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The Global Threat from the Irreversible Accumulation of Trifluoroacetic Acid (TFA)
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Cite this: Environ. Sci. Technol. 2024, 58, 45, 19925–19935
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https://doi.org/10.1021/acs.est.4c06189
Published October 30, 2024

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Abstract

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Trifluoroacetic acid (TFA) is a persistent and mobile substance that has been increasing in concentration within diverse environmental media, including rain, soils, human serum, plants, plant-based foods, and drinking water. Currently, TFA concentrations are orders of magnitude higher than those of other per- and polyfluoroalkyl substances (PFAS). This accumulation is due to many PFAS having TFA as a transformation product, including several fluorinated gases (F-gases), pesticides, pharmaceuticals, and industrial chemicals, in addition to direct release of industrially produced TFA. Due to TFA’s extreme persistence and ongoing emissions, concentrations are increasing irreversibly. What remains less clear are the thresholds where irreversible effects on local or global scales occur. There are indications from mammalian toxicity studies that TFA is toxic to reproduction and that it exhibits liver toxicity. Ecotoxicity data are scarce, with most data being for aquatic systems; fewer data are available for terrestrial plants, where TFA bioaccumulates most readily. Collectively, these trends imply that TFA meets the criteria of a planetary boundary threat for novel entities because of increasing planetary-scale exposure, where potential irreversible disruptive impacts on vital earth system processes could occur. The rational response to this is to instigate binding actions to reduce the emissions of TFA and its many precursors.

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Rapidly increasing TFA concentrations, coupled with TFA’s extreme persistence, mobility and the possibility of irreversible impacts, should prompt action to reduce emissions of TFA and its precursors.

Introduction

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Trifluoroacetic acid (TFA) belongs to the subclass of per- and polyfluoroalkyl substances (PFAS) known as ultrashort-chain perfluoroalkyl acids (PFAAs). TFA is by far the most abundant PFAS in the environment. (1−6) Neuwald et al. demonstrated that TFA accounted for more than 90% of the total PFAS mass (of 46 individual PFAS analyzed) in various drinking water sources in Germany. (2) Tian et al. observed that concentrations of TFA and perfluoropropionic acid (PFPrA) in air, dry-deposition particles, and plant leaves surrounding two landfills in China were an order of magnitude higher than those of the 21 other PFAS analyzed. (4) Chen et al. measured 25 PFAS around two fluorochemical manufacturing plants in China, covering 8 different media (air, various water, soil, dust, plant leaves, sediment), with TFA concentrations being consistently 1–2 orders of magnitude higher than those of other PFAS. (5)
An initial wave of scientific interest in the environmental fate and effects of TFA started around the mid-1990s, due to novel fluorinated refrigerants (hydrofluorocarbons (HFCs) and hydrochlorofluorocarbons (HCFCs)) being introduced to the market after the ozone-depleting chlorofluorocarbons (CFCs) were phased out under the 1987 Montreal Protocol on Substances that Deplete the Ozone Layer. (7−12) Many of the fluorinated refrigerants are referred to as F-gases (encompassing gases with an R–CF3 moiety, R–CF2–R moiety, or inorganic fluorides). When F-gases or other fluorinated organic substances contain a C–CF3 moiety that is resistant to biochemical or photochemical degradation, TFA will commonly be a terminal degradation product. In recent years, interest in TFA has been re-established due to rapidly increasing concentrations observed in remote locations, as well as its ubiquity in drinking water sources and human blood. (2,13−15)
Since the 1990s, it has been suggested that hazard-related concerns of TFA and other short-chain PFAAs are much lower than those of PFAAs with longer perfluoroalkyl chains, which are more bioaccumulative and generally more toxic. (8,9,16−23) However, these early reports did not consider TFA’s ubiquitous accumulation in the environment, in particular its observed accumulation in water resources and bioaccumulation in various plants, including crops. Although there are fewer toxicological data compared to long-chain PFAAs, we maintain that there are more than sufficient data to conclude that TFA poses a risk to humans and the environment and meets the criteria of a planetary boundary threat for novel entities. (24−27) We will present evidence for this based on TFA’s (1) increasing planetary exposure, which is (2) irreversible and increasing due to emissions from many sources and could thereby cause (3) long-lasting disruptive effects on human health and vital earth system processes. Our analysis leads to the conclusion that policy, industry initiatives, and innovation actions should be enacted globally to reduce TFA emissions as soon as possible to protect future generations from potential irreversible effects of TFA accumulation.

