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Ecotoxicology and Public Health

Fluorinated Compounds in North American Cosmetics
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  • Heather D. Whitehead
    Heather D. Whitehead
    Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, United States
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  • Marta Venier
    Marta Venier
    O’Neill School of Public and Environmental Affairs, Indiana University, Bloomington, Indiana 47405, United States
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    Orcidhttps://orcid.org/0000-0002-2089-8992
  • Yan Wu
    Yan Wu
    O’Neill School of Public and Environmental Affairs, Indiana University, Bloomington, Indiana 47405, United States
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    Orcidhttps://orcid.org/0000-0001-7876-261X
  • Emi Eastman
    Emi Eastman
    Department of Physics, University of Notre Dame, Notre Dame, Indiana 46556, United States
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  • Shannon Urbanik
    Shannon Urbanik
    Department of Chemistry, Hope College, Holland, Michigan 49423, United States
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  • Miriam L. Diamond
    Miriam L. Diamond
    Department of Earth Sciences, University of Toronto, Toronto, Ontario M5S 3B1, Canada
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    Orcidhttps://orcid.org/0000-0001-6296-6431
  • Anna Shalin
    Anna Shalin
    Department of Earth Sciences, University of Toronto, Toronto, Ontario M5S 3B1, Canada
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  • Heather Schwartz-Narbonne
    Heather Schwartz-Narbonne
    Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6, Canada
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    Orcidhttps://orcid.org/0000-0003-4776-0974
  • Thomas A. Bruton
    Thomas A. Bruton
    Green Science Policy Institute, Berkeley, California 94709, Canada
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  • Arlene Blum
    Arlene Blum
    Green Science Policy Institute, Berkeley, California 94709, Canada
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  • Zhanyun Wang
    Zhanyun Wang
    Institute of Environmental Engineering, ETH Zürich, 8093 Zürich, Switzerland
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    Orcidhttps://orcid.org/0000-0001-9914-7659
  • Megan Green
    Megan Green
    Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, United States
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  • Meghanne Tighe
    Meghanne Tighe
    Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, United States
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    Orcidhttps://orcid.org/0000-0002-8930-892X
  • John T. Wilkinson
    John T. Wilkinson
    Department of Physics, University of Notre Dame, Notre Dame, Indiana 46556, United States
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    Sean McGuinness
    Department of Physics, University of Notre Dame, Notre Dame, Indiana 46556, United States
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    Graham F. Peaslee
    Department of Physics, University of Notre Dame, Notre Dame, Indiana 46556, United States
    *Email: [email protected]
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    Orcidhttps://orcid.org/0000-0001-6311-648X
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Environmental Science & Technology Letters

Cite this: Environ. Sci. Technol. Lett. 2021, 8, 7, 538–544
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https://doi.org/10.1021/acs.estlett.1c00240
Published June 15, 2021

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Abstract

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Per- and polyfluoroalkyl substances (PFAS), a highly persistent and potentially toxic class of chemicals, are added to cosmetics to increase their durability and water resistance. To assess this potential health and environmental risk, 231 cosmetic products purchased in the U.S. and Canada were screened for total fluorine using particle-induced gamma-ray emission spectroscopy. Of the eight categories tested, foundations, mascaras, and lip products had the highest proportion of products with high total fluorine ≥0.384 μg F/cm2. Twenty-nine products including 20 with high total fluorine concentrations were analyzed using targeted LC-MS/MS and GC-MS. PFAS concentrations ranged from 22–10,500 ng/g product weight, with an average and a median of 264 and 1050 ng/g product weights, respectively. Here, 6:2 and 8:2 fluorotelomer compounds, including alcohols, methacrylates, and phosphate esters, were most commonly detected. These compounds are precursors to PFCAs that are known to be harmful. The ingredient lists of most products tested did not disclose the presence of fluorinated compounds exposing a gap in U.S. and Canadian labeling laws. The manufacture, use, and disposal of cosmetics containing PFAS are all potential opportunities for health and ecosystem harm. Given their direct exposure routes into people, better regulation is needed to limit the widespread use of PFAS in cosmetics.

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Introduction

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Per- and polyfluoroalkyl substances (PFAS) comprise a class of more than 4700 chemical compounds for which the characteristic perfluorinated carbon moiety confers hydrophobic chemical properties and environmental persistence. Since the 1950s, these compounds have been widely used in industrial products such as firefighting foams and consumer products such as coated fabrics, carpets, cookware and other food packaging, and many others. (1−4) In 2019, the retail value of personal care products was estimated to be more than $100 billion (USD) in North America, with approximately $20 billion coming from cosmetics. (5) While several studies have documented the use of PFAS in cosmetics from Europe and Asia, no such data exist in North America. (6−8) PFAS in cosmetics may pose a risk to human health through direct and indirect exposure, as well as a risk to ecosystem health throughout the lifecycle of these products. PFAS are used in cosmetics due to their properties such hydrophobicity and film-forming ability, which are thought to increase product wear, durability, and spreadability. Additional claimed benefits are increased skin absorption of the product and improvements in the appearance or texture of skin. (9)
Gluge et al. (9) recently noted that the magnitude of PFAS use in cosmetics in several European countries was difficult to estimate due to lax regulatory requirements for reporting PFAS use. Requirements in the United States (U.S.) and Canada are similarly lax. Use and labeling of cosmetic ingredients in the U.S. is regulated by the Federal Food, Drug, and Cosmetics Act of 1938 and the Fair Packaging and Labeling Act of 1967. These acts do not regulate the type or kind of testing that is needed to determine the safety of cosmetic ingredients, and exemptions exist for labeling ingredients which are considered proprietary. (10) In Canada, the Food and Drugs Act, the Cosmetic Regulations, and the Consumer Packaging and Labeling Act and Regulations regulate the labeling and safety of cosmetics. (11) These require all ingredients (except “incidental” ingredients such as processing agents) to be disclosed both to federal regulators and to consumers on product packaging.
Cosmetics industry-associated groups usually assess the potential hazards of new and emerging ingredients in North American cosmetics. Ingredient names are defined and disclosed per the guidelines given in the International Cosmetic Ingredient Dictionary and Handbook. (12) This document is prepared by the International Cosmetic Ingredient Nomenclature Committee, which is a group sponsored by the Personal Care Products Council. (13) This council includes more than 600 member companies that produce and distribute the “vast majority” of personal care products in the U.S. (14) The Personal Care Product Council also funds the Cosmetic Ingredient Review (CIR) which seeks to assess the safety of cosmetic ingredients. Assessments made by CIR are subsequently utilized by regulatory bodies when determining the need for new or modified regulations. Without formal regulations that define how cosmetic ingredients should be labeled, the INCI Dictionary and Handbook is used by cosmetic manufacturers when determining how to label chemical ingredients. However, using this handbook for guidance to establish the presence of PFAS from ingredient labels is complicated by the series of exemptions and generalized guidelines for polymers, silanes and siloxanes, color additives, and substituted compounds.
Three studies have measured PFAS in a total of 72 cosmetics available in Sweden, Denmark, Japan, and the Republic of Korea between 2009–2017. (6−8) These publications focused on the measurement of PFAS in cosmetics using LC-MS/MS as well as total fluorine through combustion ion chromatography (CIC). Cosmetics analyzed in these studies were those that disclosed a fluorinated ingredient in their labeling, including foundations, facial creams, concealers, and other personal care products such as sunscreens and shaving foams. Lip and eye products, two prominent classes of products in the North American cosmetics market, were surveyed at low frequencies in these previous studies, presumably because labeling did not indicate the presence of a fluorinated ingredient. Of concern is that these classes of cosmetics are applied close to the eyes and the mouth, which could increase exposure and hence risk due to enhanced absorption and ingestion.
Our goal was to determine the occurrence of PFAS in cosmetics in U.S. and Canada, especially mascaras and lipsticks, using particle-induced gamma-ray emission (PIGE) spectroscopy to rapidly screen total fluorine concentrations in 231 cosmetic products, followed by targeted analysis. PIGE has previously been utilized to measure total fluorine levels, the combination of inorganic and organic sources of fluorine in food packaging and firefighting textiles and foams. (15−17) Targeted analysis of PFAS was conducted on a subset of products by means of liquid chromatography-tandem mass spectrometry (LC-MS/MS) and gas chromatographic mass spectrometry (GC-MS). Finally, we discuss the U.S. and Canadian regulatory regimes with respect to PFAS use in cosmetics by evaluating the relationship between PFAS presence and its disclosure, or lack thereof, on ingredient labels.

Materials and Methods

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A total of 231 cosmetics were purchased or obtained as free samples for analysis. U.S. cosmetics were purchased from retailers in Indiana and Michigan including Ulta Beauty, Sephora, Target, and Bed Bath & Beyond from 2016 to 2020. Canadian products were purchased online from Sephora and Shoppers Drug Mart in Toronto, ON, Canada in 2020. Canadian products included replicates of cosmetics purchased in the U.S. as well as five products from Canadian brands. Products selected for targeted analysis were repurchased in 2020 in both the U.S. and Canada to compare the amount and kinds of PFAS present. All ingredients were tabulated, including those listed as “may or may not be present”. Samples were grouped into categories based on the intended use of the product as defined by the manufacturer (Table S1). All brands analyzed and their product categories are reported in Table S2. Information on the collection and analysis of ingredient lists are given in the SI.
For PIGE analysis, all samples were applied to the surface of a fluorine-free Whatman 1 qualitative filter paper (Sigma-Aldrich, St. Louis, MO) or standard fluorine-free copier paper. These papers were also used as blanks. Samples were mounted to stainless steel target frames for ex vacuo ion beam analysis. These analyses were conducted on two particle accelerators, one at Hope College between 2016 and 2017 and the second at the University of Notre Dame between 2018 and 2020. Instrumental changes were made to the particle accelerator at the University of Notre Dame between 2018 and 2020. Fluorinated paper standards were analyzed at each facility to normalize the fluorine signals given at these different locations and time points. Details of this normalization, as well as the instrumental analysis using PIGE and of the use of inorganic fluoride standards soaked into paper to convert fluorine signals to a total fluorine concentration, are shown in Table S3 and Figure S1. The limit of detection (LOD) was 0.127 μg F/cm2, and the limit of quantification was 0.384 μg F/cm2, as determined by the standard response of prepared external inorganic fluoride standards. Replicate PIGE analyses were performed on roughly 5% of the samples, and a blank was measured every ∼50 samples as QA/QC. Note that PIGE measures fluorine from inorganic and organic sources giving a measurement of the total fluorine in a sample.
Twenty-nine products including 20 with high total fluorine signals were selected for targeted analysis using LC-MS/MS and GC-MS. Full names, abbreviations, and methods for all 53 PFASs and additional information including the analytes measured for targeted analysis are given in Tables S4–S7 and have been adapted from methods previously published. (18) Details of the targeted analysis are reported in the Supporting Information, including details on QA/QC. Briefly, 50–100 mg of product was spiked with surrogate standards before sonicating twice with 3 mL of 4:1 hexane–isopropanol and twice with 3 mL of 1:1 methanol–acetonitrile. Supernatants were combined and concentrated to a final volume of 5 mL under nitrogen. Concentrates were vortexed and centrifuged with 100 mg of Envi-Carb for cleanup, concentrated again under nitrogen, and filtered. Filtrate was transferred to polypropylene vials and spiked with internal standards for quantitation. LC-MS/MS analysis was done using an ultrahigh performance LC coupled with a triple-quadrupole MS (Agilent 1290 Infinity II UPLC–6470 QQQ-MS) in negative electrospray ionization mode. GC-MS analysis was performed on an Agilent 7890 GC–5977B PCI-MS operated in the positive chemical ionization mode. Additional instrumental parameters can be found in the Supporting Information of Wu et al. (18) A procedural blank and a matrix spike sample were processed along with each batch sample to evaluate possible contamination from laboratory operations and the performance of our method. The recoveries of surrogate standards were all in the range of 60%–130%. Samples were corrected for recovery using the appropriate surrogate standards (Table S7). After this correction, matrix spike recoveries of individual analytes were all within 80%–115%. Additionally, data reported in this study were blank corrected by subtracting the corresponding average blank on a mass basis. The method detection limits (MDLs) were defined as the average procedural blank +3 × standard deviation (n = 5) or the amount of chemical generating a signal-to-noise of 5 if the compound was not detected in the procedural blanks.

