis of eggs from osprey (Pandion haliaetus), tawny owl (Strix aluco), and common kestrel (Falco tinnunculus)
Show others...
2016 (English)In: Environmental Research, ISSN 0013-9351, E-ISSN 1096-0953, Vol. 149, 40-47 p.Article in journal (Refereed) Published
Abstract [en]

The level of PFAS (per- and polyfluorinated alkyl substances) contamination in freshwater and terrestrial Swedish environments in 2013/2014 was assessed by analyzing a range of perfluorinated alkyl acids, fluorotelomer acids, sulfonamides, sulfonamidoethanols and polyfluoralkyl phosphate diesters (diPAPs) in predator bird eggs. Stable isotopes ((13)C and (15)N) were analyzed to elucidate the dietary source. The tawny owl (Strix aluco, n=10) and common kestrel (Falco tinnunculus, n=40), two terrestrial species, and the osprey (Pandion haliaetus, n=30), a freshwater specie were included. In addition, a temporal trend (1997-2001, 2008-2009, 2013) in osprey was studied as well. The PFAS profile was dominated by perfluorooctane sulfonic acid (PFOS) in eggs from osprey and tawny owl, while for common kestrel perfluorinated carboxylic acids (∑PFCA) exceeded the level of PFOS. PFOS concentration in osprey eggs remained at the same level between 1997 and 2001 and 2013. For the long-chained PFCAs, there were a significant increase in concentrations in osprey eggs between 1997 and 2001 and 2008-2009. The levels of PFOS and PFCAs were about 10 and five times higher, respectively, in osprey compared to tawny owl and common kestrel. Evidence of direct exposure from PFCA precursor compounds to birds in both freshwater and terrestrial environment was observed. Low levels of diPAPs were detected in a few samples of osprey (<0.02-2.4ng/g) and common kestrel (<0.02-0.16ng/g) eggs, and 6:2 FTSA was detected in a majority of the osprey eggs (<6.3-52ng/g). One saturated telomer acid (7:3 FTCA), which is a transformation marker from precursor exposure, was detected in all species (<0.24-2.7ng/g). The (15)N data showed higher levels in osprey eggs compared to tawny owl and common kestrel, indicating that they feed on a 2-3 times higher trophic level. We conclude that ospreys are continuously exposed to PFAS at levels where adverse toxic effects have been observed in birds.

Place, publisher, year, edition, pages
San Diego, USA: Academic Press, 2016
Keyword
diPAPs, PFAS, Bird of prey, Freshwater, Terrestrial
National Category
Environmental Sciences
Research subject
Enviromental Science
Identifiers
urn:nbn:se:oru:diva-50315 (URN)10.1016/j.envres.2016.04.038 (DOI)000378366000006 ()27174782 (PubMedID)2-s2.0-84965046283 (Scopus ID)
Note

Funding Agency:

Swedish Environmental Protection Agency (SEPA)  2220-14-004

Available from: 2016-05-27 Created: 2016-05-16 Last updated: 2016-10-14Bibliographically approved

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