Increasing Planetary Exposure

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A review of the scientific literature was conducted to obtain an overview of average and maximum concentrations in diverse environmental media (see the Supporting Information (SI) for a full methodology and collected data). In brief, 43 studies reporting on TFA concentrations spanning from the late 1990s to the 2020s were selected, and monitoring data were analyzed. Collectively, these data indicate that TFA exposure is widespread and is increasing.
Recent median concentrations of TFA in precipitation were measured at 0.29 μg/L in the USA, (28) 0.21 μg/L in Germany, (29) and 0.70 μg/L in Fuxin, China. (5) The median drinking water concentrations reported in the recent peer-reviewed literature vary from 0.08 μg/L in the USA (Indiana) (18) to 1.5 μg/L in Germany, (2) and 0.23 μg/L in samples from 19 different countries other than Germany. (30) This has relevance to TFA being included within regulatory definitions of “total PFAS”. These median concentrations are either similar to or higher than the proposed limits of total PFAS in drinking water in the EU draft recast Drinking Water Directive, (31) which places a threshold of 0.5 μg/L for total PFAS. (32) A recent report measuring TFA in European surface water and groundwater recorded an exceedance of the 0.5 μg/L threshold in 79% of the samples, with more than 98% of the detected mass of total PFAS being TFA. (32) A Swiss study reported detecting TFA in 560 out of 564 drinking water samples in 2023, with 69% of the concentrations above 0.5 μg/L, among which were 2 samples with TFA concentrations above 9 μg/L and 75 between 1 and 9 μg/L. (33)
If there is TFA contamination in soil or water, short and ultrashort PFAAs undergo rapid uptake and bioaccumulation in crops and other plants, particularly in their aerial compartments. (34−37) Chen et al. (5) detected concentrations of up to 3800 mg/kgdw of TFA in plants in the vicinity of a fluorochemical industrial site in China with an average field bioaccumulation factor of 13,000. In general, TFA has been enriching in conifer needles, (5,38) maize, (5,39) leaves of various tree species, (4,5) and some wetland species. (40) Consequently, high concentrations of TFA in plant-based foods (41) and plant-based beverages such as juice, (42) beer, and tea (30) were reported, indicating that the ingestion of plant-based foods and beverages could be a substantial route for human (and animal) exposure.
TFA was detected in human blood from China (43) with median concentrations of 8.46 μg/L, similar to the levels of long-chain PFAAs, although TFA is not considered bioaccumulative according to regulatory criteria (which typically refer to bioaccumulation in aquatic species entering the food chain and not to bioaccumulation in plants). (44) A similar study in the USA reported a median of 6 μg/L and a maximum of 77 μg/L, (18) where TFA alone had a 57% contribution to the total mass of 39 detected PFAS in human serum. Thus, the concentrations of TFA in nonoccupationally exposed US citizens are similar to the concentrations of bioaccumulative legacy long-chain PFAAs (e.g., PFOS, PFHxS, PFNA, PFDA) measured in the serum of occupationally exposed workers. (45) Because of high uptake, TFA reaches levels in human serum that are much higher than its low bioaccumulation potential in aquatic species would indicate.
To demonstrate the change in concentrations and trends over the years, Figure 1 presents a comparison of pre-2010 and post-2010 data (by the reported year of sampling, not the year of publication). This cutoff year of 2010 was chosen because there was a slump of interest in TFA in the peer-reviewed literature between the years 2008 to 2012. Prior to this time, research on TFA attracted attention in relation to the introduction of F-gases around the late 1990s to replace CFCs. In more recent years, TFA has attracted increased attention due to it more commonly being included and detected during PFAS monitoring campaigns. The first of January 2010 also coincides with the final deadline for stopping the last remaining production of CFCs; (46) even though the transition to F-gases occurred much before this time. (15)

Figure 1

Figure 1. Comparison of TFA concentrations detected in different media summarized as before 2010 (green) and after 2010 (in red). Reported values of maximum concentrations found in the literature review are shown as vertical bars and mean values of reported monitoring means and medians are shown with overlapping dots. Numbers indicating the number of summarized individual data points are shown above the corresponding bars. In cases of either green or red bars and dots missing, data were not available for the given media and/or time frame. For air concentrations before 2010 only two studies were available, one of which reported only mean measured concentrations (see Table S1 for the full data set and Figure S3 for air data presented as concentrations from individual studies).

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When pre- and post-2010 concentration data are available in a specific medium (Figure 1), an increase in TFA by over an order of magnitude in both maximum and mean concentrations in several environmental compartments is evident, including for precipitation, rivers and streams, groundwater, drinking water, soil, and plants. While atmospheric media were the main focus of monitoring studies dated pre-2010 (especially precipitation), more data from other media became available after this cutoff year─with new media relevant to human exposure (e.g., plant-based beverages, crops, indoor and outdoor dust, human serum), ecosystem exposure (e.g., animals such as locusts, autochthonous tree species), as well as other media that were rarely measured before (e.g., drinking water). Comprehensive figures with concentrations across different media are available in the SI (Figures S1–S4).
More detailed time trends are available at specific locations. Urban surface waters around Beijing were sampled in 2002 (47) and were resampled in 2012, (48) showing up to a 17-fold increase in TFA concentrations over 10 years, while tap water detections went from nondetection to 0.16 μg/L in 2012. (48) Freeling et al. reported an increase in wet deposition in Germany from 22 to 30 t/year during 1995–1996 to 68 to 98 t/year in 2019. (29) Pickard et al. used dated Arctic ice cores to show a rapid increase in deposited TFA after the entry-into-force of the Montreal Protocol, from nondetection or a few ng/L in segments before 1989 to 0.13 and 0.15 μg/L in segments dated 2015 and 2017, respectively. (15) In 2021, Cahill et al. reported a 6-fold increase in TFA in a stream transect in California since 1998. (49) Freeling et al. analyzed archived leaf samples of different tree species for TFA and observed increases by factors of up to 12.5 in TFA concentrations in some species from 1989 to 2020. (50) A study in indoor and outdoor dust found a 4-fold increase in TFA between 2013 and 2017. (51)