Results and Discussion

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Total Fluorine Screening Using PIGE

A total of 231 cosmetics across eight categories including lip products, eye products, foundations, face products, mascaras, concealers, eyebrow products, and miscellaneous products were analyzed using PIGE (Table S1). Foundations produced the highest median total fluorine concentration, while mascaras produced the largest range of total fluorine measurements. Table S8 and Figure S2 provide additional analysis of the PIGE data in each category including the μg F/cm2 distribution for all 231 products analyzed. We characterized the concentration of total fluorine for each product as containing fluorine ≤ LOD (0–0.127 μg F/cm2, 32%), fluorine between LOD and LOQ (0.127–0.384 μg F/cm2, 16%), and high fluorine (>0.384 μg F/cm2, 52%) as shown in Figure 1. For the subset of products analyzed by targeted analysis, concentrations ranged from LOD greater than 42.3 to 2360 μg F/g product (Table S9). The cosmetic categories that had the highest percentage of high fluorine products were foundations (63%), eye products (58%), mascaras (47%), and lip products (55%).

Figure 1

Figure 1. Foundations produced the highest median total fluorine (μg F/cm2) in 231 products groups across eight categories. Breakdown of the number of products tested in each of the eight products categories and proportion of items in each category that was categorized as high, moderate, and low total fluorine concentrations. Several mascaras gave the highest fluorine concentrations measured. All remaining categories produced similar medians but with varying ranges. The three cosmetic categories that had the highest proportion of high fluorine concentrations were foundations, mascaras, and lip products.

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A comparison of the total fluorine concentrations with those reported by Schultes et al. (7) revealed similar ppm measurements of PFAS for overlapping cosmetic product categories such as foundations. The nine foundations tested in ref (14) had total fluorine concentrations determined using CIC from LOD of less than 91.1 to 3120 μg/g which is a similar range to that reported here. Total fluorine reported by Brinch et al. (8) ranged from 3.3 to 740 μg/g, lower than ranges reported here and by Schultes et al. (7)
Analysis of the total fluorine concentrations from PIGE revealed interesting trends within the selected categories. High fluorine levels were found in products commonly advertised as “wear-resistant” to water and oils or “long-lasting” including foundations, liquid lipsticks, and waterproof mascaras. (19−22) These terms align with the functionality given for the use of many PFAS in cosmetics in industrial literature. (23−25) The percentage of products with high fluorine concentrations in foundations, mascaras, and lip products suggested a possible link to the use of fluorinated ingredients in their manufacturing. Hence, foundations, mascaras, and lip products were selected for targeted MS analyses. Additional analyses of these trends determined from PIGE analysis are given in Table S9.

Targeted Analyses Using GC-MS and LC-MS/MS

All 29 cosmetic products contained detectable levels of at least four PFAS as shown in Table 1, with a maximum of 13 individual PFAS detected in a single product (Tables S11 and S12). Fluorotelomer alcohols (FTOHs), methacrylates (FTMAs), and phosphate esters (PAPs) were the most frequently detected PFAS and also those contributing the most to total PFAS (Table S13). All of the collected products were used without homogenizing the entire mass or volume of the product before analysis. Differences in both the total fluorine concentrations from PIGE and targeted analyses results, which were not significantly correlated, suggests (1) numerous PFAS are not on the target list, (2) the presence of inorganic or polymeric fluorine, or (3) an effect due to the lack of homogenization or different shades/colors being chosen or all of the above.
Table 1. Summary of Total Fluorine Concentration (μg F/cm2) Measured by PIGE, Total PFAS Concentrations Measured with GC/MS and LC/MS/MS, and Number of Individual PFAS Detected in Each Sample from the 53 Compounds Targeted
U.S. Products
Sample IDPIGE (μg F/cm2)Sum of 53 PFAS concentrations (ng/g)Number of PFAS detected
Foundation 10.4661478
Foundation 25.8210,5006
Foundation 34.2086011
Lips 15.7444513
Lips 2<0.12715609
Lips 31.722637
Lips 4<0.1272167
Mascara 16.428948
Mascara 2<0.1275684
Mascara 3<0.1273184
Mascara 42.972646
Mascara 53.972156
Canadian products
Sample IDPIGE (μg F/cm2)Sum of 53 PFAS concentrations (ng/g)Number of PFAS detected
Foundation 10.8957010
Foundation 25.877713
Foundation 37.07193012
Foundation 42.32100010
Lips 19.912157
Lips 2<0.127110013
Lips 33.76382011
Lips 4<0.38416109
Lips 51.162358
Lips 634.4309010
Mascara 2<0.1278810
Mascara 3<0.127986
Mascara 412.71929
Mascara 59.17958
Mascara 621.716110
Mascara 7<0.1273656
Mascara 83.03227
The 6:2 species of these groups were the most commonly detected. Here, 6:2 FTOH was detected at a frequency of 100% and 94%, and 6:2 FTMA was detected at a frequency of 100% and 82%, in U.S. and Canadian products, respectively. The 6:2 monoPAP was detected at a frequency of 58% and 71% in U.S. and Canadian products, respectively. The high frequency of the 6:2 species presumably illustrates the overall industrial shift from longer chains, 8:2 and 10:2 PFAS, to shorter-chain variants in the market. (26) However, 8:2 FTOH, 8:2 FTMA, and 8:2 monoPAP were commonly found in U.S. and Canadian products signaling the continued use of or carryover contamination of longer-chain PFAS. Previous work on the biodegradation in mammals of both 8:2 FTOH and 6:2 FTOH has found that a fraction of FTOHs can undergo a series of metabolic transformations that result in the formation of terminal PFCAs, including perfluoropentanoic acid (PFPeA), perfluorohexanoic acid (PFHxA), and perfluoroheptanoic acid (PFHpA), as well as longer-chain PFAS such as PFOA (in the case of 8:2 and longer FTOHs). (26,27) Meta-analyses point to high toxicity and potentially bioaccumulative properties of some metabolites of 6:2 and 8:2 FTOHs. (28,29) Of the samples subjected to targeted analyses, PFPeA was detected in 33% and 35% of the U.S. and Canadian products, respectively. The concentrations of PFCAs detected were substantially lower than those of FTOHs, PAPs, and FTMAcs.
The measurement of both PAPs and PFCAs in these samples agrees with previous studies. Fujii et al. (6) hypothesized that the measured levels of PFCAs in products in the Republic of Korea and Japan were attributed to PAPs disclosed on the products’ ingredient lists. Measurement of PFCAs was expected to be from the use of PAPs, either as carryover contamination from their manufacturing or as degradation products since PAPs are formed from the condensation of FTOH with phosphate. (6,30) Brinch et al. (8) and Schultes et al. (7) generated similar results for PFCAs, and the latter identified various mono- and di-PAPs in 9 of the 31 products tested. Three foundations from ref (7) which disclosed PAPs on their ingredient labels reported concentrations of PAPs in the parts-per-million (μg/g) range. However, products that did not disclose a PAP had concentrations from 11.2 to 282 ng/g, similar to our reported values of 0.05–244 ng/g for various mono- and di-PAPs.
Another potential source of PFCAs is the FTMAc detected here in both high frequency and concentration. Here, 8:2 FTMAc can breakdown into 8:2 FTOH, leading to increases in measurable PFCA concentrations, as previously described. (26,31,32) We speculate that the high concentrations of FTOHs measured here are likely due to both the impurities, as well as the breakdown, of both FTMAcs and PAPs. High levels of these nonpolymeric PFAS in products applied to the skin are a cause of concern due to potentially serious health risks as described above. (28,29) Detection of FTMAcs in cosmetics is reported here for the first time. Their potential use in cosmetics as a film-forming agent was noted in 2018 by the CIR who reported insufficient data to enable an assessment of the safety of four FTMAc-based side-chain fluorinated polymers but that none of the cosmetic products surveyed were found to contain these four compounds. (33)

Comparison of Total Fluorine and Targeted Analyses to Ingredient Labeling

Only 8% of the 231 cosmetics screened for total fluorine had any PFAS listed as ingredients, and only 3% of the 29 cosmetics in which targeted PFAS were measured had any PFAS listed as ingredients. Thus, we compiled a list of ingredients to try to determine the likely ingredient(s) responsible for PFAS in the 12 U.S. products chosen for targeted analysis. A total of 166 ingredients were listed across all 12 cosmetic products with 37% of these ingredients being listed on multiple product’s ingredient lists. Tables S14–S16 provide the full lists of labeled ingredients and a heatmap relating ingredient frequency to total fluorine concentration from PIGE. Inorganic sources of fluorine found on ingredient labels included both natural and synthetic forms of minerals and clays used as bulking agents and/or colorants, such as synthetic fluorphlogopite and disteardimonium hectorite. Additional bulking agents and/or colorants include mica and talc, which are known to contain inorganic fluoride. As described by Fujii et al. (6) and in various patents filed by cosmetic manufacturers, both mica and talc can be treated with PAPs to provide hydrophobic properties that improve the durability and wear of applied cosmetics. (34,35) The same is true of other ingredients including silica, Nylon-12, and color additives.
Other potential sources of PFAS measured here include fluorinated versions of methicone and dimethicone, acrylate and methacrylate, and silicone polymers. (36−41) These ingredients can be purchased under trade names from chemical suppliers, for example, Fluorosil products from Siltech or Pecosil fluorinated products from Phoenix Chemical, Inc., among others. (23,25) We speculate that PFAS detected were from these ingredients described on the labels using only their generalized name, for example, methicone, acrylate. This interpretation is supported by documents suggesting that fluorinated ingredients and ingredients treated with PFAS were used in concentrations ranging from 0.1%–6.5% of the total cosmetic product weight. (34,35,41) These concentrations are similar to the highest concentrations of the total fluorine measured here.
The measurements of high total fluorine concentrations in a variety of cosmetic products in combination with the detection of several PFAS classes using targeted analysis indicate widespread use of fluorinated ingredients in cosmetics. Of particular concern are the high levels of 6:2 and 8:2 FTOHs, which are precursors to PFCAs that are known to be environmentally mobile and can cause adverse effects in both humans and the environment. Results from the analyses of ingredient labels confirm that the use of fluorinated ingredients is poorly disclosed and contributes to the difficulty in estimating the magnitude of PFAS use in cosmetics. These estimates are important for understanding the kinds and amounts of PFAS in relation to direct human exposure during product use. For example, PFAS could be ingested when lipstick containing PFAS is inadvertently ingested, and some PFAS in mascara could be absorbed through tear ducts. Without requirements for labeling, consumers cannot choose to avoid such exposures to PFAS in products they purchase. The use of PFAS in products also contributes to human and ecosystem exposures throughout the lifecycle of the product from PFAS manufacturing to product end of life. Cosmetic use contributes to PFAS entering wastewater streams leading to environmental accumulation of PFAS. This can lead to additional human exposure.
The high detection frequency found by PIGE and concentrations of PFAS measured by targeted analyses in this study suggest the need for better government oversight of PFAS, including the labeling of all cosmetic products containing these chemicals. Furthermore, given the considerable potential for human and ecosystem exposure and health harm, we question the use of any member of the highly persistent, potentially toxic, and very large class of PFAS in cosmetics. Better labeling and government oversight of harmful chemicals in personal care products are needed.

