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Pan, Y., Wang, J., Yeung, L. W. Y., Wei, S. & Dai, J. (2020). Analysis of emerging per- and polyfluoroalkyl substances: Progress and current issues. TrAC. Trends in analytical chemistry, 124, Article ID 115481.
Open this publication in new window or tab >>Analysis of emerging per- and polyfluoroalkyl substances: Progress and current issues
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2020 (English)In: TrAC. Trends in analytical chemistry, ISSN 0165-9936, E-ISSN 1879-3142, Vol. 124, article id 115481Article, review/survey (Refereed) Published
Abstract [en]

The increasingly stringent restrictions on legacy per- and polyfluoroalkyl substances (PFASs) have led to the compensatory use of new fluorinated replacements. These new compounds, hereafter referred to as emerging PFASs, continue to be discovered and are now showing ubiquity in abiotic and biotic environments. Thus, there is an urgent need for robust, yet sensitive analytical methods to determine their occurrence and understand their behavior, fate, impact, and toxicity. Here, we review the up-to-date sample preparation and analytical methodologies for emerging PFASs based on peer-reviewed literature published in the past three years (2015-2018). The determination of emerging PFASs is similar to that of legacy PFASs, with satisfactory performances for most emerging PFASs achieved using conventional extraction and analytical approaches. However, the determination of certain specific analytes remains challenging due to the unavailability of standards and reference materials, low recoveries and matrix effects, background contamination, and poor sensitivities due to in-source fragmentation. Despite recent progress in identifying ionic semi-volatile PFASs with liquid chromatograph-high-resolution mass spectrometry (LC-HRMS), our knowledge on new types of neutral volatile PFASs remains poor due to limited non-target analysis using gas chromatograph (GC)-HRMS.

Place, publisher, year, edition, pages
Elsevier, 2020
Keywords
Per- and polyfluoroalkyl substances, Emerging contaminants, Extraction, Liquid chromatography, Triple quadrupole, Quantification, Non-target screening, High-resolution mass spectrometry, In-source fragmentation, Isomer-specific analysis
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:oru:diva-80850 (URN)10.1016/j.trac.2019.04.013 (DOI)000518368000003 ()2-s2.0-85064568538 (Scopus ID)
Note

Funding Agencies:

National Natural Science Foundation of China 21737004

Chinese Academy of Sciences XDB14040202

Available from: 2020-03-26 Created: 2020-03-26 Last updated: 2020-03-26Bibliographically approved
Björnsdotter, M., Yeung, L. W. Y., Kärrman, A. & Ericson Jogsten, I. (2020). Challenges in the analytical determination of ultra-short-chain perfluoroalkyl acids and implications for environmental and human health. Analytical and Bioanalytical Chemistry
Open this publication in new window or tab >>Challenges in the analytical determination of ultra-short-chain perfluoroalkyl acids and implications for environmental and human health
2020 (English)In: Analytical and Bioanalytical Chemistry, ISSN 1618-2642, E-ISSN 1618-2650Article, review/survey (Refereed) Epub ahead of print
Abstract [en]

Ultra-short-chain perfluoroalkyl acids have recently gained attention due to increasing environmental concentrations being observed. The most well-known ultra-short-chain perfluoroalkyl acid is trifluoroacetic acid (TFA) which has been studied since the 1990s. Potential sources and the fate of ultra-short-chain perfluoroalkyl acids other than TFA are not well studied and data reporting their environmental occurrence is scarce. The analytical determination of ultra-short-chain perfluoroalkyl acids is challenging due to their high polarity resulting in low retention using reversed-phase liquid chromatography. Furthermore, recent studies have reported varying extraction recoveries in water samples depending on the water matrix and different methods have been suggested to increase the extraction recovery. The present review gives an overview of the currently used analytical methods and summarizes the findings regarding potential analytical challenges. In addition, the current state of knowledge regarding TFA and other ultra-short-chain perfluoroalkyl acids, namely perfluoropropanoic acid, trifluoromethane sulfonic acid, perfluoroethane sulfonic acid, and perfluoropropane sulfonic acid‚ are reviewed. Both known and potential sources as well as environmental concentrations are summarized and discussed together with their fate and the environmental and human implications.