An Irreversible Burden from Multiple Sources of Emissions

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Based on its persistence and high mobility due to lack of sorption, (13,52) TFA’s ultimate recipient is the Earth’s hydrosphere. As TFA is omnipresent in all water bodies, from groundwater, oceanic water, ice cores, drinking water to bottled water, (1,2,15,30,48,53−55) dilution in many ways has already occurred, with the only substantial remaining dilution medium being the deep ocean. Similarly, enrichment in plants will follow constantly increasing TFA concentrations as water and soil concentrations increase. With limited processes for elimination from plant tissues because of TFA’s persistence (no biotransformation) and its lack of volatility (as it is a strong acid in water and fully ionized), constant passive uptake from soil pore water via the transpiration stream can be expected for the lifetime of the plant as long as there is an input of TFA available. This theory is supported by findings for other short- and ultrashort-chain PFAAs (36) and is in agreement with the results by Zhang et al., (56) who did not observe a steady-state concentration being reached for TFA in their wheat experiments.
Exposure of TFA within agricultural and other ecosystems has not been assessed to the same extent as it has for other, longer-chain PFAAs; (57−62) however, it is inevitable that with increasing emissions on the global scale, the mean TFA concentrations in humans (serum), animals and plants will increase. The only potential environmentally relevant pathways of TFA degradation are overtone photodissociation in the troposphere and biologically catalyzed conversion processes that convert TFA to fluoroform (CF3H). (63) This is likely negligible in terms of TFA mass loss, as TFA is readily scavenged from the atmosphere by wet (and to a lower extent, dry) deposition, before it spreads rapidly in the terrestrial hydrosphere. (12,48,64) Nevertheless, considering the high TFA concentrations, even a low conversion of TFA to fluoroform may have an observable impact on atmospheric fluoroform concentrations. (63) Methods to remove TFA from water are expensive and often inefficient due to TFA’s persistence and mobility. (53,65−67) In some cases, water purification methods as common as ozonation and chlorination are also a source of TFA, depending on the presence of TFA-precursors. (53) The most effective solution would be reverse osmosis (RO) to upconcentrate TFA, followed by some intensive destruction techniques. However, RO treatment of water, particularly wastewater, compared to other forms of water treatment is expensive, (68,69) requires a substantial amount of energy (70) and typically results in 50% water loss. (71) The necessity of RO for water treatment is also in contradiction to Article 7(3) of the EU’s Water Framework Directive, which states “Member States shall ensure the necessary protection for the bodies of water identified with the aim of avoiding deterioration in their quality in order to reduce the level of purification treatment required in the production of drinking water”. (72) Destructive techniques for concentrated TFA, such as incinerating RO concentrates or even biomass containing TFA, may lead to harmful byproducts, including fluoroform (a potent greenhouse gas with a GWP of 14,800 times that of CO2 over 100 years). (63,73)
We mentioned above that one source of increasing TFA concentrations is the increased use of F-gases used as refrigerant chemicals; it is worth looking into this in more detail. Refrigerant chemicals have a history of being problematic. CFCs were originally introduced as “safer”, alternative refrigerants to ammonia, sulfur dioxide and methyl chloride, until it was discovered that CFCs were volatile enough to reach the stratosphere and release Cl radicals that lead to the decomposition of stratospheric ozone, particularly over Antarctica. (74−76) In this manner, CFCs were a planetary boundary threat associated with severe impacts. (77) To protect the ozone layer from poorly reversible depletion, the Montreal Protocol (78) required CFCs used in refrigeration and