Supporting Information

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.estlett.1c00240.

  • Additional details and parameters used for the instrumental analyses, including PIGE analysis and targeted LC-MS/MS and GC-MS analyses. List of categories used to categorize the cosmetics analyzed, as well as a list of cosmetic brands sampled. Full results of targeted LC-MS/MS and GC-MS analyses, as well as a summary of various features of the total fluorine analyses. Detection frequencies of various PFAS classes for targeted analysis. Summary of label information for all ingredients used in the targeted products. (PDF)

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Author Information

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  • Corresponding Author
  • Authors
    • Heather D. Whitehead - Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, United States
    • Marta Venier - O’Neill School of Public and Environmental Affairs, Indiana University, Bloomington, Indiana 47405, United States;  Orcidhttps://orcid.org/0000-0002-2089-8992
    • Yan Wu - O’Neill School of Public and Environmental Affairs, Indiana University, Bloomington, Indiana 47405, United States;  Orcidhttps://orcid.org/0000-0001-7876-261X
    • Emi Eastman - Department of Physics, University of Notre Dame, Notre Dame, Indiana 46556, United States
    • Shannon Urbanik - Department of Chemistry, Hope College, Holland, Michigan 49423, United States
    • Miriam L. Diamond - Department of Earth Sciences, University of Toronto, Toronto, Ontario M5S 3B1, Canada;  Orcidhttps://orcid.org/0000-0001-6296-6431
    • Anna Shalin - Department of Earth Sciences, University of Toronto, Toronto, Ontario M5S 3B1, Canada
    • Heather Schwartz-Narbonne - Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6, Canada;  Orcidhttps://orcid.org/0000-0003-4776-0974
    • Thomas A. Bruton - Green Science Policy Institute, Berkeley, California 94709, Canada
    • Arlene Blum - Green Science Policy Institute, Berkeley, California 94709, Canada
    • Zhanyun Wang - Institute of Environmental Engineering, ETH Zürich, 8093 Zürich, Switzerland;  Orcidhttps://orcid.org/0000-0001-9914-7659
    • Megan Green - Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, United States
    • Meghanne Tighe - Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, United States;  Orcidhttps://orcid.org/0000-0002-8930-892X
    • John T. Wilkinson - Department of Physics, University of Notre Dame, Notre Dame, Indiana 46556, United States
    • Sean McGuinness - Department of Physics, University of Notre Dame, Notre Dame, Indiana 46556, United States
  • Notes
    The authors declare no competing financial interest.

Acknowledgments

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Funding was provided by Environment and Climate Change Canada, Great Lakes Protection Initiative (GCXE21P039) and Natural Sciences and Engineering Research Council of Canada (NSERC, RGPIN-2017-06654). E. Eastman and S. Urbanik were funded through NSF-REU 1559848 and NSF-RUI 1306074. We gratefully acknowledge Jerome Gan Shih Yi at the University of Notre Dame who assisted with collection and preparation of cosmetic samples for PIGE analysis collected in 2020.

