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Tracking fluorinated chemicals and identifying alternatives in contemporary consumer products and technologies
Stockholm University, Faculty of Science, Department of Environmental Science.ORCID iD: 0009-0001-0662-6202
2026 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Per- and polyfluoroalkyl substances (PFAS) are a large group of synthetic chemicals with unique physicochemical properties that have led to their widespread use, ranging from everyday consumer products to critical technologies. Their extreme persistence, combined with other hazardous properties, raises significant concerns for human health and the environment. Limited understanding of PFAS uses across different applications, together with gaps in analytical capabilities, hampers progress towards their phase out and replacement with safer alternatives. 

In this work, analytical investigations were combined with a search of potential PFAS alternatives. Fluorine-based analytical approaches were applied to assess PFAS use across different product categories (Papers I and II), and pyrolysis-gas chromatography-mass spectrometry (Py-GC-MS) was explored to address analytical gaps related to polymeric PFAS (Paper II). Emissions of fluorinated compounds associated with the lifecycle of lithium-ion batteries (LIBs) were investigated to evaluate their relevance as a contamination source in Europe (Paper III). Finally, alternative chemistries to PFAS were explored for applications in stone sealers (Paper I) and LIBs (Paper IV).

In Paper I, total fluorine (TF) analysis of commercial stone sealers revealed that 81% contained fluorine, with concentrations reaching up to 27 150 µg F/g, most likely originating from polymeric PFAS. Extractable organofluorine (EOF) analysis confirmed the predominantly organic nature of the fluorine, and targeted analysis identified polyfluoroalkyl phosphate esters (PAPs) as the dominant PFAS class. Six products were presumably identified as not containing intentionally added PFAS, instead relying on organosilicon-based chemistries, some of which are currently under regulatory scrutiny.

Paper II investigated the application of Py-GC-MS following initial TF screening of cookware (up to 550 000 µg F/g), textiles (up to 1 600 µg F/g), electronics (up to 2 100 µg F/g) and personal care products (up to 630 000 µg F/g). The method demonstrated the ability to detect polytetrafluoroethylene (PTFE) in unknown samples down to 0.1-0.2 wt% and to differentiate between different side-chain fluorinated polymers commonly used in textile applications.

In Paper III, targeted analysis of electrolyte-related anions used in LIBs, such as bis(trifluoromethanesulfonyl)imide (TFSI-), hexafluorophosphate (PF6-) and tetrafluoroborate (BF4-), revealed their widespread occurrence in water samples, with varying regional profiles. BF4- dominated the contamination profile of the Danube in Hungary, while temporal sampling of the River Erpe in Germany showed elevated TFSI- and PF6- concentrations potentially connected to industrial activities, with marked decreases observed during a temporary plant shutdown. In Sweden, recycling and landfill sites were identified as major contributors to environmental TFSI- and PF6-, with concentrations reaching up to 300 ng/L for TFSI- and 39 000 ng/L for PF6-, primarily in landfill-related samples.

Paper IV examined the availability of PFAS alternatives for critical LIB components, specifically cathodes and electrolytes, through a literature review and interviews with experts from academia and industry. The results indicate that while PFAS-free LIBs appear to be technically feasible, such solutions are not yet widely established and require further evaluation with respect to performance, durability, and economic viability. Nevertheless, the outlook is rather promising, as several companies have already introduced PFAS-free solutions or are actively developing them.

Overall, the combination of fluorine mass balance approaches and Py-GC-MS proved effective for screening consumer products for PFAS and for supporting regulatory enforcement. The results further highlight substitution, guided by robust analytical data and lifecycle considerations, as the most effective long-term strategy to reduce PFAS emissions. However, alternatives require careful evaluation to avoid regrettable substitution, particularly in critical technologies such as LIBs.