air conditioning systems to be substituted with HCFCs and HFCs (79) or natural refrigerants. HCFCs have lower ozone depletion potential than CFCs, and HFCs have no ozone depletion potential; however, HFCs have a high global warming potential (GWP). (79) Further amendments to the Montreal Protocol and the European F-gas Regulation aimed to replace the high-GWP F-gases with low-GWP alternatives. (80) Nevertheless, the substances proposed as replacements–hydrofluoroolefins (HFOs) and even currently applied HFCs–add to the problem because many HFOs and HFCs can be either partially (e.g., HFC-134a, HFC-143a, HFC-1234ze, HCFO-1233zd) or completely (e.g., HFC-227ea, HFO-1225ye(E), HFO-1225ye(Z), u-HCFC-1224yd(Z), and HFO-1234yf) transformed to TFA. (81,82) The use of HFO-1234yf was estimated to be responsible for 6900 t/year emissions of TFA in 2020 in the EU alone, with a potential increase in emissions up to 47,650 t/year by 2050. (81) This shift in F-gases could cause emissions of TFA to increase by orders of magnitude in the coming years, (81) along with a corresponding contribution to climate impacts due to the formation of more fluoroform from TFA in the troposphere. (63)
Another major source of TFA is direct emissions from industrial production and processes. For example, TFA is registered under EU’s Regulation 1907/2006 on the Registration, Evaluation, Authorisation and Restriction of Chemicals (REACH) as manufactured and/or imported into the EU in volumes ranging from 100 to 1000 tons per year. (52) Additionally, TFA is used as an intermediate, but this usage does not require the registration of production volumes. Xie et al. measured TFA in the surrounding environment (surface water, groundwater, air, dust, soil) of three fluorochemical plants near Jinan, China, that manufacture inorganic fluorine products, TFA and fluoride-containing intermediates. (83) Whereas Xie et al. reported surface water concentrations up to a maximum of 2.6 μg/L, (83) concentrations up to 7500 μg/L were recently reported in surface water of the river Arias in the vicinity of a production plant producing TFA and related PFAS in Southern France. (84,85)
In addition to F-gases and direct TFA production, (83−85) there are several other precursors contributing to the accumulation of TFA in the environment, including a variety of groups of chemicals containing the C–CF3 moiety, such as agrochemicals, (53,86−88) pharmaceuticals, (53) (fluoro)polymers, (89−91) and other PFAS. (13,53,92) TFA and its precursors can be emitted from point sources such as the (fluoro)chemical industry, (5,53) wastewater treatment plants, landfills, (4,93,94) and sites with a history of the use of aqueous film-forming foams (AFFFs). (93,95) The German Environment Agency (Umweltbundesamt, UBA) published estimates for TFA emissions from sources in Germany. (96) The available data indicate that refrigerants and blowing agents were the largest quantifiable source of TFA with emissions at ∼2000 t/year in Germany, followed by pesticides at ∼457 t/year (mainly flufenacet, diflufenican, and fluazinam), and human pharmaceuticals at ∼29 t/year. Emissions from other sources, such as direct production of TFA, biocides, veterinary pharmaceuticals, and fluorochemicals in products could not be quantified in that study. (96) There have been speculations about natural sources of TFA, but these have been discredited by Joudan et al., (97) who demonstrated that only increasing anthropogenic sources of TFA can explain its exponential increase in recent decades. A source of TFA that has been recognized since the 1990s and is garnering increasing attention is the transformation products from the thermal destruction of fluoropolymers, (98) as well as treatment of PFAS by destruction methods. (53,99,100) TFA formation yields of diverse PFAS destruction methods are often unknown and this should therefore be investigated when developing new destruction methods for PFAS. (16) TFA has been dubbed a “Substance from Multiple Sources” by Nödler and Scheurer, (101) highlighting the difficulty in ascertaining the main sources of TFA in monitoring studies of water resources. (14,19)