Place, publisher, year, edition, pages
Springer, 2020
Keywords
Perfluoroethane sulfonic acid, Perfluoropropane sulfonic acid, Perfluoropropanoic acid, Trifluoroacetic acid, Trifluoromethane sulfonic acid, Ultra-short-chain perfluoroalkyl acid, Extraction, Analytical challenge, Analytical determination, Environmental concentration, Environmental occurrence, Perfluoroalkyl acids, Reversed phase liquid-chromatography, Liquid chromatography
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:oru:diva-81970 (URN)10.1007/s00216-020-02692-8 (DOI)2-s2.0-85084523174 (Scopus ID)
Available from: 2020-05-22 Created: 2020-05-22 Last updated: 2020-05-22Bibliographically approved
Dubocq, F., Wang, T., Yeung, L. W. Y., Sjöberg, V. & Kärrman, A. (2020). Characterization of the Chemical Contents of Fluorinated and Fluorine-Free Firefighting Foams Using a Novel Workflow Combining Nontarget Screening and Total Fluorine Analysis. Environmental Science and Technology, 54(1), 245-254
Open this publication in new window or tab >>Characterization of the Chemical Contents of Fluorinated and Fluorine-Free Firefighting Foams Using a Novel Workflow Combining Nontarget Screening and Total Fluorine Analysis
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2020 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 54, no 1, p. 245-254Article in journal (Refereed) Published
Abstract [en]

Aqueous film-forming foams (AFFFs) are widely used to extinguish liquid fires due to their film-forming properties. AFFF formulation historically contains per- and polyfluoroalkyl substances (PFASs) that can be very persistent and pose a health risk to biota and humans. Detailed analysis of the chemical composition of AFFFs can provide a better understanding on the potential environmental impact of the ingredients. In this study, a novel workflow combining target analysis, nontarget screening analysis (NTA), total fluorine (TF) analysis, and inorganic fluoride (IF) analysis was applied to disclose the chemical composition of 24 foams intended for liquid fires. Foams marketed as containing PFASs as well as fluorine-free foams were included. By comparing the sum of targeted PFASs and total organofluorine concentrations, a mass balance of known and unknown organofluorine could be calculated. Known organofluorine accounted for <1% in most fluorine-containing AFFFs, and it was confirmed that the foams marketed as fluorine-free did not contain measurable amounts of organofluorine substances. Five fluorinated substances were tentatively identified, and non-fluorinated zwitterionic betaine compounds, which are considered to be replacement substances for PFASs, were tentatively identified in the organofluorine-free foams.

Place, publisher, year, edition, pages
ACS Publications, 2020
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:oru:diva-78825 (URN)10.1021/acs.est.9b05440 (DOI)000506723200027 ()31789512 (PubMedID)
Funder
Swedish Civil Contingencies AgencyKnowledge Foundation
Note

Funding Agency:

Swedish Chemicals Agency

Available from: 2019-12-20 Created: 2019-12-20 Last updated: 2020-01-27Bibliographically approved
Koch, A., Aro, R., Wang, T. & Yeung, L. W. Y. (2020). Towards a comprehensive analytical workflow for the chemical characterisation of organofluorine in consumer products and environmental samples. TrAC. Trends in analytical chemistry, 123, Article ID 115423.
Open this publication in new window or tab >>Towards a comprehensive analytical workflow for the chemical characterisation of organofluorine in consumer products and environmental samples
2020 (English)In: TrAC. Trends in analytical chemistry, ISSN 0165-9936, E-ISSN 1879-3142, Vol. 123, article id 115423Article, review/survey (Refereed) Published
Abstract [en]

This review summarizes and discusses eight analytical methods for organofluorine (OF) analysis, which offer detection limits suitable for consumer products and environmental samples. Direct sample analysis of OF only applies to some techniques on consumer products, whereas others require sample pretreatment or concentration before measurements. Comparison between methods for OF analysis were found to be difficult because of different selectivity (between OF and fluoride), sensitivity and type of samples (bulk, extract, surface) analysed. Neither inter-laboratory comparison on OF analysis nor suitable certified reference materials have been used for method validation, which makes data comparability between studies challenging. A top down approach for the comprehensive assessment of OF is proposed, where OF/extractable OF is first measured, followed by target analysis to obtain unquantifiable OF concentrations using the mass balance approach. For further identification of unquantifiable OF, approaches such as total oxidizable precursor assay, suspect and non-target screening are briefly discussed.