References

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    Perfluoroalkyl and polyfluoroalkyl substances (PFAS) are used in a wide range of products of all day life. Due to their toxicol. potential, an emerging focus is directed towards their exposure to humans. This study investigated the PFAS load of consumer products in a broad perspective. Perfluoroalkyl sulfonic acids (C4, C6-C8, C10-PFSA), carboxylic acids (C4-C14-PFCA) and fluorotelomer alcs. (4:2, 6:2; 8:2 and 10:2 FTOH) were analyzed in 115 random samples of consumer products including textiles (outdoor materials), carpets, cleaning and impregnating agents, leather samples, baking and sandwich papers, paper baking forms and ski waxes. PFCA and PFSA were analyzed by HPLC-MS/MS, whereas FTOH were detected by GC/CI-MS. Consumer products such as cleaning agents or some baking and sandwich papers show low or negligible PFSA and PFCA contents. On the other hand, high PFAS levels were identified in ski waxes (up to about 2000 μg/kg PFOA), leather samples (up to about 200 μg/kg PFBA and 120 μg/kg PFBS), outdoor textiles (up to 19 μg/m2 PFOA) and some other baking papers (up to 15 μg/m2 PFOA). Moreover, some test samples like carpet and leather samples and outdoor materials exceeded the EU regulatory threshold value for PFOS (1 μg/m2). A diverse mixt. of PFASs can be found in consumer products for all fields of daily use in varying concns. This study proves the importance of screening and monitoring of consumer products for PFAS loads and the necessity for an action to regulate the use of PFASs, esp. PFOA, in consumer products.
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    Herzke, D.; Olsson, E.; Posner, S. Perfluoroalkyl and polyfluoroalkyl substances (PFASs) in consumer products in Norway - A pilot study. Chemosphere 2012, 88 (8), 980– 987,  DOI: 10.1016/j.chemosphere.2012.03.035
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    Perfluoroalkyl and polyfluoroalkyl substances (PFASs) in consumer products in Norway - A pilot study
    Herzke, Dorte; Olsson, Elisabeth; Posner, Stefan
    Chemosphere (2012), 88 (8), 980-987CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
    Perfluoroalkyl and polyfluoroalkyl substances (PFAS) are used in numerous industrial and consumer products because of their special chem. properties, for instance the ability to repel both water and oil. A broad variety of PFAS have been introduced into the Norwegian market through industrial use (e.g. via fire fighting foams and paints) as well as in treated customer products such as textiles and coated paper. Our present knowledge of the exact chem. PFAS compns. in prepns. using perfluorinated compds. is limited. This lack of knowledge means that it is difficult to provide an accurate assessment of human exposure to these compds. or to the amt. of waste that may contain treated products. It is a growing concern that these potentially harmful compds. can now be found throughout the global environment. Samples of consumer products and prepns. were collected in Norway, with supplemental samples from Sweden. In 27 of the 30 analyzed consumer products and prepns. a no. of polyfluorinated substances that were analyzed were detected but this does not exclude the occurrence of unknown PFAS. Notable was that perfluorooctanesulfonate (PFOS), which has been strictly regulated in Norway since 2007, was found in amts. close to or exceeding the EU regulatory level in 4 of the 30 analyzed products, all within the leather or carpet product groups. High amts. of fluorotelomer alcs. (FTOHs) were found in waterproofing agents, carpets and textiles, consistent with earlier findings by Fiedler et al. (2010). The presence of PFAS in a broad range of consumer products can give rise to a const. diffuse human exposure that might eventually result in harm to humans.
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  4. 4
    Sunderland, E. M.; Hu, X. C.; Dassuncao, C.; Tokranov, A. K.; Wagner, C. C.; Allen, J. G. A Review of the Pathways of Human Exposure to Poly- and Perfluoroalkyl Substances (PFASs) and Present Understanding of Health Effects. J. Exposure Sci. Environ. Epidemiol. 2019, 29, 131– 147,  DOI: 10.1038/s41370-018-0094-1
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    A review of the pathways of human exposure to poly- and perfluoroalkyl substances (PFASs) and present understanding of health effects
    Sunderland, Elsie M.; Hu, Xindi C.; Dassuncao, Clifton; Tokranov, Andrea K.; Wagner, Charlotte C.; Allen, Joseph G.
    Journal of Exposure Science & Environmental Epidemiology (2019), 29 (2), 131-147CODEN: JESEBS; ISSN:1559-0631. (Nature Research)
    A review. Here, we review present understanding of sources and trends in human exposure to poly- and perfluoroalkyl substances (PFASs) and epidemiol. evidence for impacts on cancer, immune function, metabolic outcomes, and neurodevelopment. More than 4000 PFASs have been manufd. by humans and hundreds have been detected in environmental samples. Direct exposures due to use in products can be quickly phased out by shifts in chem. prodn. but exposures driven by PFAS accumulation in the ocean and marine food chains and contamination of groundwater persist over long timescales. Serum concns. of legacy PFASs in humans are declining globally but total exposures to newer PFASs and precursor compds. have not been well characterized. Human exposures to legacy PFASs from seafood and drinking water are stable or increasing in many regions, suggesting obsd. declines reflect phase-outs in legacy PFAS use in consumer products. Many regions globally are continuing to discover PFAS contaminated sites from aq. film forming foam (AFFF) use, particularly next to airports and military bases. Exposures from food packaging and indoor environments are uncertain due to a rapidly changing chem. landscape where legacy PFASs have been replaced by diverse precursors and custom mols. that are difficult to detect. Multiple studies find significant assocns. between PFAS exposure and adverse immune outcomes in children. Dyslipidemia is the strongest metabolic outcome assocd. with PFAS exposure. Evidence for cancer is limited to manufg. locations with extremely high exposures and insufficient data are available to characterize impacts of PFAS exposures on neurodevelopment. Preliminary evidence suggests significant health effects assocd. with exposures to emerging PFASs. Lessons learned from legacy PFASs indicate that limited data should not be used as a justification to delay risk mitigation actions for replacement PFASs.
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    Beauty and Personal Care in North America, July 3, 2020 ed.; Euromonitor International, 2020.
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    Fujii, Y.; Harada, K. H.; Koizumi, A. Occurrence of perfluorinated carboxylic acids (PFCAs) in personal care products and compounding agents. Chemosphere 2013, 93 (3), 538– 544,  DOI: 10.1016/j.chemosphere.2013.06.049
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    Occurrence of perfluorinated carboxylic acids (PFCAs) in personal care products and compounding agents
    Fujii, Yukiko; Harada, Kouji H.; Koizumi, Akio
    Chemosphere (2013), 93 (3), 538-544CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
    Perfluorinated carboxylic acids (PFCAs), including perfluorooctanoic acid (PFOA), are persistent org. pollutants that pose human health risks. However, sources of contamination and exposure pathways of PFCAs were not explored. In this study, PFCA concns. were quantified in personal care products. Among 24 samples that listed fluorinated compds., such as polyfluoroalkyl phosphate esters (PAPs), in their international nomenclature of cosmetic ingredients (INCI) labels, 21 contained PFCAs (13 of 15 cosmetic samples, and 8 of 9 sunscreen samples). The concns. of total PFCAs ranged from not detected to 5.9 μg g-1 for cosmetics and from not detected to 19 μg g-1 for sunscreens. We also investigated components of PFCAs in cosmetics and sunscreens. Com. available compounding agents, mica and talc, which were treated with PAPs were analyzed and high concns. of PFCAs were detected (total PFCAs 2.5 μg g-1 for talc treated with PAPs, 35.0 μg g-1 for mica treated with PAPs). To the best of our knowledge, this is the 1st report on contamination of end consumer products contg. PAPs with high concns. of PFCAs.
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    Schultes, L.; Vestergren, R.; Volkova, K.; Westberg, E.; Jacobson, T.; Benskin, J. P. Per- and polyfluoroalkyl substances and fluorine mass balance in cosmetic products from the Swedish market: Implications for environmental emissions and human exposure. Environmental Science: Processes and Impacts 2018, 20 (12), 1680– 1690,  DOI: 10.1039/C8EM00368H
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    Per- and polyfluoroalkyl substances and fluorine mass balance in cosmetic products from the Swedish market: implications for environmental emissions and human exposure
    Schultes, Lara; Vestergren, Robin; Volkova, Kristina; Westberg, Emelie; Jacobson, Therese; Benskin, Jonathan P.
    Environmental Science: Processes & Impacts (2018), 20 (12), 1680-1690CODEN: ESPICZ; ISSN:2050-7895. (Royal Society of Chemistry)
    Per-and polyfluoroalkyl substances (PFASs) are a diverse class of < 4700 chems. used in com. products and industrial processes. Concerns surrounding PFASs are principally due to their widespread occurrence in humans and the environment and links to adverse health effects. One of the lesser known uses for PFASs is in cosmetic products (CPs) which come into contact with the skin (e.g. hair products, powders, sunblocks, etc.). In the present work, thirty-one CPs from five product categories (cream, foundation, pencil, powder and shaving foam) were analyzed for 39 PFASs by liq. chromatog.-tandem mass spectrometry, as well as extractable org. fluorine (EOF) and total fluorine (TF) by combustion ion chromatog. (CIC). This multi-platform approach enabled detn. of the fraction of fluorine accounted for by known PFASs (i.e. fluorine mass balance). Foundations and powders contained 25 different PFASs with the most frequently detected being perfluorinated carboxylic acids (perfluoroheptanoic acid and perfluorohexanoic acid) and polyfluoroalkyl phosphate esters (PAPs). U+03C314PAP concns. up to 470μg g-1 were measured in products listing mixts. of PAPs as an ingredient. For all samples, U+03C3 39PFAS concns. only explained a small fraction of the EOF and TF, pointing to the presence of unknown org. and/or inorg. fluorinated substances, including polymers. While creams, pencil and shaving foams did not contain measurable concns. of any of the 39 PFASs targeted here, CIC revealed high to moderate TF content. Overall, these data highlight the need for further investigations into the occurrence of PFASs in CPs and their importance with regards to human and environmental exposure.
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    Brinch, A.; Jensen, A. A.; Christensen, F. Risk Assessment of Fluorinated Substances in Cosmetic Products; Danish Environmental Protection Agency, 2018; pp 1– 116.
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    Glüge, J.; Scheringer, M.; Cousins, I. T.; DeWitt, J. C.; Goldenman, G.; Herzke, D.; Lohmann, R.; Ng, C. A.; Trier, X.; Wang, Z. An overview of the uses of per- and polyfluoroalkyl substances (PFAS). Environmental Science: Processes & Impacts 2020, 22, 2345– 2373,  DOI: 10.1039/D0EM00291G
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    International Cosmetic Ingredient Dictionary and Handbook, 16th ed.; Personal Care Products Council: Washington, DC, 2016; Vol. 1.
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    International Cosmetic Ingredient Nomenclature Committee (INC). https://www.personalcarecouncil.org/resources/inci/background-information/international-cosmetic-ingredient-nomenclature-committee-inc/ (accessed Jan 22, 2021).
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    Benotti, M. J.; Fernandez, L. A.; Peaslee, G. F.; Douglas, G. S.; Uhler, A. D.; Emsbo-Mattingly, S. A forensic approach for distinguishing PFAS materials. Environ. Forensics 2020, 21, 319– 333,  DOI: 10.1080/15275922.2020.1771631
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    A forensic approach for distinguishing PFAS materials
    Benotti, Mark J.; Fernandez, Loretta A.; Peaslee, Graham F.; Douglas, Gregory S.; Uhler, Allen D.; Emsbo-Mattingly, Stephen
    Environmental Forensics (2020), 21 (3-4), 319-333CODEN: EFNOAI; ISSN:1527-5922. (Taylor & Francis, Inc.)
    The widespread detection of per- and polyfluoroalkyl substances (PFAS) throughout the world and the ongoing proliferation of environmental regulations has prompted the need for a forensic approach for the source attribution of PFAS. Current LC-MS/MS std. methods are sensitive and robust, but only characterize a small fraction of the total potential PFAS signature. Other, more powerful anal. tools such as HRMS exist, and have been used to characterize some of the unknown or "non-target" fraction of PFAS, but these methods are expensive and not widely available. This paper presents a tiered approach to PFAS forensics based on std. methods and/or other relatively inexpensive methodologies. The approach outlined herein is broken into three tiers, including (1) a screening method to assess the general characteristics of the bulk PFAS signature; (2) a std. method to sensitively measure PFAS compds. of regulatory interest; and (3) a method for resolving the isomer patterns of select PFAS compds. The combination of these readily accessible methods is illustrated herein with different source materials, including aq. film forming foam (AFFF) conc. samples and food contact materials (FCMs). The tiered PFAS forensic approach bridges the gap between ground breaking academic methods and prodn. lab. throughput for the purpose of identifying valuable forensic information available in PFAS source materials.
