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Environmental occurrence and fate of semifluorinated n-alkanes and perfluorinated alkyl acids present in ski waxes
Stockholm University, Faculty of Science, Department of Applied Environmental Science (ITM).
2011 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Highly fluorinated organic compounds are emerging environmental contaminants of concern, due to their persistence, ubiquitous distribution, bioaccumulation potential and toxicity. Ski waxes are sources of highly fluorinated chemicals to the environment that have not been investigated so far. Some contain fluorinated additives such as semifluorinated n-alkanes (SFAs). This thesis investigated the fate of SFAs after abrasion onto snow through skiing activities. Furthermore, perfluorinated alkyl acids (PFAAs) were found to be present in fluorinated ski waxes. A lot of attention has been paid to elucidating the environmental fate of PFAAs during the past decade. However, nothing was known so far about their release from melting snow packs.

Analytical methods for quantification of SFAs in different environmental matrices were developed. The methods were used to investigate the fate of SFAs during snow melt and to study their occurrence in ski areas. Laboratory snow melt experiments and model-based fate simulations suggested that SFAs will sorb to the snow grain surface and particles in the bulk snow and, after snowmelt, will end up on the underlying (soil) surface. SFAs were detected and quantified for the first time in snow and soil samples taken from a ski area in Sweden. Comparison of concentrations in snow and soil did not give any evidence for long-term accumulation of SFAs in surface soil, but suggested volatilization of shorter chain homologues during snow melt. Such a volatilization could also explain an observed SFA pattern difference between snow and soil samples.

Laboratory scale snow melt experiments were also used to investigate the behavior of PFAAs during snowmelt. PFAAs were released with the melt water from the snow pack in pulses. The pulses occurred early, late or with a so far unknown peak elution in the middle of the snowmelt, depending on the hydrophobicity of the PFAAs. These peak releases were further influenced by the age of the snow pack and thus the snow surface area and to a lesser extent by pH and ion concentrations.

Place, publisher, year, edition, pages
Stockholm: Department of Applied Environmental Science (ITM), Stockholm University , 2011. , 35 p.
Keyword [en]
Semifluorinated n-alkanes, Perfluorinated alkyl acids, ski waxes, snow, soil, fate
National Category
Natural Sciences
Research subject
Applied Environmental Science
Identifiers
URN: urn:nbn:se:su:diva-56405ISBN: 978-91-7447-280-6OAI: oai:DiVA.org:su-56405DiVA: diva2:411051
Public defence
2011-05-27, William-Olssonsalen, Geovetenskapens hus, Svante Arrhenius väg 14, Stockholm, 10:00 (English)
Opponent
Supervisors
Available from: 2011-05-05 Created: 2011-04-15 Last updated: 2012-01-26Bibliographically approved
List of papers
1. Trace Analytical Methods for Semifluorinated n-Alkanes in Snow, Soil, and Air
Open this publication in new window or tab >>Trace Analytical Methods for Semifluorinated n-Alkanes in Snow, Soil, and Air
2010 (English)In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 82, no 11, 4551-4557 p.Article in journal (Refereed) Published
Abstract [en]

Semifluorinated n-alkanes (SFAs) are anthropogenic chemicals that are used in ski waxes and, thus, are released directly into the environment, but their subsequent fate and distribution are as yet unknown. Therefore, simple, selective, and sensitive methods were developed for analyzing trace amounts of SFAs in snow/water, soil, and air samples by gas chromatography coupled to electron capture negative ionization mass spectrometry (GC/ECNI-MS). Recoveries were generally in the range of 70-120%, depending on the compound and matrix. The analytical sensitivity was higher for SFAs with longer fluorinated chains, and the instrumental limits of detection ranged from 0.3 to 260 pg injected, providing method detection limits of 0.54-311 ng L-1, 0.004-9.86 ng g(-1), and 0.4-531 ng m(-3) for snow (analyzed as its meltwater), soil, and air samples, respectively. Using the developed procedures, SFAs were found in snow (meltwater) and soil samples from a small cross-country ski area in Sweden at concentrations up to 1.3 mu g L-1 and 47 pg g(-1), respectively.