Place, publisher, year, edition, pages
Elsevier, 2020
Keywords
Fluorine mass balance, Extractable organofluorine (EOF), Per- and polyfluoroalkyl substances (PFASs), Combustion ion chromatography (CIC), Particle-induced gamma-ray emission spectrometry (PIGE), Inductively coupled plasma MS/MS (ICP-MS/MS)
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:oru:diva-80250 (URN)10.1016/j.trac.2019.02.024 (DOI)000512979800001 ()2-s2.0-85062809595 (Scopus ID)
Funder
Swedish Research Council, 2015-00320Swedish Research Council Formas, 2016-01158Knowledge Foundation, 20160019
Available from: 2020-02-28 Created: 2020-02-28 Last updated: 2020-02-28Bibliographically approved
Sadia, M., Yeung, L. W. Y. & Fiedler, H. (2020). Trace level analyses of selected perfluoroalkyl acids in food: Method development and data generation. Environmental Pollution, 263, Article ID 113721.
Open this publication in new window or tab >>Trace level analyses of selected perfluoroalkyl acids in food: Method development and data generation
2020 (English)In: Environmental Pollution, ISSN 0269-7491, E-ISSN 1873-6424, Vol. 263, article id 113721Article in journal (Refereed) Epub ahead of print
Abstract [en]

To comprise the future requirements to detect low levels of perfluoroalkyl acids (PFAAs) including branched and linear perfluorooctane sulfonic acid (PFOS), perfluorooctanoic acid (PFOA), and perfluorohexane sulfonic acid (PFHxS) in food items, analytical methods for their determination in five different food matrices (cow milk, butter, chicken meat, beef, and fish) were developed and validated. Analytical method for eggs was only validated for PFOS and PFOA because of interfering substance appeared in some samples. The method applied on foods of animal origin includes alkaline digestion, extraction, and clean-up with solid phase extraction and adsorption on granular carbon where necessary. The method was shown effective to eliminate taurodeoxycholic acid (TDC), a bile acid that is an endogenous interference compound in egg samples causing ionization suppression and false positive result for PFOS when 499 &gt; 80 transition was used for quantification. The validation was performed and resulted in recoveries &gt;70% for all three PFAAs, the limits of quantification (LOQs) in all matrices were 3.1 pg g−1, 3.4 pg g−1, and 4.9 pg g−1 for PFHxS, PFOA, and L-PFOS, respectively. The optimized method was successfully applied to 53 food samples from the Swedish market and from developing countries. PFOS and PFOA were detected in all samples. PFHxS was detected in 76% of the samples. Further method development on separating interfering substance from PFHxS in egg is warranted due to relatively high detection of this compound in other food items. With this method, concentrations in the low pg g−1 range in food samples of animal origin were quantified including the branched PFOS isomers. This method can be applied to enforce potential future limit values for PFOS and PFOA as a consequence of the recent European Food Safety Authority (EFSA) recommendation where the tolerable intakes have been drastically lowered. Further method development is needed for foods of plant origin such as vegetables, flour, nuts, or bread. 

Place, publisher, year, edition, pages
Elsevier, 2020
Keywords
Bile acid, European Food Safety Authority (EFSA), Fatty foods, Perfluoroalkyl substances, United Nations Environment Programme (UNEP)
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:oru:diva-81006 (URN)10.1016/j.envpol.2019.113721 (DOI)32229370 (PubMedID)2-s2.0-85082431969 (Scopus ID)
Available from: 2020-04-03 Created: 2020-04-03 Last updated: 2020-04-03Bibliographically approved
Mullin, L. G., Katz, D. R., Riddell, N., Plumb, R., Burgess, J. A., Yeung, L. W. Y. & Ericson Jogsten, I. (2019). Analysis of hexafluoropropylene oxide-dimer acid (HFPO-DA) by liquid chromatography-mass spectrometry (LC-MS): Review of current approaches and environmental levels. TrAC. Trends in analytical chemistry, 118, 828-839
Open this publication in new window or tab >>Analysis of hexafluoropropylene oxide-dimer acid (HFPO-DA) by liquid chromatography-mass spectrometry (LC-MS): Review of current approaches and environmental levels
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2019 (English)In: TrAC. Trends in analytical chemistry, ISSN 0165-9936, E-ISSN 1879-3142, Vol. 118, p. 828-839Article, review/survey (Refereed) Published
Abstract [en]

Emerging per- and polyfluorinated compounds (PFAS) compounds are of increasing interest for environmental monitoring, one being hexafluoropropylene oxide-dimer acid (HFPO-DA), commonly referred to as GenX. The following review describes existing liquid chromatography-mass spectrometry (LC-MS) methods used to analyse HFPO-DA, including sample preparation and method sensitivity relative to other PFAS. Analytical challenges are also described, in particular the significant formation of in-source fragmentation, dimer and dimer adducts which detract from [M-H](-) signal. Lastly, detected levels of HFPO-DA in environmental and biological samples are compared across the limited number of available field exposure studies, which found several mu g/L concentrations in water samples taken near fluorochemical plant discharges.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
HFPO-DA, GenX, Negative polarity electrospray ionisation, Liquid chromatography, Mass spectrometry
National Category
Chemical Sciences
Identifiers
urn:nbn:se:oru:diva-76970 (URN)10.1016/j.trac.2019.05.015 (DOI)000486383900064 ()31501636 (PubMedID)
Note