Place, publisher, year, edition, pages
Stockholm: Department of Environmental Science, Stockholm University , 2026. , p. 27
Keywords [en]
PFAS, fluorinated polymers, fluorine mass balance, stone sealers, combustion ion chromatography, pyrolysis-gas chromatography-mass spectrometry, lithium-ion batteries, emissions, PFAS alternatives
National Category
Environmental Sciences Analytical Chemistry
Research subject
Environmental Sciences
Identifiers
URN: urn:nbn:se:su:diva-251819ISBN: 978-91-8107-504-5 (print)ISBN: 978-91-8107-505-2 (electronic)OAI: oai:DiVA.org:su-251819DiVA, id: diva2:2032812
Public defence
2026-03-13, De Geersalen, Geovetenskapens hus, Svante Arrhenius väg 14 and online via Zoom, public link is available at the department website, Stockholm, 10:00 (English)
Opponent
Supervisors
Available from: 2026-02-18 Created: 2026-01-27 Last updated: 2026-02-06Bibliographically approved
List of papers
1. Fluorine Mass Balance in Commercial Stone Sealers from the US Market and Evaluation of PFAS-free Alternatives
Open this publication in new window or tab >>Fluorine Mass Balance in Commercial Stone Sealers from the US Market and Evaluation of PFAS-free Alternatives
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

Widespread use of per- and polyfluoroalkyl substances (PFAS) by the building industry places it among the major consumers of these chemicals. At the same time, ambiguous labelling and a lack of PFAS measurements in building materials hampers the possibility for consumers to select products which are PFAS-free. To address this, 35 representative sealers were analyzed using a fluorine mass balance approach, combining total and extractable organofluorine (TF and EOF, respectively) measurements with targeted PFAS analysis. TF analysis showed that 81% of the sealers contained fluorinated compounds at concentrations ranging from <LOD up to 27 150 µg F/g. A comparison to EOF revealed that the fluorine in most products was extractable and organic (EOF range <LOD up to 24 073 µg F/g), and most likely PFAS. Nevertheless, targeted PFAS analysis could only account for up to 31% of EOF, pointing to the presence of polymeric PFAS and potentially other low molecular PFAS. Among the detected PFAS, polyfluoroalkyl phosphate esters (PAPs) were the dominant sub-class. Six products appeared to not contain intentionally added PFAS, with organosilicone chemistry identified as the main functional component. Notably, organosilicone-based compounds are also under regulatory scrutiny, and differing views on their risks highlight the broader challenge of identifying truly safer alternatives.

Keywords
PFAS, building materials, total fluorine, extractable organofluorine, CIC, PIGE
National Category
Environmental Sciences
Research subject
Environmental Chemistry; Environmental Sciences
Identifiers
urn:nbn:se:su:diva-251690 (URN)
Funder
Swedish Research Council Formas, 2020-01978EU, Horizon 2020, 101036756
Available from: 2026-01-26 Created: 2026-01-26 Last updated: 2026-01-27
2. Identification and quantification of fluorinated polymers in consumer products by combustion ion chromatography and pyrolysis-gas chromatography-mass spectrometry
Open this publication in new window or tab >>Identification and quantification of fluorinated polymers in consumer products by combustion ion chromatography and pyrolysis-gas chromatography-mass spectrometry
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2024 (English)In: Environmental Science: Processes & Impacts, ISSN 2050-7887, E-ISSN 2050-7895, Vol. 26, no 1, p. 82-93Article in journal (Refereed) Published
Abstract [en]

Total fluorine was determined in 45 consumer product samples from the Swedish market which were either suspected or known to contain fluorinated polymers. Product categories included cookware (70–550 000 ppm F), textiles (10–1600 ppm F), electronics (20–2100 ppm F), and personal care products (10–630 000 ppm F). To confirm that the fluorine was organic in nature, and deduce structure, a qualitative pyrolysis-gas chromatography-mass spectrometry (pyr-GC/MS) method was validated using a suite of reference materials. When applied to samples with unknown PFAS content, the method was successful at identifying polytetrafluoroethylene (PTFE) in cookware, dental products, and electronics at concentrations as low as 0.1–0.2 wt%. It was also possible to distinguish between 3 different side-chain fluorinated polymers in textiles. Several products appeared to contain high levels of inorganic fluorine. This is one of the few studies to quantify fluorine in a wide range of consumer plastics and provides important data on the concentration of fluorine in materials which may be intended for recycling, along with insights into the application of pyr-GC/MS for structural elucidation of fluorinated polymers in consumer products.