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    Peaslee, G. F.; Wilkinson, J. T.; McGuinness, S. R.; Tighe, M.; Caterisano, N.; Lee, S.; Gonzales, A.; Roddy, M.; Mills, S.; Mitchell, K. Another Pathway for Firefighter Exposure to Per- and Polyfluoroalkyl Substances: Firefighter Textiles. Environ. Sci. Technol. Lett. 2020, 7, 594– 599,  DOI: 10.1021/acs.estlett.0c00410
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    Another Pathway for Firefighter Exposure to Per- and Polyfluoroalkyl Substances: Firefighter Textiles
    Peaslee, Graham F.; Wilkinson, John T.; McGuinness, Sean R.; Tighe, Meghanne; Caterisano, Nicholas; Lee, Seryeong; Gonzales, Alec; Roddy, Matthew; Mills, Simon; Mitchell, Krystle
    Environmental Science & Technology Letters (2020), 7 (8), 594-599CODEN: ESTLCU; ISSN:2328-8930. (American Chemical Society)
    Occupational exposure to aq. film-forming foams (AFFF) can lead to elevated concns. of per- and polyfluorinated alkyl substances (PFAS) in firefighter blood sera. AFFF are also one PFAS exposure source in the general population due to their environmental persistence and soly. in groundwater. Due to documented PFAS adverse health effects, the primary concern to date for the fire services centered on repeated AFFF use and exposure. This work presents an addnl. PFAS exposure source for firefighters: PFAS shed from their protective clothing. Textiles in firefighter turn-out gear had high total F concns. (up to 2%); individual PFAS were identified and measured on new and used firefighting turn-out gear. Used gear showed lower PFAS concn. and increased migration to untreated material. Textile storage area dust measurements also suggested direct loss of PFAS from the textile fluoropolymers. Since PFAS shed from turn-out gear textiles are more mobile, they represent another exposure source for firefighters which warrants addnl. study.
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    Schaider, L. A.; Balan, S. A.; Blum, A.; Andrews, D. Q.; Strynar, M. J.; Dickinson, M. E.; Lunderberg, D. M.; Lang, J. R.; Peaslee, G. F. Fluorinated Compounds in U.S. Fast Food Packaging. Environ. Sci. Technol. Lett. 2017, 4 (3), 105– 111,  DOI: 10.1021/acs.estlett.6b00435
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    Fluorinated Compounds in U.S. Fast Food Packaging
    Schaider, Laurel A.; Balan, Simona A.; Blum, Arlene; Andrews, David Q.; Strynar, Mark J.; Dickinson, Margaret E.; Lunderberg, David M.; Lang, Johnsie R.; Peaslee, Graham F.
    Environmental Science & Technology Letters (2017), 4 (3), 105-111CODEN: ESTLCU; ISSN:2328-8930. (American Chemical Society)
    Per- and polyfluoroalkyl substances (PFASs) are highly persistent synthetic chems., some of which have been assocd. with cancer, developmental toxicity, immunotoxicity, and other health effects. PFASs in grease-resistant food packaging can leach into food and increase dietary exposure. We collected ∼400 samples of food contact papers, paperboard containers, and beverage containers from fast food restaurants throughout the U.S. and measured total fluorine using Particle-Induced Gamma-ray Emission (PIGE) spectroscopy. PIGE can rapidly and inexpensively measure total fluorine in solid-phase samples. We found that 46% of food contact papers and 20% of paperboard samples contained detectable fluorine (>16 nmol/cm2). Liq. chromatog./high-resoln. mass spectrometry anal. on a subset of 20 samples found perfluorocarboxylates, perfluorosulfonates, and other known PFASs and/or unidentified polyfluorinated compds. (based on nontargeted anal.). Total peak area for PFASs was higher in 70% of samples (10 of 14) with total fluorine >200 nmol/cm2 compared to six samples with total fluorine <16 nmol/cm2. Samples with high total fluorine but low levels of measured PFASs may contain volatile PFASs, PFAS polymers, newer replacement PFASs, or other fluorinated compds. The prevalence of fluorinated chems. in fast food packaging demonstrates their potentially significant contribution to dietary PFAS exposure and environmental contamination during prodn. and disposal.
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    Wu, Y.; Romanak, K.; Bruton, T.; Blum, A.; Venier, M. Per- and polyfluoroalkyl substances in paired dust and carpets from childcare centers. Chemosphere 2020, 251, 126771,  DOI: 10.1016/j.chemosphere.2020.126771
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    Per- and polyfluoroalkyl substances in paired dust and carpets from childcare centers
    Wu, Yan; Romanak, Kevin; Bruton, Tom; Blum, Arlene; Venier, Marta
    Chemosphere (2020), 251 (), 126771CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
    Carpets can be a significant source of per- and polyfluoroalkyl substances (PFASs) in the indoor environment and may be an esp. important source of exposure for children and toddlers. Most previous studies focused on measuring indoor dust only. In this study, we measured PFAS concns. in paired carpet and dust samples from 18 California childcare centers in 2018 to investigate carpet as a contributor to PFASs in dust. Median total PFAS concns. (.sum.PFASs) in carpets and dust were 471 ng/g and 523 ng/g, resp. 6:2 FTOH and 6:2 FTSA were the two dominant PFASs, collectively accounting for over 50% of the .sum.PFASs in both media. Other frequently detected PFASs included C4-C14 perfluoroalkylcarboxylic acids, C4-C8 perfluoroalkylsulfonic acids, PFDS, 4:2 FTSA, 8:2 FTSA, FOSA, MeFOSE, EtFOSE, 8:2 FTOH, and 10:2 FTOH. We found strong assocns. between PFAS levels in carpet and dust pairs, suggesting that carpets can be a source and a sink for PFASs. The estd. total perfluoroalkyl acids (PFAA) intake via dust ingestion for children was 0.023, 0.096, and 1.9 ng/kg body wt./day in the low-, intermediate-, and high-exposure scenarios, resp. Our data suggest that PFASs of emerging concern are playing an increasingly important role in indoor exposure to PFASs.
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    Bui, H. S.; Coleman-Nally, D. Film-Forming Technology and Skin Adhesion in Long-Wear Cosmetics. Adhesion in Pharmaceutical, Biomedical and Dental Fields 2017, 141– 166,  DOI: 10.1002/9781119323716.ch7
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    Film-forming technology and skin adhesion in long-wear cosmetics
    Bui, Hy Si; Coleman-Nally, Debra
    Adhesion in Pharmaceutical, Biomedical and Dental Fields (2017), (), 141-166CODEN: 69XADJ ISSN:. (John Wiley & Sons, Inc.)
    It is desirable to formulate cosmetic and personal care products with film-forming agents, due to their inherent ability to adhere well to the skin surface. Addnl., they aid in application, wear and non-transfer properties of a product. However, film- forming agents can be taut and/or tacky on the skin, resulting in discomfort and consumer dissatisfaction. Therefore, balancing adhesion and comfort on the skin is imperative in developing a product, but it is also a tech. challenge. This chapter reviews current polymeric film-forming systems, such as silicone resins and silicone film- formers that are used in cosmetic formulations to obtain optimal product performance.
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    Richard, C. Lipstick Adhesion Measurement. Surface Science and Adhesion in Cosmetics 2021, 635– 662,  DOI: 10.1002/9781119654926.ch18
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    Pawar, A. B.; Falk, B. Use of Advanced Silicone Materials in Long-Lasting Cosmetics. Surface Science and Adhesion in Cosmetics 2021, 151– 182,  DOI: 10.1002/9781119654926.ch5
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    Lam, H. Factors Enhancing Adhesion of Color Cosmetic Products to Skin: The Role of Pigments and Fillers. Surface Science and Adhesion in Cosmetics 2021, 487– 541,  DOI: 10.1002/9781119654926.ch15
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    Butt, C. M.; Muir, D. C. G.; Mabury, S. A. Biotransformation pathways of fluorotelomer-based polyfluoroalkyl substances: A review. Environ. Toxicol. Chem. 2014, 33 (2), 243– 267,  DOI: 10.1002/etc.2407
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    Biotransformation pathways of fluorotelomer-based polyfluoroalkyl substances: A review
    Butt, Craig M.; Muir, Derek C. G.; Mabury, Scott A.
    Environmental Toxicology and Chemistry (2014), 33 (2), 243-267CODEN: ETOCDK; ISSN:0730-7268. (Wiley-Blackwell)
    A review. The study reviews the current state of knowledge regarding the biotransformation of fluorotelomer-based compds., with a focus on compds. that ultimately degrade to form perfluoroalkyl carboxylates (PFCAs). Most metab. studies have been performed with either microbial systems or rats and mice, and comparatively few studies have used fish models. Furthermore, biotransformation studies thus far have predominately used the 8:2 fluorotelomer alc. (FTOH) as the substrate. However, there have been an increasing no. of studies investigating 6:2 FTOH biotransformation as a result of industry's transition to shorter-chain fluorotelomer chem. Studies with the 8:2 FTOH metab. universally show the formation of perfluorooctanoate (PFOA) and, to a smaller fraction, perfluorononanoate (PFNA) and lower-chain-length PFCAs. In general, the overall yield of PFOA is low, presumably because of the multiple branches in the biotransformation pathways, including conjugation reactions in animal systems. There have been a few studies of non-FTOH biotransformation, which include polyfluoroalkyl phosphates (PAPs), 8:2 fluorotelomer acrylate (8:2 FTAC), and fluorotelomer carboxylates (FTCAs, FTUCAs). The PAPs compds. and 8:2 FTAC were shown to be direct precursors to FTOHs and thus follow similar degrdn. pathways. Environ Toxicol Chem 2014;33:243-267. © 2013 SETAC.
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    Kabadi, S. V.; Fisher, J.; Aungst, J.; Rice, P. Internal exposure-based pharmacokinetic evaluation of potential for biopersistence of 6:2 fluorotelomer alcohol (FTOH) and its metabolites. Food Chem. Toxicol. 2018, 112, 375– 382,  DOI: 10.1016/j.fct.2018.01.012
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    Internal exposure-based pharmacokinetic evaluation of potential for biopersistence of 6:2 fluorotelomer alcohol (FTOH) and its metabolites
    Kabadi, Shruti V.; Fisher, Jeffrey; Aungst, Jason; Rice, Penelope
    Food and Chemical Toxicology (2018), 112 (), 375-382CODEN: FCTOD7; ISSN:0278-6915. (Elsevier Ltd.)
    Polyfluorinated compds. (PFCs) are authorized for use as greaseproofing agents in food contact paper. As C8-PFCs (8-carbons) are known to accumulate in tissues, shorter-chain C6-PFCs (6-carbons) have replaced C8-PFCs in many food contact applications. However, the potential of C6-PFCs for human biopersistence has not been fully evaluated. For the first time, we provide internal exposure ests. to key metabolites of 6:2 fluorotelomer alc. (6:2 FTOH), a monomeric component of C6-PFCs, to extend our understanding of exposure beyond ests. of external exposure. Pharmacokinetic data from published rat and human studies on 6:2 FTOH were used to est. clearance and area under the curve (AUC) for its metabolites: 5:3 fluorotelomer carboxylic acid (5:3 A), perfluorohexanoic acid (PFHxA) and perfluoroheptanoic acid (PFHpA). Internal exposure to 5:3 A was the highest of evaluated metabolites across species and it had the slowest clearance. Addnl., 5:3 A clearance decreased with increasing 6:2 FTOH exposure. Our anal. provides insight into assocn. of increased internal 5:3 A exposure with high biopersistence potential of 6:2 FTOH. Our results identify 5:3 A as an important biomarker of internal 6:2 FTOH exposure for use in biomonitoring studies, and are potentially useful for toxicol. assessment of chronic dietary 6:2 FTOH exposure.
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    Comparative analysis of the toxicological databases for 6:2 fluorotelomer alcohol (6:2 FTOH) and perfluorohexanoic acid (PFHxA)
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    Food and Chemical Toxicology (2020), 138 (), 111210CODEN: FCTOD7; ISSN:0278-6915. (Elsevier Ltd.)
    6:2 Fluorotelomer alc. (6:2 FTOH) is a short-chain polyfluoroalkyl substance (PFAS) in polymeric PFAS used in fast food packaging and stain- and water-resistant textiles and may be degrdn. products of some components of aq. film-forming foams (AFFF). The general population is exposed to 6:2 FTOH by inhalation of evaps. from treated surfaces or ambient concns. in air, ingestion of indoor dust, or ingestion of food packaged in materials contg. PFAS. Although exposure to 6:2 FTOH is pervasive, little is known concerning human health effects of this compd. Some published risk assessments have assumed that perfluorohexanoic acid (PFHxA), a metabolite of 6:2 FTOH, adequately models the human health effects of 6:2 FTOH. Recently identified studies conducted with 6:2 FTOH and its metabolite, 5:3 acid, have provided information that enables comparison of the toxicol. profiles of PFHxA and 6:2 FTOH. This article summarizes a comparative anal. of the toxicol. effects of PFHxA and 6:2 FTOH in rodents to det. whether data for PFHxA adequately models potential hazards of 6:2 FTOH exposure. Our anal. demonstrates that 6:2 FTOH is significantly more toxic than PFHxA. Use of toxicol. studies conducted with PFHxA to assess 6:2 FTOH exposure may significantly underestimate human health risk.
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  • Abstract