Disruptive Effects on Human Health and Earth System Processes

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There may be disruptive effects of TFA on human health or on Earth system processes that are currently unknown, similar to how the effects of longer-chain PFAAs on human health and CFCs on the ozone layer were initially unknown by the broader scientific and regulatory community. Overcoming this ignorance is the hardest part of understanding that a certain novel entity that is irreversibly increasing in concentrations globally may pose a planetary boundary threat. (25) Such effects cannot be fully described or anticipated by established paradigms of hazard and risk assessment. However, as those paradigms are commonly used in defining regulatory human and ecosystem health thresholds for chemicals, this is where we start our analysis of TFA potentially causing a disruptive impact on a planetary scale.

Known Health and Environmental Thresholds

A recent review by Dekant and Dekant (17) summarized the mammalian toxicity of TFA, referring specifically to human toxicity. Most toxicity tests on which human health risk assessments were based are rat studies, which found mild liver hypertrophy (increased size of the liver) as the lead effect at daily doses of > 1000 mg/kgbw in a 90-day feeding study. More human-relevant tests directed toward a mechanistic understanding and not only toward filling regulatory apical end points should be conducted in the future. Currently, there is an intention under EU Regulation 1272/2008 on the Classification, Labeling and Packaging of Substances and Mixtures (CLP) to classify TFA and its salts under Category 1B: Presumed human reproductive toxicant, based on new evidence of embryo-fetal developmental toxicity in rabbits, submitted to the European Chemicals Agency (ECHA) by Germany. (52,102,103) If TFA were to be classified as toxic for reproduction, this could have an impact on future threshold values in food and drinking water. In 2020, Germany established a human-health guideline value for TFA in drinking water at 60 μg/L, which is based on a chronic rat toxicity (feeding) study, but emphasized that the concentration in drinking water should be kept as low as reasonably possible and a value of 10 μg/L should be targeted. (104) In 2023, The Netherlands derived an indicative drinking water value for TFA at 2.2 μg/L, based on the potency factor relative to perfluorooctanoic acid (PFOA) and its threshold for drinking water. (105) Considering that the mean and maximum TFA concentrations in German drinking water sources were recently measured at 0.9 and 12.4 μg/L, (2) respectively, it is plausible that drinking water concentrations in many areas have or will exceed the 2.2 μg/L threshold in the near future.
Under the EU’s CLP Regulation, TFA is classified as harmful to aquatic life with long-lasting effects (H412). (106) Under REACH, the toxicological threshold for the general population (Derived No Effect Level, DNEL) is derived only for the oral route and set to 0.042 mg/kgbw/day, while for other routes of exposure, no hazard has been assumed and concluded. The threshold for the oral route was derived based on the observed effects from a 90-day rat-feeding study. (52) Human toxicokinetic evaluation of TFA showed rapid oral absorption, submission to enterohepatic circulation, and body distribution via blood, which included passing through the placenta barrier. The main excretion routes are considered to be via urine and bile. (52) Although TFA is not bioaccumulative according to regulatory criteria referring to aquatic organisms, (52) internal concentrations may increase due to continuous accumulation in exposure media, such as drinking water and plant-based food and beverages.
Contrary to the most recent human toxicological review, (17) a similar recent review is not available for (eco)toxicity data. We conducted a search of the USEPA ECOTOX database (107) and ECHA registration dossiers (52) and found that most efforts toward the determination of (eco)toxicity of TFA are from the 1990s. Algae are considered the most sensitive trophic level, with S. capricornutum the most sensitive species and 120 μg/L the lowest determined No-Observed Effect Concentration (NOEC), which was determined for the TFA sodium salt (Solvay data, ECOTOX database extracted for TFA/NaTFA and reported in Berends et al. (8,107)). Selected ecotoxicity end points (acute and chronic) for other organisms are reported in Table S2 of the Supporting Information, with listed ecotoxicological thresholds and their abbreviations. Overall, most of the testing was performed for acute toxicity with only a few studies investigating the chronic toxicity of TFA.
Predicted no-effect concentrations (PNECs) are concentration thresholds commonly derived in environmental risk assessment that should be protective of the whole ecosystem. They are based on ecotoxicity data and extrapolation factors based on data abundance, test duration (acute/chronic), and data quality/uncertainty. (108) For TFA, the lowest PNEC of 0.12 μg/L was derived by Xie et al. (83) and was based on algae that were previously shown as the most sensitive trophic level. The PNEC of 0.12 μg/L was derived from a NOEC of 120 μg/L by using an uncertainty factor of 1000, chosen because of the scarcity of (eco)toxicity data in the peer-reviewed literature and because extrapolation to the marine environment requires extra precaution (typically by a factor of 10 compared to freshwater). The ECHA REACH dossier reports a freshwater PNEC of 560 μg/L and a marine water PNEC of 56 μg/L, both based on the algal study reporting the 72 h ErC10 (EC10 based on growth rate) of 5600 μg/L. (52) Almost all surface water median and/or mean concentrations from peer-reviewed studies reported as post-2010 already exceed the precautionary PNEC of 0.12 μg/L as derived by Xie et al. (83) (Table S1, Figure S2), while the NOEC of 120 μg/L and ECHA’s PNEC of 560 μg/L are exceeded by some recently detected maximum freshwater/surface water values. (84,85)
Among terrestrial organisms (ecotoxicity studies), only crop plants were tested for TFA toxicity in the REACH dossier. The EC50 was 4.7 mg/kg soil dry weight, and a long-term NOEC was 0.83 mg/kg soil dry weight. It was mostly the plant shoot growth that was affected. (52) Further testing of TFA plant toxicity is needed, due to the scarcity of plant toxicity studies with sufficiently high internal plant concentrations, and for including other vascular plants than crops. (13) However, the long-term NOEC determined in crops (52) is already similar to soil TFA background concentrations and is several orders of magnitude lower than TFA soil concentrations in contamination hotspots (Figure 1, Figure S4). (5,39)
Given the persistence of TFA, exposure to TFA should be considered chronic and lifelong for all species. However, chronic studies are still relatively scarce, with chronic data from standardized tests being limited in time of exposure to, for example, 35 days in fish, 21 days in Daphnia, 90 days in rats, or 36 days in crop plants (52) (Table S2, SI), which are insufficient in their extrapolation to potential impacts from lifetime exposure to TFA. Hence, none of the current studies considered actual long-term exposure to TFA, which would be more relevant given its ubiquitous and increasing presence over long time scales.
In contrast to the analysis above, other authors (109,110) recently concluded the risk of TFA to humans and the environment is de minimis (i.e., negligible) based on examples like a projected concentration of TFA in the ocean of 0.2 μg/L by 2100 compared to the NOEC in the algae R. subcapitata of 2500 μg/L, (109,110) as well as the median human serum levels of 8.46 μg/L in the serum of staff of Nankai University being 4 orders of magnitude below effect doses in rats. However, we disagree that these are sufficient data to conclude negligible risk, considering that the conclusion ignores terrestrial environments, assumes that the lowest measured environmental effect levels are known despite the lack of long-term chronic exposure data for other species, and does not consider diverse human exposure pathways in the context of increasing TFA concentration in diet and potential unknown adverse effects, such as on embryo development. Given the persistence and accumulation of TFA, there could be other, unknown environmental and health impacts for which the current science is ignorant.