Funding Agency:

Intramural EPA  EPA999999

Available from: 2019-10-02 Created: 2019-10-02 Last updated: 2019-10-02Bibliographically approved
Yeung, L. W. Y., Yamashita, N. & Falandysz, J. (2019). Legacy and emerging perfluorinated and polyfluorinated compounds: An update. Chemosphere, 237, Article ID UNSP 124506.
Open this publication in new window or tab >>Legacy and emerging perfluorinated and polyfluorinated compounds: An update
2019 (English)In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 237, article id UNSP 124506Article in journal, Editorial material (Other academic) Published
Place, publisher, year, edition, pages
Elsevier, 2019
National Category
Environmental Sciences
Identifiers
urn:nbn:se:oru:diva-78515 (URN)10.1016/j.chemosphere.2019.124506 (DOI)000496896700130 ()31400742 (PubMedID)2-s2.0-85073703038 (Scopus ID)
Available from: 2019-12-10 Created: 2019-12-10 Last updated: 2019-12-10Bibliographically approved
Kärrman, A., Wang, T., Kallenborn, R., Langseter, A. M., Grønhovd, S. M., Ræder, E. M., . . . Fredriksson, F. (2019). PFASs in the Nordic environment: Screening of Poly- and Perfluoroalkyl Substances (PFASs) and Extractable Organic Fluorine (EOF) in the Nordic Environment. Copenhagen: Nordisk Ministerråd
Open this publication in new window or tab >>PFASs in the Nordic environment: Screening of Poly- and Perfluoroalkyl Substances (PFASs) and Extractable Organic Fluorine (EOF) in the Nordic Environment
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2019 (English)Report (Refereed)
Abstract [en]

This report describes a screening study of in all ninety-nine conventional and emerging per- and polyfluoroalkyl substances (PFASs) in the Nordic environment. In addition, extractable organic fluorine (EOF) was analysed. The latter can provide the amount, but not identity, of organofluorine in the samples, which in turn can be used to assess the mass balance between known and unknown PFASs. The study was initiated by the Nordic Screening Group and funded by these and the Nordic Council of Ministers through the Chemicals Group. A total of 102 samples were analyzed in this study, including bird eggs, fish, marine mammals, terrestrial mammals, surface water, WWTP effluents and sludge, and air. Samples were collected by institutes from the participating countries and self-governing areas; Denmark, Faroe Islands, Finland, Greenland, Iceland, Norway, and Sweden.

Place, publisher, year, edition, pages
Copenhagen: Nordisk Ministerråd, 2019. p. 153
Series
TemaNord, ISSN 0908-6692 ; 2019:515
National Category
Environmental Management
Research subject
Environment and Climate; Chemicals
Identifiers
urn:nbn:se:oru:diva-81431 (URN)10.6027/TN2019-515 (DOI)978-92-893-6061-6 (ISBN)978-92-893-6062-3 (ISBN)978-92-893-6063-0 (ISBN)
Funder
Nordic Council of Ministers
Note

The study was conducted on behalf of the Nordic Screening group (www.nor-dicscreening.org) which commissioned and funded the work with financial support gra-ciously provided by the Nordic Council of Ministers Chemicals Group, and the partici-pating agencies and institutes.

Available from: 2020-04-30 Created: 2020-04-30 Last updated: 2020-04-30
Koch, A., Kärrman, A., Yeung, L. W. Y., Jonsson, M., Ahrens, L. & Wang, T. (2019). Point source characterization of per- and polyfluoroalkyl substances (PFASs) and extractable organofluorine (EOF) in freshwater and aquatic invertebrates. Environmental Science: Processes & Impacts, 21(11), 1887-1898
Open this publication in new window or tab >>Point source characterization of per- and polyfluoroalkyl substances (PFASs) and extractable organofluorine (EOF) in freshwater and aquatic invertebrates
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2019 (English)In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 21, no 11, p. 1887-1898Article in journal (Refereed) Published
Abstract [en]