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    Figure 1

    Figure 1. Foundations produced the highest median total fluorine (μg F/cm2) in 231 products groups across eight categories. Breakdown of the number of products tested in each of the eight products categories and proportion of items in each category that was categorized as high, moderate, and low total fluorine concentrations. Several mascaras gave the highest fluorine concentrations measured. All remaining categories produced similar medians but with varying ranges. The three cosmetic categories that had the highest proportion of high fluorine concentrations were foundations, mascaras, and lip products.

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  • References

    This article references 41 other publications.

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      Perfluoroalkyl and polyfluoroalkyl substances (PFAS) are used in a wide range of products of all day life. Due to their toxicol. potential, an emerging focus is directed towards their exposure to humans. This study investigated the PFAS load of consumer products in a broad perspective. Perfluoroalkyl sulfonic acids (C4, C6-C8, C10-PFSA), carboxylic acids (C4-C14-PFCA) and fluorotelomer alcs. (4:2, 6:2; 8:2 and 10:2 FTOH) were analyzed in 115 random samples of consumer products including textiles (outdoor materials), carpets, cleaning and impregnating agents, leather samples, baking and sandwich papers, paper baking forms and ski waxes. PFCA and PFSA were analyzed by HPLC-MS/MS, whereas FTOH were detected by GC/CI-MS. Consumer products such as cleaning agents or some baking and sandwich papers show low or negligible PFSA and PFCA contents. On the other hand, high PFAS levels were identified in ski waxes (up to about 2000 μg/kg PFOA), leather samples (up to about 200 μg/kg PFBA and 120 μg/kg PFBS), outdoor textiles (up to 19 μg/m2 PFOA) and some other baking papers (up to 15 μg/m2 PFOA). Moreover, some test samples like carpet and leather samples and outdoor materials exceeded the EU regulatory threshold value for PFOS (1 μg/m2). A diverse mixt. of PFASs can be found in consumer products for all fields of daily use in varying concns. This study proves the importance of screening and monitoring of consumer products for PFAS loads and the necessity for an action to regulate the use of PFASs, esp. PFOA, in consumer products.
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      3
      Perfluoroalkyl and polyfluoroalkyl substances (PFASs) in consumer products in Norway - A pilot study
      Herzke, Dorte; Olsson, Elisabeth; Posner, Stefan
      Chemosphere (2012), 88 (8), 980-987CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
      Perfluoroalkyl and polyfluoroalkyl substances (PFAS) are used in numerous industrial and consumer products because of their special chem. properties, for instance the ability to repel both water and oil. A broad variety of PFAS have been introduced into the Norwegian market through industrial use (e.g. via fire fighting foams and paints) as well as in treated customer products such as textiles and coated paper. Our present knowledge of the exact chem. PFAS compns. in prepns. using perfluorinated compds. is limited. This lack of knowledge means that it is difficult to provide an accurate assessment of human exposure to these compds. or to the amt. of waste that may contain treated products. It is a growing concern that these potentially harmful compds. can now be found throughout the global environment. Samples of consumer products and prepns. were collected in Norway, with supplemental samples from Sweden. In 27 of the 30 analyzed consumer products and prepns. a no. of polyfluorinated substances that were analyzed were detected but this does not exclude the occurrence of unknown PFAS. Notable was that perfluorooctanesulfonate (PFOS), which has been strictly regulated in Norway since 2007, was found in amts. close to or exceeding the EU regulatory level in 4 of the 30 analyzed products, all within the leather or carpet product groups. High amts. of fluorotelomer alcs. (FTOHs) were found in waterproofing agents, carpets and textiles, consistent with earlier findings by Fiedler et al. (2010). The presence of PFAS in a broad range of consumer products can give rise to a const. diffuse human exposure that might eventually result in harm to humans.
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      4
      A review of the pathways of human exposure to poly- and perfluoroalkyl substances (PFASs) and present understanding of health effects
      Sunderland, Elsie M.; Hu, Xindi C.; Dassuncao, Clifton; Tokranov, Andrea K.; Wagner, Charlotte C.; Allen, Joseph G.
      Journal of Exposure Science & Environmental Epidemiology (2019), 29 (2), 131-147CODEN: JESEBS; ISSN:1559-0631. (Nature Research)
      A review. Here, we review present understanding of sources and trends in human exposure to poly- and perfluoroalkyl substances (PFASs) and epidemiol. evidence for impacts on cancer, immune function, metabolic outcomes, and neurodevelopment. More than 4000 PFASs have been manufd. by humans and hundreds have been detected in environmental samples. Direct exposures due to use in products can be quickly phased out by shifts in chem. prodn. but exposures driven by PFAS accumulation in the ocean and marine food chains and contamination of groundwater persist over long timescales. Serum concns. of legacy PFASs in humans are declining globally but total exposures to newer PFASs and precursor compds. have not been well characterized. Human exposures to legacy PFASs from seafood and drinking water are stable or increasing in many regions, suggesting obsd. declines reflect phase-outs in legacy PFAS use in consumer products. Many regions globally are continuing to discover PFAS contaminated sites from aq. film forming foam (AFFF) use, particularly next to airports and military bases. Exposures from food packaging and indoor environments are uncertain due to a rapidly changing chem. landscape where legacy PFASs have been replaced by diverse precursors and custom mols. that are difficult to detect. Multiple studies find significant assocns. between PFAS exposure and adverse immune outcomes in children. Dyslipidemia is the strongest metabolic outcome assocd. with PFAS exposure. Evidence for cancer is limited to manufg. locations with extremely high exposures and insufficient data are available to characterize impacts of PFAS exposures on neurodevelopment. Preliminary evidence suggests significant health effects assocd. with exposures to emerging PFASs. Lessons learned from legacy PFASs indicate that limited data should not be used as a justification to delay risk mitigation actions for replacement PFASs.
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      Fujii, Y.; Harada, K. H.; Koizumi, A. Occurrence of perfluorinated carboxylic acids (PFCAs) in personal care products and compounding agents. Chemosphere 2013, 93 (3), 538– 544,  DOI: 10.1016/j.chemosphere.2013.06.049
      6
      Occurrence of perfluorinated carboxylic acids (PFCAs) in personal care products and compounding agents
      Fujii, Yukiko; Harada, Kouji H.; Koizumi, Akio
      Chemosphere (2013), 93 (3), 538-544CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
      Perfluorinated carboxylic acids (PFCAs), including perfluorooctanoic acid (PFOA), are persistent org. pollutants that pose human health risks. However, sources of contamination and exposure pathways of PFCAs were not explored. In this study, PFCA concns. were quantified in personal care products. Among 24 samples that listed fluorinated compds., such as polyfluoroalkyl phosphate esters (PAPs), in their international nomenclature of cosmetic ingredients (INCI) labels, 21 contained PFCAs (13 of 15 cosmetic samples, and 8 of 9 sunscreen samples). The concns. of total PFCAs ranged from not detected to 5.9 μg g-1 for cosmetics and from not detected to 19 μg g-1 for sunscreens. We also investigated components of PFCAs in cosmetics and sunscreens. Com. available compounding agents, mica and talc, which were treated with PAPs were analyzed and high concns. of PFCAs were detected (total PFCAs 2.5 μg g-1 for talc treated with PAPs, 35.0 μg g-1 for mica treated with PAPs). To the best of our knowledge, this is the 1st report on contamination of end consumer products contg. PAPs with high concns. of PFCAs.
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      7
      Per- and polyfluoroalkyl substances and fluorine mass balance in cosmetic products from the Swedish market: implications for environmental emissions and human exposure
      Schultes, Lara; Vestergren, Robin; Volkova, Kristina; Westberg, Emelie; Jacobson, Therese; Benskin, Jonathan P.
      Environmental Science: Processes & Impacts (2018), 20 (12), 1680-1690CODEN: ESPICZ; ISSN:2050-7895. (Royal Society of Chemistry)
      Per-and polyfluoroalkyl substances (PFASs) are a diverse class of < 4700 chems. used in com. products and industrial processes. Concerns surrounding PFASs are principally due to their widespread occurrence in humans and the environment and links to adverse health effects. One of the lesser known uses for PFASs is in cosmetic products (CPs) which come into contact with the skin (e.g. hair products, powders, sunblocks, etc.). In the present work, thirty-one CPs from five product categories (cream, foundation, pencil, powder and shaving foam) were analyzed for 39 PFASs by liq. chromatog.-tandem mass spectrometry, as well as extractable org. fluorine (EOF) and total fluorine (TF) by combustion ion chromatog. (CIC). This multi-platform approach enabled detn. of the fraction of fluorine accounted for by known PFASs (i.e. fluorine mass balance). Foundations and powders contained 25 different PFASs with the most frequently detected being perfluorinated carboxylic acids (perfluoroheptanoic acid and perfluorohexanoic acid) and polyfluoroalkyl phosphate esters (PAPs). U+03C314PAP concns. up to 470μg g-1 were measured in products listing mixts. of PAPs as an ingredient. For all samples, U+03C3 39PFAS concns. only explained a small fraction of the EOF and TF, pointing to the presence of unknown org. and/or inorg. fluorinated substances, including polymers. While creams, pencil and shaving foams did not contain measurable concns. of any of the 39 PFASs targeted here, CIC revealed high to moderate TF content. Overall, these data highlight the need for further investigations into the occurrence of PFASs in CPs and their importance with regards to human and environmental exposure.
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      There is no corresponding record for this reference.
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      Benotti, M. J.; Fernandez, L. A.; Peaslee, G. F.; Douglas, G. S.; Uhler, A. D.; Emsbo-Mattingly, S. A forensic approach for distinguishing PFAS materials. Environ. Forensics 2020, 21, 319– 333,  DOI: 10.1080/15275922.2020.1771631
      15
      A forensic approach for distinguishing PFAS materials
      Benotti, Mark J.; Fernandez, Loretta A.; Peaslee, Graham F.; Douglas, Gregory S.; Uhler, Allen D.; Emsbo-Mattingly, Stephen
      Environmental Forensics (2020), 21 (3-4), 319-333CODEN: EFNOAI; ISSN:1527-5922. (Taylor & Francis, Inc.)
      The widespread detection of per- and polyfluoroalkyl substances (PFAS) throughout the world and the ongoing proliferation of environmental regulations has prompted the need for a forensic approach for the source attribution of PFAS. Current LC-MS/MS std. methods are sensitive and robust, but only characterize a small fraction of the total potential PFAS signature. Other, more powerful anal. tools such as HRMS exist, and have been used to characterize some of the unknown or "non-target" fraction of PFAS, but these methods are expensive and not widely available. This paper presents a tiered approach to PFAS forensics based on std. methods and/or other relatively inexpensive methodologies. The approach outlined herein is broken into three tiers, including (1) a screening method to assess the general characteristics of the bulk PFAS signature; (2) a std. method to sensitively measure PFAS compds. of regulatory interest; and (3) a method for resolving the isomer patterns of select PFAS compds. The combination of these readily accessible methods is illustrated herein with different source materials, including aq. film forming foam (AFFF) conc. samples and food contact materials (FCMs). The tiered PFAS forensic approach bridges the gap between ground breaking academic methods and prodn. lab. throughput for the purpose of identifying valuable forensic information available in PFAS source materials.
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    16. 16
      Peaslee, G. F.; Wilkinson, J. T.; McGuinness, S. R.; Tighe, M.; Caterisano, N.; Lee, S.; Gonzales, A.; Roddy, M.; Mills, S.; Mitchell, K. Another Pathway for Firefighter Exposure to Per- and Polyfluoroalkyl Substances: Firefighter Textiles. Environ. Sci. Technol. Lett. 2020, 7, 594– 599,  DOI: 10.1021/acs.estlett.0c00410
      16
      Another Pathway for Firefighter Exposure to Per- and Polyfluoroalkyl Substances: Firefighter Textiles
      Peaslee, Graham F.; Wilkinson, John T.; McGuinness, Sean R.; Tighe, Meghanne; Caterisano, Nicholas; Lee, Seryeong; Gonzales, Alec; Roddy, Matthew; Mills, Simon; Mitchell, Krystle
      Environmental Science & Technology Letters (2020), 7 (8), 594-599CODEN: ESTLCU; ISSN:2328-8930. (American Chemical Society)