National Category
Natural Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-49227 (URN)10.1021/ac1005519 (DOI)000278062800036 ()
Note
authorCount :2Available from: 2010-12-13 Created: 2010-12-13 Last updated: 2011-04-18Bibliographically approved
2. Theoretical and Experimental Simulation of the Fate of Semifluorinated n-Alkanes during Snowmelt
Open this publication in new window or tab >>Theoretical and Experimental Simulation of the Fate of Semifluorinated n-Alkanes during Snowmelt
Show others...
2010 (English)In: Environmental Science and Technology, ISSN 1086-931X, Vol. 44, no 17, 6692-6697 p.Article in journal (Refereed) Published
Abstract [en]

Semifluorinated n-alkanes (SFAs) are highly fluorinated anthropogenic chemicals that are released into the environment through their use in ski waxes. Nothing is known about their environmental partitioning in general and their fate during snowmelt in particular. Properties were estimated for a range of SFAs with different chain lengths and degrees of fluorination using the SPARC calculator and poly parameter linear free energy relationships (ppLFERs). The calculations resulted in very low water solubility and vapor pressures and, consequently, high log KOW and log KOA values. Artificially produced snow in a cold room was spiked with a range of SFAs and subsequently melted with infrared lamps. Melt water, particles, and air samples taken during melting were analyzed. Both calculations and experiments showed that SFAs used in ski waxes will bind to particles or snow grain surfaces during snowmelt and thus are predicted to end up on the soil surface in skiing areas.

National Category
Natural Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-56401 (URN)10.1021/es101562w (DOI)
Available from: 2011-04-15 Created: 2011-04-15 Last updated: 2011-04-18Bibliographically approved
3. Laboratory studies on the fate of perfluoroalkyl carboxylates and sulfonates during snow melt
Open this publication in new window or tab >>Laboratory studies on the fate of perfluoroalkyl carboxylates and sulfonates during snow melt
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(English)Article in journal (Refereed) Submitted
National Category
Natural Sciences
Research subject
Applied Environmental Science
Identifiers
urn:nbn:se:su:diva-56403 (URN)
Available from: 2011-04-15 Created: 2011-04-15 Last updated: 2011-04-18Bibliographically approved
4. Environmental occurrence and fate of semifluorinated n-alkanes in snow and soil samples from a ski area
Open this publication in new window or tab >>Environmental occurrence and fate of semifluorinated n-alkanes in snow and soil samples from a ski area
2011 (English)In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 85, no 9, 1458-1463 p.Article in journal (Refereed) Published
Abstract [en]

Semifluorinated n-alkanes (SFAs) with carbon chain lengths of 22 to approximately 36 atoms are present in fluorinated ski waxes to reduce the friction between ski base and snow, resulting in a better glide. Semifluorinated n-alkenes (SFAenes) are byproducts in the production process of SFAs and are also found in ski waxes. Snow and soil samples from a ski area in Sweden were taken after a large skiing competition and after snowmelt, respectively, and analyzed for SFAs and SFAenes. Single analyte concentrations in snow (analyzed as melt water) ranged from a few ng L(-1) up to 300 mu g L(-1). Sigma SFA concentrations decreased significantly from the start to the finish of the ski trail. Single analyte concentrations in soil ranged up to 9 ng g(-1) dw. Sigma SFA concentrations in soil did not show a trend along the ski trail. This may be due to the fact that concentrations in soil, although strongly influenced by the competition, reflect inputs during the whole skiing season. The chemical inventory in snow was greater than the inventory in soil for shorter chain SFAs (C(22)-C(28)) and for all SFAenes. Additionally, a significant change in SFA patterns between snow and soil samples was found. These observations suggested volatilization of shorter chain SFAs and of SFAenes during snowmelt. Evidence for long-term accumulation of SFAs in surface soil over several skiing seasons was not found.

Keyword
Semifluorinated n-alkanes, SFAs, SFAenes, Soil, Snow, Ski wax
National Category
Natural Sciences
Identifiers
urn:nbn:se:su:diva-71134 (URN)10.1016/j.chemosphere.2011.08.028 (DOI)000298459000007 ()
Note
authorCount :3Available from: 2012-01-26 Created: 2012-01-26 Last updated: 2012-01-26Bibliographically approved

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