Unknown Environmental and Health Impacts

As TFA is accumulating in diverse ecosystems, researchers should focus on nontraditional exposure and impact pathways that affect biogeochemical processes. Despite the extremely high plant uptake of TFA, controlled uptake experiments have rarely been performed and reported for TFA. Zhang et al. (56) performed a set of hydroponic experiments with TFA and other ultrashort and short PFCAs. Here, the root uptake was exceptionally high for TFA when compared to other PFCAs, e.g., the root concentration factor of TFA was >1600 L/kg, (56) 2 orders of magnitude higher than usually determined for PFCAs with 3–5 perfluorinated carbons in similar experiments. (111−113) Chen et al. (5) found a similar pattern for chain length dependence across PFCAs and the field-based soil-water distribution coefficients (Kd). They determined Kd values that were higher than expected for TFA (and PFPrA), demonstrating the opposite to the commonly observed trend of Kd decreasing as the perfluoroalkyl chain length decreases from 11 to 3 perfluorinated carbons for PFCAs and PFSAs. (114−117) This indicates that the interface partitioning of TFA and interactions with soils and plants need to be further researched and accounted for in assessing its environmental fate and behavior properties, particularly its (bio)accumulation potential. Such research needs to be extended to agricultural systems, such as the transfer from crops containing elevated levels of TFA to livestock (meat and milk) and human diets, as well as a transfer of TFA from plants through diverse food webs, similar to previous research on other PFAS. (58−61)
Direct effects of TFA on soil quality were only recently investigated. (118) Effects on the soil pH, microbial respiration, bacterial abundance and litter decomposition were reported, the latter being affected at concentrations similar to current TFA concentrations in soil for contamination hotspots as described in Chen et al. (5) (0.0013–2.4 mg/kgdw). Effects other than litter decomposition were statistically significant only at high TFA concentrations (≥10 mg/kg) which could be a result of acidity-related effects, as the pH significantly decreased at concentrations of 10 mg/kg and higher (TFA in the acid form was directly used in the testing). (118) Bott and Standley observed the incorporation of TFA into cells by microbial communities in freshwater surface sediments (119) after also demonstrating TFA incorporation in biomolecules such as proteins in aquatic organisms spanning a range of trophic levels. (11) Concentrations that were used in these ∼1.5 to 2.5-year experiments overlap with those currently observed in waters worldwide, ranging from 2.2 to 43 μg/L (Table S1, Figure S2, SI), and resulted in significant cell incorporation of TFA. (119) It was also indicated that at elevated concentrations, the presence of TFA in the atmosphere may influence aerosols and cloud formation, boosting the formation of atmospheric clusters involved in new aerosol particle formation. (120,121) As concentrations of TFA will likely increase by at least an order of magnitude in the coming decade, further investigations of TFA on biogeochemical processes are warranted.

Environmental Implications

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Based on the evidence presented above, the increasing accumulation of TFA can be considered to meet the three conditions of a planetary boundary threat (122,123) for novel entities as defined by Persson et al.: (25) “Condition 1 (C1) – the pollution has a disruptive effect on a vital earth system process of which we are ignorant; Condition 2 (C2) – the disruptive effect is not discovered until the associated impacts are, or inevitably will be, manifested at a global scale; and Condition 3 (C3) the impacts are poorly reversible because the level of pollution in the global environment cannot be readily reduced...” Condition 1 (C1) is fulfilled based on the many thresholds that could be exceeded of which we are ignorant; including surface water concentrations (84,85) that exceed (83) ECHA’s PNEC of 560 μg/L; soil concentrations that exceed the lowest established NOEC (0.83 mg/kg soil); (52) and, indications of human toxicity that have led to precautionary thresholds in drinking water. (104) The existence of such health advisory and regulatory values has been used as the basis for establishing C1 in relation to four PFAAs in a previous study. (27) The possibility of other long-term disruptive effects, which may be already occurring but of which we are ignorant, further supports the C1 being fulfilled, particularly considering the absence of studies of TFA exposure in agricultural systems and diverse food webs. Condition 2 (C2) is fulfilled as TFA is already present globally in all environmental media, such as its ongoing bioaccumulation in vascular plants, the accumulation in arctic regions, its ubiquity in groundwater, and the global occurrence of industrial sites that are TFA hotspots where impacts are most likely; therefore, when impacts are discovered, they would be global. Since effects are realized globally and will be irreversible for the foreseeable future, condition 3 (C3) is fulfilled due to TFA’s extreme persistence and mobility coupled with emissions from multiple sources.
Although, currently, TFA does not have as well-established health advisories or regulatory limits as other PFAA, (27) it is likely that new advisories/limits will be introduced in the coming years when more research on the impacts of TFA emerges. With the projected exponential increase in TFA concentrations in the environment, (81) food and in humans, the question is not if TFA can exceed a planetary boundary, but which irreversible health or Earth system impacts would be first observed at a planetary scale, and where thresholds of TFA emissions should be set to limit the severity of such impacts.
The potential long-term, irreversible impacts from the rapidly increasing emissions of TFA from anthropogenic sources should be used as a rationale to start immediately discussing policy, industry, and innovation actions toward the phase-out of high-volume substances that lead to increasing TFA accumulation. Obvious places to start would be to limit the direct production of TFA, and more importantly, of TFA-precursors, such as HFOs (like HFO-1234yf) and pesticides such as flufenacet. (13,53,96) Other pharmaceuticals, veterinary products and industrial chemicals that release TFA via transformation processes (7) should also be considered for phase-out or substitutions, following the principles of safe-and-sustainable by design (124) and essential use (125) to avoid regrettable substitution (126) to more hazardous substances. As discussions and policy mechanisms to phase out the sources of TFA could take some time, the rational response to the global threat posed by accumulating TFA is to act swiftly before irreversible impacts are manifested at a global scale to humans and the environment. Transitioning away from TFA and its precursors is the most effective way of safeguarding future generations from this planetary boundary threat.

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    H.P.H.A and A.G. contributed equally to this paper.

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    The authors declare no competing financial interest.