      Occupational exposure to aq. film-forming foams (AFFF) can lead to elevated concns. of per- and polyfluorinated alkyl substances (PFAS) in firefighter blood sera. AFFF are also one PFAS exposure source in the general population due to their environmental persistence and soly. in groundwater. Due to documented PFAS adverse health effects, the primary concern to date for the fire services centered on repeated AFFF use and exposure. This work presents an addnl. PFAS exposure source for firefighters: PFAS shed from their protective clothing. Textiles in firefighter turn-out gear had high total F concns. (up to 2%); individual PFAS were identified and measured on new and used firefighting turn-out gear. Used gear showed lower PFAS concn. and increased migration to untreated material. Textile storage area dust measurements also suggested direct loss of PFAS from the textile fluoropolymers. Since PFAS shed from turn-out gear textiles are more mobile, they represent another exposure source for firefighters which warrants addnl. study.
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    17. 17
      Schaider, L. A.; Balan, S. A.; Blum, A.; Andrews, D. Q.; Strynar, M. J.; Dickinson, M. E.; Lunderberg, D. M.; Lang, J. R.; Peaslee, G. F. Fluorinated Compounds in U.S. Fast Food Packaging. Environ. Sci. Technol. Lett. 2017, 4 (3), 105– 111,  DOI: 10.1021/acs.estlett.6b00435
      17
      Fluorinated Compounds in U.S. Fast Food Packaging
      Schaider, Laurel A.; Balan, Simona A.; Blum, Arlene; Andrews, David Q.; Strynar, Mark J.; Dickinson, Margaret E.; Lunderberg, David M.; Lang, Johnsie R.; Peaslee, Graham F.
      Environmental Science & Technology Letters (2017), 4 (3), 105-111CODEN: ESTLCU; ISSN:2328-8930. (American Chemical Society)
      Per- and polyfluoroalkyl substances (PFASs) are highly persistent synthetic chems., some of which have been assocd. with cancer, developmental toxicity, immunotoxicity, and other health effects. PFASs in grease-resistant food packaging can leach into food and increase dietary exposure. We collected ∼400 samples of food contact papers, paperboard containers, and beverage containers from fast food restaurants throughout the U.S. and measured total fluorine using Particle-Induced Gamma-ray Emission (PIGE) spectroscopy. PIGE can rapidly and inexpensively measure total fluorine in solid-phase samples. We found that 46% of food contact papers and 20% of paperboard samples contained detectable fluorine (>16 nmol/cm2). Liq. chromatog./high-resoln. mass spectrometry anal. on a subset of 20 samples found perfluorocarboxylates, perfluorosulfonates, and other known PFASs and/or unidentified polyfluorinated compds. (based on nontargeted anal.). Total peak area for PFASs was higher in 70% of samples (10 of 14) with total fluorine >200 nmol/cm2 compared to six samples with total fluorine <16 nmol/cm2. Samples with high total fluorine but low levels of measured PFASs may contain volatile PFASs, PFAS polymers, newer replacement PFASs, or other fluorinated compds. The prevalence of fluorinated chems. in fast food packaging demonstrates their potentially significant contribution to dietary PFAS exposure and environmental contamination during prodn. and disposal.
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    18. 18
      Wu, Y.; Romanak, K.; Bruton, T.; Blum, A.; Venier, M. Per- and polyfluoroalkyl substances in paired dust and carpets from childcare centers. Chemosphere 2020, 251, 126771,  DOI: 10.1016/j.chemosphere.2020.126771
      18
      Per- and polyfluoroalkyl substances in paired dust and carpets from childcare centers
      Wu, Yan; Romanak, Kevin; Bruton, Tom; Blum, Arlene; Venier, Marta
      Chemosphere (2020), 251 (), 126771CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
      Carpets can be a significant source of per- and polyfluoroalkyl substances (PFASs) in the indoor environment and may be an esp. important source of exposure for children and toddlers. Most previous studies focused on measuring indoor dust only. In this study, we measured PFAS concns. in paired carpet and dust samples from 18 California childcare centers in 2018 to investigate carpet as a contributor to PFASs in dust. Median total PFAS concns. (.sum.PFASs) in carpets and dust were 471 ng/g and 523 ng/g, resp. 6:2 FTOH and 6:2 FTSA were the two dominant PFASs, collectively accounting for over 50% of the .sum.PFASs in both media. Other frequently detected PFASs included C4-C14 perfluoroalkylcarboxylic acids, C4-C8 perfluoroalkylsulfonic acids, PFDS, 4:2 FTSA, 8:2 FTSA, FOSA, MeFOSE, EtFOSE, 8:2 FTOH, and 10:2 FTOH. We found strong assocns. between PFAS levels in carpet and dust pairs, suggesting that carpets can be a source and a sink for PFASs. The estd. total perfluoroalkyl acids (PFAA) intake via dust ingestion for children was 0.023, 0.096, and 1.9 ng/kg body wt./day in the low-, intermediate-, and high-exposure scenarios, resp. Our data suggest that PFASs of emerging concern are playing an increasingly important role in indoor exposure to PFASs.
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    19. 19
      Bui, H. S.; Coleman-Nally, D. Film-Forming Technology and Skin Adhesion in Long-Wear Cosmetics. Adhesion in Pharmaceutical, Biomedical and Dental Fields 2017, 141– 166,  DOI: 10.1002/9781119323716.ch7
      19
      Film-forming technology and skin adhesion in long-wear cosmetics
      Bui, Hy Si; Coleman-Nally, Debra
      Adhesion in Pharmaceutical, Biomedical and Dental Fields (2017), (), 141-166CODEN: 69XADJ ISSN:. (John Wiley & Sons, Inc.)
      It is desirable to formulate cosmetic and personal care products with film-forming agents, due to their inherent ability to adhere well to the skin surface. Addnl., they aid in application, wear and non-transfer properties of a product. However, film- forming agents can be taut and/or tacky on the skin, resulting in discomfort and consumer dissatisfaction. Therefore, balancing adhesion and comfort on the skin is imperative in developing a product, but it is also a tech. challenge. This chapter reviews current polymeric film-forming systems, such as silicone resins and silicone film- formers that are used in cosmetic formulations to obtain optimal product performance.
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    20. 20
      Richard, C. Lipstick Adhesion Measurement. Surface Science and Adhesion in Cosmetics 2021, 635– 662,  DOI: 10.1002/9781119654926.ch18
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      Pawar, A. B.; Falk, B. Use of Advanced Silicone Materials in Long-Lasting Cosmetics. Surface Science and Adhesion in Cosmetics 2021, 151– 182,  DOI: 10.1002/9781119654926.ch5
      There is no corresponding record for this reference.
    22. 22
      Lam, H. Factors Enhancing Adhesion of Color Cosmetic Products to Skin: The Role of Pigments and Fillers. Surface Science and Adhesion in Cosmetics 2021, 487– 541,  DOI: 10.1002/9781119654926.ch15
      There is no corresponding record for this reference.
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      Phoenix Chemical Product Catalog 2019. https://phoenix-chem.com/catalogs-brochures/phoenixs-product-catalog/ (accessed Jan 22, 2021).
      There is no corresponding record for this reference.
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      SPE Cosmetics and Personal Care Product Catalogue 2020. https://www.spe-cosmetics.com/media/spe-web-12-2020.pdf (accessed Jan 22, 2021).
      There is no corresponding record for this reference.
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      Siltech Innovative Silicones for the Personal Care Industry. https://www.siltech.com/wp-content/uploads/2017/11/Personal_Care_Products.pdf (acessed Jan 22, 2021).
      There is no corresponding record for this reference.
    26. 26
      Butt, C. M.; Muir, D. C. G.; Mabury, S. A. Biotransformation pathways of fluorotelomer-based polyfluoroalkyl substances: A review. Environ. Toxicol. Chem. 2014, 33 (2), 243– 267,  DOI: 10.1002/etc.2407
      26
      Biotransformation pathways of fluorotelomer-based polyfluoroalkyl substances: A review
      Butt, Craig M.; Muir, Derek C. G.; Mabury, Scott A.
      Environmental Toxicology and Chemistry (2014), 33 (2), 243-267CODEN: ETOCDK; ISSN:0730-7268. (Wiley-Blackwell)
      A review. The study reviews the current state of knowledge regarding the biotransformation of fluorotelomer-based compds., with a focus on compds. that ultimately degrade to form perfluoroalkyl carboxylates (PFCAs). Most metab. studies have been performed with either microbial systems or rats and mice, and comparatively few studies have used fish models. Furthermore, biotransformation studies thus far have predominately used the 8:2 fluorotelomer alc. (FTOH) as the substrate. However, there have been an increasing no. of studies investigating 6:2 FTOH biotransformation as a result of industry's transition to shorter-chain fluorotelomer chem. Studies with the 8:2 FTOH metab. universally show the formation of perfluorooctanoate (PFOA) and, to a smaller fraction, perfluorononanoate (PFNA) and lower-chain-length PFCAs. In general, the overall yield of PFOA is low, presumably because of the multiple branches in the biotransformation pathways, including conjugation reactions in animal systems. There have been a few studies of non-FTOH biotransformation, which include polyfluoroalkyl phosphates (PAPs), 8:2 fluorotelomer acrylate (8:2 FTAC), and fluorotelomer carboxylates (FTCAs, FTUCAs). The PAPs compds. and 8:2 FTAC were shown to be direct precursors to FTOHs and thus follow similar degrdn. pathways. Environ Toxicol Chem 2014;33:243-267. © 2013 SETAC.
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    27. 27
      Kabadi, S. V.; Fisher, J.; Aungst, J.; Rice, P. Internal exposure-based pharmacokinetic evaluation of potential for biopersistence of 6:2 fluorotelomer alcohol (FTOH) and its metabolites. Food Chem. Toxicol. 2018, 112, 375– 382,  DOI: 10.1016/j.fct.2018.01.012
      27
      Internal exposure-based pharmacokinetic evaluation of potential for biopersistence of 6:2 fluorotelomer alcohol (FTOH) and its metabolites
      Kabadi, Shruti V.; Fisher, Jeffrey; Aungst, Jason; Rice, Penelope
      Food and Chemical Toxicology (2018), 112 (), 375-382CODEN: FCTOD7; ISSN:0278-6915. (Elsevier Ltd.)
      Polyfluorinated compds. (PFCs) are authorized for use as greaseproofing agents in food contact paper. As C8-PFCs (8-carbons) are known to accumulate in tissues, shorter-chain C6-PFCs (6-carbons) have replaced C8-PFCs in many food contact applications. However, the potential of C6-PFCs for human biopersistence has not been fully evaluated. For the first time, we provide internal exposure ests. to key metabolites of 6:2 fluorotelomer alc. (6:2 FTOH), a monomeric component of C6-PFCs, to extend our understanding of exposure beyond ests. of external exposure. Pharmacokinetic data from published rat and human studies on 6:2 FTOH were used to est. clearance and area under the curve (AUC) for its metabolites: 5:3 fluorotelomer carboxylic acid (5:3 A), perfluorohexanoic acid (PFHxA) and perfluoroheptanoic acid (PFHpA). Internal exposure to 5:3 A was the highest of evaluated metabolites across species and it had the slowest clearance. Addnl., 5:3 A clearance decreased with increasing 6:2 FTOH exposure. Our anal. provides insight into assocn. of increased internal 5:3 A exposure with high biopersistence potential of 6:2 FTOH. Our results identify 5:3 A as an important biomarker of internal 6:2 FTOH exposure for use in biomonitoring studies, and are potentially useful for toxicol. assessment of chronic dietary 6:2 FTOH exposure.
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    28. 28
      Rice, P. A.; Aungst, J.; Cooper, J.; Bandele, O.; Kabadi, S. V. Comparative analysis of the toxicological databases for 6:2 fluorotelomer alcohol (6:2 FTOH) and perfluorohexanoic acid (PFHxA). Food Chem. Toxicol. 2020, 138, 111210– 111210,  DOI: 10.1016/j.fct.2020.111210
      28
      Comparative analysis of the toxicological databases for 6:2 fluorotelomer alcohol (6:2 FTOH) and perfluorohexanoic acid (PFHxA)
      Rice, Penelope A.; Aungst, Jason; Cooper, Jessica; Bandele, Omari; Kabadi, Shruti V.
      Food and Chemical Toxicology (2020), 138 (), 111210CODEN: FCTOD7; ISSN:0278-6915. (Elsevier Ltd.)
      6:2 Fluorotelomer alc. (6:2 FTOH) is a short-chain polyfluoroalkyl substance (PFAS) in polymeric PFAS used in fast food packaging and stain- and water-resistant textiles and may be degrdn. products of some components of aq. film-forming foams (AFFF). The general population is exposed to 6:2 FTOH by inhalation of evaps. from treated surfaces or ambient concns. in air, ingestion of indoor dust, or ingestion of food packaged in materials contg. PFAS. Although exposure to 6:2 FTOH is pervasive, little is known concerning human health effects of this compd. Some published risk assessments have assumed that perfluorohexanoic acid (PFHxA), a metabolite of 6:2 FTOH, adequately models the human health effects of 6:2 FTOH. Recently identified studies conducted with 6:2 FTOH and its metabolite, 5:3 acid, have provided information that enables comparison of the toxicol. profiles of PFHxA and 6:2 FTOH. This article summarizes a comparative anal. of the toxicol. effects of PFHxA and 6:2 FTOH in rodents to det. whether data for PFHxA adequately models potential hazards of 6:2 FTOH exposure. Our anal. demonstrates that 6:2 FTOH is significantly more toxic than PFHxA. Use of toxicol. studies conducted with PFHxA to assess 6:2 FTOH exposure may significantly underestimate human health risk.
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    29. 29
      Huang, M. C.; Robinson, V. G.; Waidyanatha, S.; Dzierlenga, A. L.; DeVito, M. J.; Eifrid, M. A.; Gibbs, S. T.; Blystone, C. R. Toxicokinetics of 8:2 fluorotelomer alcohol (8:2-FTOH) in male and female Hsd:Sprague Dawley SD rats after intravenous and gavage administration. Toxicology Reports 2019, 6 (May), 924– 932,  DOI: 10.1016/j.toxrep.2019.08.009