Major point sources of per- and polyfluoroalkyl substances (PFASs) cause ubiquitous spread of PFASs in the environment. In this study, surface water and aquatic invertebrates at three Swedish sites impacted by PFAS point sources were characterized, using homologue, isomer and extractable organofluorine (EOF) profiling as well as estimation of bioaccumulation factors (BAFs) and mass discharge. Two sites were impacted by fire training (sites A and R) and the third by industrial runoff (site K). Mean Σ25PFASs concentration in water was 1920 ng L-1 at site R (n = 3), which was more than 20- and 10-fold higher than those from sites A and K, respectively. PFOS was the most predominant PFAS in all waters samples, constituting 29-79% of Σ25PFAS concentrations. Several branched isomers were detected and they substantially contributed to concentrations in surface water (e.g. 49-78% of ΣPFOS) and aquatic invertebrates (e.g. 15-28% of ΣPFOS). BAFs in the aquatic invertebrates indicated higher bioaccumulation for long chain PFASs and lower bioaccumulation for branched PFOS isomers compared to linear PFOS. EOF mass balance showed that Σ25target PFASs in water could explain up to 55% of EOF at site R. However, larger proportions of EOF (>92%) remained unknown in water from sites A and K. Mass discharges were for the first time estimated for EOF and revealed that high amounts of EOF (e.g. 8.2 g F day-1 at site A) could be transported by water to recipient water bodies relative to Σ25PFASs (e.g. 0.15 g day-1 at site A). Overall, we showed that composition profiling, BAFs and EOF mass balance can improve the characterization of PFASs around point sources.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2019
National Category
Oceanography, Hydrology and Water Resources Environmental Sciences
Identifiers
urn:nbn:se:oru:diva-76827 (URN)10.1039/c9em00281b (DOI)000498711800007 ()31552402 (PubMedID)2-s2.0-85074962116 (Scopus ID)
Funder
Swedish Research Council, 2015-00320Swedish Research Council Formas, 2016-01158Knowledge Foundation, 20160019
Available from: 2019-09-30 Created: 2019-09-30 Last updated: 2019-12-13Bibliographically approved
Uwayezu, J.-N., Yeung, L. W. Y. & Bäckström, M. (2019). Sorption of PFOS isomers on goethite as a function of pH, dissolved organic matter (humic and fulvic acid) and sulfate. Chemosphere, 233, 896-904
Open this publication in new window or tab >>Sorption of PFOS isomers on goethite as a function of pH, dissolved organic matter (humic and fulvic acid) and sulfate
2019 (English)In: Chemosphere, ISSN 0045-6535, E-ISSN 1879-1298, Vol. 233, p. 896-904Article in journal (Refereed) Published
Abstract [en]

Understanding the distribution of PFOS isomers between the aqueous phase and goethite is crucial, since it is an abundant sorbent and thus may have a large influence on the mobility of PFOS. This study was conducted to understand the effects of pH, humic acid (HA), fulvic acid (FA) and sulfate on sorption of PFOS isomers. The results will increase the understanding about what parameters may control the fate and transport of PFOS in surface and ground water.

The study was conducted by adding PFOS spiked water to a goethite slurry with different aqueous chemistry. Levels of total PFOS and PFOS isomers were quantified using an Ultra-Performance Liquid Chromatograph coupled to a triple quadrupole mass spectrometer. Results showed that sorption of PFOS was mainly dependent on pH; sorption decreased as pH increased. Presence of HA increased log K-d from 1.29 to 2.03, 1.76 to 1.92 and 1.51 to 1.96 at pH 5.50-7.50 for 3-/4-/4-PFOS, 6-/2-PFOS and L-PFOS, respectively. Changes in the aqueous chemistry also affected the behaviour of PFOS as the addition of Na2SO4 enhanced the sorption of PFOS. Results showed that L-PFOS was more readily sorbed to goethite at pH < 4.35 both in the presence and in the absence of humic or fulvic acids. At pH > 4.5 the 3-/4-/5-PFOS isomer group was more associated to goethite. Besides electrostatic interactions, which controlled the sorption of PFOS, this study indicate that the presence of dissolved humic substances in the aqueous phase enhances the sorption via hydrophobic mechanisms.

Place, publisher, year, edition, pages
Elsevier, 2019
Keywords
Goethite, Perfluorooctane sulfonate, Sorption, Humic substances, Electrostatic and hydrophobic interactions
National Category
Environmental Sciences
Identifiers
urn:nbn:se:oru:diva-75699 (URN)10.1016/j.chemosphere.2019.05.252 (DOI)000477691500099 ()31340417 (PubMedID)2-s2.0-85067315052 (Scopus ID)
Funder
Knowledge Foundation, 20160019
Available from: 2019-08-14 Created: 2019-08-14 Last updated: 2019-08-14Bibliographically approved
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ORCID iD: ORCID iD iconorcid.org/0000-0001-6800-5658

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