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Hans Peter H. Arp, NGI, is an environmental chemist interested in how fundamental aspects of physical chemistry can be utilized as applied tools for understanding and preventing pollution exposure. His projects focus on designing solutions through policy mechanisms, chemical properties, interdisciplinary collaboration, and sustainable technologies to enable the circular economy and help create a zero-pollution society. He holds a PhD from ETH Zürich (2008) and a professorship at the Norwegian University of Science and Technology (since 2018). He is an Associate Editor for the journal Environmental Science: Processes and Impacts (since 2024).

Acknowledgments

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Funding is acknowledged under the European Union’s Horizon 2020 research and innovation program project ZeroPM, under grant agreement No 101036756, and the Horizon Europe project ARAGORN under grant agreement 101112723. M. Scheringer acknowledges financial support by the RECETOX Research Infrastructure (LM2023069) financed by the Ministry of Education, Youth and Sports of the Czech Republic. Gabriel Salierno, Gretta Goldenman, Rainer Lohmann, and Cora Young are thanked for providing comments on a preprint version.

References

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This article references 126 other publications.

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Recognizing this, industry embarked on a research and assessment program to study the potential effects of trifluoroacetate (TFA) on the environment and to investigate possible degrdn. pathways. The results of these recently completed studies are summarized below and described in further detail in this paper. Trifluoroacetic acid is a strong org. acid with a pKa of 0.23. It is miscible with water and its low octanol/water partition coeff. (log Pow = -2.1) indicates no potential to bioaccumulate. Industrial use is limited and environmental releases are very low. Some addnl. TFA will be formed from the breakdown of a few halogenated hydrocarbons, most notably HFC-134a (CF3CH2F), HCFC-124 (CF3CHFCl), and HCFC-123 (CF3CHCl2). As these substances have only been produced in limited com. quantities, their contribution to environmental levels has been minimal. Surprisingly, environmental measurements in many of diverse locations show existing levels of 100 to 300 ng·l-1 in water with one site (Dead Sea) having a level of 6400 ng·l-1. These levels cannot be accounted for based on current atm. sources and imply a long-term, possibly pre-industrial source. Generally, soil retention of TFA is poor although soils with high levels of org. matter have been shown to have a greater affinity for TFA when contrasted to soils with low levels of org. matter. This appears to be an adsorption phenomenon, not irreversible binding. Therefore, TFA will not be retained in soil, but will ultimately enter the aq. compartment. Modeling of emission rates and subsequent conversion rates for precursors has led to ests. of max. levels of TFA in rain water in the region of 0.1 μg·l-1 in the year 2020. TFA is resistant to both oxidative and reductive degrdn. While there had been speculation regarding the possibility of TFA being degraded into monofluoroacetic acid (MFA), the rate of breakdown of MFA is so much higher than for TFA that any MFA formed would rapidly degrade. Therefore, there would be no buildup of MFA regardless of the levels of TFA present in the environment. Although highly resistant to microbial degrdn., there have been two reports of TFA degrdn. under anaerobic conditions. In the first study, natural sediments reduced TFA. However, even though this work was done in replicate, the investigators and others were unable to reproduce it in subsequent studies. In the second study, radiolabeled TFA was removed from a mixed anaerobic in vitro microcosm. Limited evidence of decarboxylation has also been reported for two strains of bacteria grown under highly specific conditions. TFA was not biodegraded in a semi-continuous activated sludge test even with prolonged incubation (up to 84 days). TFA does not accumulate significantly in lower aquatic life forms such as bacteria, small invertebrates, oligochaete worms and some aquatic plants including Lemna gibba (duckweed). Some bioaccumulation was obsd. in terrestrial higher plants, such as sunflower and wheat. This result appeared to be related to uptake with water and then concn. due to transpiration water loss. When transferred to clean hydroponic media, some elimination of TFA was seen. Also, more than 80% of the TFA in leaves was found to be water extractable, suggesting that no significant metab. of TFA had occurred. At an exposure level of 1200 mg·l-1 of sodium trifluoroacetate (NaTFA) - corresponding to 1000 mg·l-1 HTFA - no effects were seen on either Brachydanio rerio (a fish) or Daphnia magna (a water flea). With duckweed, mild effects were seen on frond increase and wt. increase at the same exposure level. At a concn. of 300 mg·l-1 no effects were obsd. Toxicity tests were conducted with 11 species of algae. For ten of these species the EC50 was greater than 100 mg·l-1. In Selenastrum capricornutum the no-effect level was 0.12 mg·l-1. At higher levels the effect was reversible. The reason for the unique sensitivity of this strain is unknown, but a recovery of the growth rate was seen when citric acid was added. This could imply a competitive inhibition of the citric acid cycle. The effect of TFA on seed germination and plant growth has been evaluated with a wide variety of plants. Application of NaTFA at 1000 mg·l-1 to seeds of