      29
      Toxicokinetics of 8:2 fluorotelomer alcohol (8:2-FTOH) in male and female Hsd:Sprague Dawley SD rats after intravenous and gavage administration
      Huang, M. C.; Robinson, V. G.; Waidyanatha, S.; Dzierlenga, A. L.; DeVito, M. J.; Eifrid, M. A.; Gibbs, S. T.; Blystone, C. R.
      Toxicology Reports (2019), 6 (), 924-932CODEN: TROEF9; ISSN:2214-7500. (Elsevier B.V.)
      Fluorotelomer alcs. (FTOHs) are used in the prodn. of persistent per- and polyfluorinated alkyl substances (PFAS). Rodents and humans metabolize FTOHs to perfluoralkyl carboxylic acids which have several assocd. toxicities. Thus, understanding the toxicokinetics of these FTOHs and their metabolites will be useful for interpreting their toxicity for humans. Here, male and female Hsd:Sprague-Dawley SD rats were administered a single dose of 8:2-FTOH via gavage (males: 12, 24, 48 mg/kg; females: 40, 80, 160 mg/kg) or IV (males: 12 mg/kg; females: 40 mg/kg). Toxicokinetics of 8:2-FTOH and two primary metabolites, perfluorooctanoic acid (PFOA) and 7:3-fluorotelomer acid (7:3-FTA) were detd. in plasma. Concns. (total) of these chems. were detd. in the liver, kidney, and brain. There was rapid absorption and distribution of 8:2-FTOH after gavage administration in male rats. The plasma elimination half-life ranged from 1.1 to 1.7 h. Kinetic parameters of 8:2-FTOH in females were similar to that in males. Bioavailability of 8:2-FTOH ranged from 22 to 41% for both sexes with no dose-dependent trends. 8:2-FTOH metabolites, PFOA and 7:3-FTA were detected in plasma following administration of the parent FTOH. Consistent with existing literature, the plasma half-life of PFOA was longer in males than in females (198-353 h and 4.47-6.9 h, resp.). The plasma half-life of 7:3-FTA was around 2-3 days in both sexes. 8:2-FTOH and 7:3-FTA were detected in all tissues; PFOA was found in the liver and kidney but not the brain. Detectable concns. of metabolites persisted longer than the parent FTOH. These data demonstrate that in rats given a single gavage dose, 8:2-FTOH is rapidly absorbed, metabolized to form PFOA and 7:3-FTA, distributed to tissues, and eliminated faster than its metabolites. Sex differences were obsd. in the tissue distribution and elimination of PFOA, but not 8:2-FTOH and 7:3-FTA.
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    30. 30
      Buck, R. C; Franklin, J.; Berger, U.; Conder, J. M; Cousins, I. T; de Voogt, P.; Jensen, A. A.; Kannan, K.; Mabury, S. A; van Leeuwen, S. P. Perfluoroalkyl and polyfluoroalkyl substances in the environment: Terminology, classification, and origins. Integr. Environ. Assess. Manage. 2011, 7 (4), 513– 541,  DOI: 10.1002/ieam.258
      30
      Perfluoroalkyl and polyfluoroalkyl substances in the environment: Terminology, classification, and origins
      Buck, Robert C.; Franklin, James; Berger, Urs; Conder, Jason M.; Cousins, Ian T.; de Voogt, Pim; Jensen, Allan Astrup; Kannan, Kurunthachalam; Mabury, Scott A.; van Leeuwen, Stefan P. J.
      Integrated Environmental Assessment and Management (2011), 7 (4), 513-541CODEN: IEAMCK; ISSN:1551-3777. (John Wiley & Sons Inc.)
      A review. The primary aim of this article is to provide an overview of perfluoroalkyl and polyfluoroalkyl substances (PFASs) detected in the environment, wildlife, and humans, and recommend clear, specific, and descriptive terminol., names, and acronyms for PFASs. The overarching objective is to unify and harmonize communication on PFASs by offering terminol. for use by the global scientific, regulatory, and industrial communities. A particular emphasis is placed on long-chain perfluoroalkyl acids, substances related to the long-chain perfluoroalkyl acids, and substances intended as alternatives to the use of the long-chain perfluoroalkyl acids or their precursors. First, we define PFASs, classify them into various families, and recommend a pragmatic set of common names and acronyms for both the families and their individual members. Terminol. related to fluorinated polymers is an important aspect of our classification. Second, we provide a brief description of the 2 main prodn. processes, electrochem. fluorination and telomerization, used for introducing perfluoroalkyl moieties into org. compds., and we specify the types of byproducts (isomers and homologues) likely to arise in these processes. Third, we show how the principal families of PFASs are interrelated as industrial, environmental, or metabolic precursors or transformation products of one another. We pay particular attention to those PFASs that have the potential to be converted, by abiotic or biotic environmental processes or by human metab., into long-chain perfluoroalkyl carboxylic or sulfonic acids, which are currently the focus of regulatory action. The Supplemental Data lists 42 families and subfamilies of PFASs and 268 selected individual compds., providing recommended names and acronyms, and structural formulas, as well as Chem. Abstrs. Service registry nos. Integr Environ Assess Manag 2011;7:513-541. © 2011 SETAC.
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    31. 31
      Rankin, K.; Lee, H.; Tseng, P. J.; Mabury, S. A. Investigating the biodegradability of a fluorotelomer-based acrylate polymer in a soil-plant microcosm by indirect and direct analysis. Environ. Sci. Technol. 2014, 48 (21), 12783– 12790,  DOI: 10.1021/es502986w
      31
      Investigating the Biodegradability of a Fluorotelomer-Based Acrylate Polymer in a Soil-Plant Microcosm by Indirect and Direct Analysis
      Rankin, Keegan; Lee, Holly; Tseng, Pablo J.; Mabury, Scott A.
      Environmental Science & Technology (2014), 48 (21), 12783-12790CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Fluorotelomer-based acrylate polymers (FTACPs) are a class of side-chain fluorinated polymers used for a variety of com. applications. The degrdn. of FTACPs through ester hydrolysis, cleavage of the polymer backbone, or both could serve as a significant source of perfluoroalkyl carboxylates (PFCAs). The biodegrdn. of FTACPs was evaluated in a soil-plant microcosm over 5.5 mo in the absence/presence of wastewater treatment plant (WWTP) biosolids using a unique FTACP detd. to be a homopolymer of 8:2 fluorotelomer acrylate (8:2 FTAC). Although structurally different from com. FTACPs, the unique FTACP possesses 8:2 fluorotelomer side chain appendages bound to the polymer backbone via ester moieties. Liberation and subsequent biodegrdn. of the 8:2 fluorotelomer appendages was indirectly detd. by monitoring for PFCAs of varying chain lengths (C6-C9) and known fluorotelomer intermediates by liq. chromatog. tandem mass spectrometry (LC-MS/MS). A FTACP biodegrdn. half-life range of 8-111 years was inferred from the 8:2 fluorotelomer alc. (8:2 FTOH) equiv. of the unique FTACP and the increase of degrdn. products. The progress of FTACP biodegrdn. was also directly monitored qual. using matrix-assisted laser desorption/ionization (MALDI-TOF) time-of-flight mass spectrometry. The combination of indirect and direct anal. indicated that the model FTACP biodegraded predominantly to perfluorooctanoate (PFOA) in soils and at a significantly higher rate in the presence of a plant and WWTP biosolids.
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    32. 32
      Royer, L. A.; Lee, L. S.; Russell, M. H.; Nies, L. F.; Turco, R. F. Microbial transformation of 8:2 fluorotelomer acrylate and methacrylate in aerobic soils. Chemosphere 2015, 129, 54– 61,  DOI: 10.1016/j.chemosphere.2014.09.077
      32
      Microbial transformation of 8:2 fluorotelomer acrylate and methacrylate in aerobic soils
      Royer, Laurel A.; Lee, Linda S.; Russell, Mark H.; Nies, Loring F.; Turco, Ronald F.
      Chemosphere (2015), 129 (), 54-61CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
      Biotransformation of fluorotelomer (FT) compds., such as 8:2 FT alc. (FTOH) is now recognized to be a source of perfluorooctanoic acid (PFOA) as well as other perfluoroalkyl acids. In this study, microbially mediated hydrolysis of FT industrial intermediates 8:2 FT acrylate (8:2 FTAC) and 8:2 FT methacrylate (8:2 FTMAC) was evaluated in aerobic soils for up to 105 d. At designated times, triplicate microcosms were sacrificed by sampling the headspace for volatile FTOHs followed by sequential extn. of soil for the parent monomers as well as transient and terminal degrdn. products. Both FTAC and FTMAC were hydrolyzed at the ester linkage as evidenced by 8:2 FTOH prodn. 8:2 FTAC and FTMAC degraded rapidly with half-lives ≤5 d and 15 d, resp. Maximum 8:2 FTOH levels were 6-13 mol% within 3-6 d. Consistent with the known biotransformation pathway of 8:2 FTOH, FT carboxylic acids and perfluoroalkyl carboxylic acids were subsequently generated including up to 10.3 mol% of PFOA (105 d). A total mass balance (parent plus metabolites) of 50-75 mol% was obsd. on the last sampling day. 7:2 sFTOH, a direct precursor to PFOA, unexpectedly increased throughout the incubation period. The likely, but unconfirmed, concomitant prodn. of acrylic acids was proposed as altering expected degrdn. patterns. Biotransformation of 8:2 FTAC, 8:2 FTMAC, and previously reported 8:2 FT-stearate for the same soils revealed the effect of the non-fluorinated terminus group linked to the FT chain on the electronic differences that affect microbially-mediated ester cleavage rates.
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    33. 33
      Johnson, W.; Zhu, J. Safety Assessment of Polyfluorinated Polymers as Used in Cosmetics Status; Cosmetic Ingredient Review: Washington, DC, 2018.
      There is no corresponding record for this reference.
    34. 34
      Kobo Fluorinated Treatments. http://www.koboproductsinc.com/Products.aspx?p=Fluorinated%20Treatments&c=Perfluorohexylethyl%20Triethoxysilane%20(FS) (accessed Jan 22, 2021).
      There is no corresponding record for this reference.
    35. 35
      Kobo Microspheres, Microsphere Complexes and Composites. http://www.koboproductsinc.com/Products_Categories.aspx?mPage=Treated%20Pigments%20Powders (accessed Jan 22, 2021).
      There is no corresponding record for this reference.
    36. 36
      Pascal, A.; Myriam, M. Homogeneous composition based on fluorinated compounds and glycols, preparation process and use in cosmetics. French Patent FR2700691A1, April 7, 1997.
      There is no corresponding record for this reference.
    37. 37
      Tajima, S.; Ikeda, T. Water-in-oil emulsion solid cosmetic. U.S. Patent US20170056302A1, October 8, 2019.
      There is no corresponding record for this reference.
    38. 38
      Tanaka, K.; Kawano, C. Cosmetic composition comprising double coated pigment. World Patent WO2003077878A1, September 25, 2003.
      There is no corresponding record for this reference.
    39. 39
      Trabelsi, V. Composition for making up the lips. U.S. Patent US9023334B2, May 5, 2015.
      There is no corresponding record for this reference.
    40. 40
      Becker, L. C.; Bergfeld, W. F.; Belsito, D. V.; Hill, R. A.; Klaassen, C. D.; Liebler, D.; Marks, J. G., Jr.; Shank, R. C.; Slaga, T. J.; Snyder, P. W.; Andersen, F. A. Safety assessment of silylates and surface-modified siloxysilicates. Int. J. Toxicol. 2013, 32 (3_suppl), 5s– 24s,  DOI: 10.1177/1091581813486299
      40
      Safety assessment of silylates and surface-modified siloxysilicates
      Becker, Lillian C.; Bergfeld, Wilma F.; Belsito, Donald V.; Hill, Ronald A.; Klaassen, Curtis D.; Liebler, Daniel; Marks, James G., Jr; Shank, Ronald C.; Slaga, Thomas J.; Snyder, Paul W.; Andersen, F. Alan
      International Journal of Toxicology (2013), 32 (3S), 5S-24S, 20CODEN: IJTOFN; ISSN:1091-5818. (Sage Publications)
      The Cosmetic Ingredient Review (CIR) Expert Panel assessed the safety of silica silylate, silica di-Me silylate, trimethylsiloxysilicate, and trifluoropropyldimethyl/trimethylsiloxysilicate as used in cosmetics. These silylates and surface-modified siloxysilicates function in cosmetics as antifoaming agents, anticaking agents, bulking agents, binders, skin-conditioning agents-emollient, skin-conditioning agents-occlusive, slip modifiers, suspension agents-nonsurfactant, and viscosity increasing agents-nonaq. The Expert Panel reviewed the available animal and clin. data as well as information from a previous CIR safety assessment of amorphous silica. The CIR Expert Panel concluded that silica silylate, silica di-Me silylate, trimethylsiloxysilicate, and trifluoropropyldimethyl/trimethylsiloxysilicate are safe as used when formulated and delivered in the final product not to be irritating or sensitizing to the respiratory tract.
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    41. 41
      O’Lenick, A., Jr. Silicones for Personal Care; Allured Publishing Corporation: Carol Stream, IL, 2008.
      There is no corresponding record for this reference.

  • Supporting Information

    Supporting Information

    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.estlett.1c00240.

    • Additional details and parameters used for the instrumental analyses, including PIGE analysis and targeted LC-MS/MS and GC-MS analyses. List of categories used to categorize the cosmetics analyzed, as well as a list of cosmetic brands sampled. Full results of targeted LC-MS/MS and GC-MS analyses, as well as a summary of various features of the total fluorine analyses. Detection frequencies of various PFAS classes for targeted analysis. Summary of label information for all ingredients used in the targeted products. (PDF)


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