National Category
Environmental Sciences
Identifiers
urn:nbn:se:su:diva-225446 (URN)10.1039/d3em00438d (DOI)001125326400001 ()38099738 (PubMedID)2-s2.0-85180087249 (Scopus ID)
Available from: 2024-01-16 Created: 2024-01-16 Last updated: 2026-01-27Bibliographically approved
3. Emissions of Fluorinated Substances from Lithium-Ion Battery Manufacturing and Recycling in Central and Northern Europe
Open this publication in new window or tab >>Emissions of Fluorinated Substances from Lithium-Ion Battery Manufacturing and Recycling in Central and Northern Europe
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

Per- and polyfluoroalkyl substances (PFAS) are recognized as problematic environmental contaminants due to their extreme persistence and other problematic properties. Electrolyte salts and imides such as lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), lithium hexafluorophosphate (LiPF6), and lithium tetrafluoroborate (LiBF4) are widely used in lithium-ion batteries (LIBs), yet their environmental emissions and occurrence remain poorly characterized. This study provides the first comparative assessment of fluorinated compounds associated with the LIB lifecycle in central and northern Europe, focusing on manufacturing in Hungary, electric vehicle production in Germany, and recycling and landfill activities in Sweden. Targeted analysis of surface water, effluent, and leachate samples revealed measurable concentrations of bis(trifluoromethanesulfonyl)imide (TFSI-), inorganic fluorinated anions hexafluorophosphate (PF6-) and tetrafluoroborate (BF4-) across all sites, with distinct regional profiles. In Hungary, BF4- dominated the Danube River and was detected in drinking water, suggesting incomplete removal during riverbank filtration. In Germany, temporal monitoring of the River Erpe showed elevated TFSI- and PF6- levels linked to industrial activity, with clear decreases during a plant shutdown. In Sweden, recycling facilities and landfills emerged as major contributors, with TFSI- concentrations exceeding 300 ng/L and PF6- reaching nearly 39 000 ng/L downstream of a landfill. While these compounds are consistent with LIB applications, they are not exclusive to batteries, and other sources cannot be ruled out. The detection of these substances in treated drinking water underscores their persistence and mobility. Our findings highlight the need for systematic monitoring, improved source attribution, and regulatory oversight of novel fluorinated substances used in LIBs to ensure that the transition to low carbon technologies does not inadvertently exacerbate chemical pollution.

Keywords
Budapest, Danube, Berlin, River Erpe, TFSI-, ultrashort-chain PFAS, TFA, PF6-, BF4-
National Category
Environmental Sciences
Research subject
Environmental Sciences; Environmental Chemistry
Identifiers
urn:nbn:se:su:diva-251695 (URN)
Funder
EU, Horizon 2020, 101036756Swedish Environmental Protection AgencySwedish Research Council Formas, 2021-02059German Research Foundation (DFG)
Available from: 2026-01-26 Created: 2026-01-26 Last updated: 2026-01-27
4. PFAS-Free Energy Storage: Investigating Alternatives for Lithium-Ion Batteries
Open this publication in new window or tab >>PFAS-Free Energy Storage: Investigating Alternatives for Lithium-Ion Batteries
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2024 (English)In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 58, no 50, p. 21908-21917Article, review/survey (Refereed) Published
Abstract [en]

The class-wide restriction proposal on perfluoroalkyl and polyfluoroalkyl substances (PFAS) in the European Union is expected to affect a wide range of commercial sectors, including the lithium-ion battery (LIB) industry, where both polymeric and low molecular weight PFAS are used. The PFAS restriction dossiers currently state that there is weak evidence for viable alternatives to the use of PFAS in LIBs. In this Perspective, we summarize both the peer-reviewed literature and expert opinions from academia and industry to verify the legitimacy of the claims surrounding the lack of alternatives. Our assessment is limited to the electrodes and electrolyte, which account for the most critical uses of PFAS in LIB cells. Companies that already offer or are developing PFAS-free electrode and electrolyte materials were identified. There are also indications that PFAS-free electrolytes are in development by at least one other company, but there is no information regarding the alternative chemistries being proposed. Our review suggests that it is technically feasible to make PFAS-free batteries for battery applications, but PFAS-free solutions are not currently well-established on the market. Successful substitution of PFAS will require an appropriate balance among battery performance, the environmental effects associated with hazardous materials and chemicals, and economic considerations.

Keywords
binder, cathode, electrolyte additives, electrolyte salt, fluoropolymers, green energy transition, PVDF, renewable energy
National Category
Environmental Sciences
Identifiers
urn:nbn:se:su:diva-240541 (URN)10.1021/acs.est.4c06083 (DOI)001370315200001 ()39630075 (PubMedID)2-s2.0-85211096325 (Scopus ID)
Available from: 2025-03-11 Created: 2025-03-11 Last updated: 2026-01-27Bibliographically approved

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