sunflower, cabbage, lettuce, tomato, mung bean, soy bean, wheat, corn, oats and rice did not affect germination. Foliar application of a soln. of 100 mg·l-1 of NaTFA to field grown plants did not affect growth of sunflower, soya, wheat, maize, oilseed rape, rice and plantain. When plantain, wheat (varieties Katepwa and Hanno) and soya were grown in hydroponic systems contg. NaTFA, no effects were seen on plantain at 32 mg·l-1, on wheat (Katepwa) and soya at 1 mg·l-1, or on wheat (Hanno) at 10 mg·l-1; some effects on growth were seen at, resp., 100 mg·l-1, 5 mg·l-1, 5 mg·l-1, and 10 mg·l-1 and above. TFA is not metabolized in mammalian systems to any great extent. It is the major final metabolite of halothane, HCFC-123 and HCFC-124. The half-life of TFA in humans is 16 h. As expected, the acute oral toxicity of the free acid is higher than the one of the sodium salt. The inhalation LC50 (2 h exposure) for mice was 13.5 mg·l-1 (2900 ppm) and for rats it was 10 mg·l-1 (2140 ppm). Thus, TFA is considered to have low inhalation toxicity. The irritation threshold for humans was 54 ppm. As one would expect of a strong acid, it is a severe irritant to the skin and eye. When conjugated with protein, it has been shown to elicit an immunol. reaction; however, it is unlikely that TFA itself would elicit a sensitization response. Repeat administration of aq. solns. have shown that TFA can cause increased liver wt. and induction of peroxisomes. Relative to the doses (0.5% in diet or 150 mg·kg-1·day-1 by gavage) the effects are mild. In a series of Ames assays, TFA was reported to be non-mutagenic. Its carcinogenic potential has not been evaluated. Although TFA was shown to accumulate in amniotic fluid following exposure of pregnant animals to high levels of halothane (1200 ppm), no fetal effects were seen. Likewise, a reprodn. study that involved exposure of animals to halothane at levels up to 4000 ppm for 4 h per day, 7 days per wk, resulted in no adverse effects. Given the high levels of halothane exposure, it is unlikely that environmental TFA is a reproductive or developmental hazard. Overall the toxicity of TFA has been evaluated in stream mesocosms, algae, higher plants, fish, animals and humans. It has been found to be of very low toxicity in all of these systems. The lowest threshold for any effects was the reversible effect on growth of one strain of algae, Selenastrum capricornutum, which was seen at 0.12 mg·l-1. There is a 1000-fold difference between the no-effect concn. and the projected environmental levels of TFA from HFCs and HCFCs (0.0001 mg·l-1). Based on available data, one can conclude that environmental levels of TFA resulting from the breakdown of alternative fluorocarbons do not pose a threat to the environment.
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  10. 10
    Likens, G. E.; Tartowski, S. L.; Berger, T. W.; Richey, D. G.; Driscoll, C. T.; Frank, H. G.; Klein, A. Transport and Fate of Trifluoroacetate in Upland Forest and Wetland Ecosystems. Proc. Natl. Acad. Sci. U.S.A. 1997, 94 (9), 4499– 4503,  DOI: 10.1073/pnas.94.9.4499
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    Standley, L. J.; Bott, T. L. Trifluoroacetate, an Atmospheric Breakdown Product of Hydrofluorocarbon Refrigerants: Biomolecular Fate in Aquatic Organisms. Environ. Sci. Technol. 1998, 32 (4), 469– 475,  DOI: 10.1021/es970161b
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    Trifluoroacetate, an Atmospheric Breakdown Product of Hydrofluorocarbon Refrigerants: Biomolecular Fate in Aquatic Organisms
    Standley, Laurel J.; Bott, Thomas L.
    Environmental Science and Technology (1998), 32 (4), 469-475CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Aquatic organisms were monitored for their ability to incorporate trifluoroacetate (TFA), an atm. breakdown product of HFC and HCFC refrigerants contg. a trifluoromethyl moiety. Because of the structural similarity of TFA to acetate, a biochem. intermediate and microbial nutrient, we suspected that organisms might use the fluorinated compd. to synthesize biomols. such as lipids and acetylated proteins. We exposed aquatic organisms (microbial communities, oligochaetes, macroinvertebrates, Callitriche sp., Lemna sp., and Impatiens capensis) to radioactive TFA ([14C]F3COOH) and examd. them for distribution of radiolabel in different classes of biomols. The most label was found in oligochaetes and I. capensis leaves at 3 and 6 μg/g (as TFA), resp., with the greatest proportion found in the protein fraction for each sample type. Aerobic microorganisms incorporated only a small fraction of the label (a few nanograms per g as TFA), and the greatest proportion of label occurred in cell wall material. We have demonstrated that selected aquatic organisms spanning a range of trophic levels incorporated the xenobiotic TFA into their biomol. fractions so that it was no longer extd. as TFA and thus was metabolically transformed.
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  12. 12
    Wujcik, C. E.; Cahill, T. M.; Seiber, J. N. Determination of Trifluoroacetic Acid in 1996–1997 Precipitation and Surface Waters in California and Nevada. Environ. Sci. Technol. 1999, 33 (10), 1747– 1751,  DOI: 10.1021/es980697c
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    Determination of Trifluoroacetic Acid in 1996-1997 Precipitation and Surface Waters in California and Nevada
    Wujcik, Chad E.; Cahill, Thomas M.; Seiber, James N.
    Environmental Science and Technology (1999), 33 (10), 1747-1751CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    The atm. degrdn. of three chlorofluorocarbon (CFC) replacement compds., namely HFC-134a, HCFC-123, and HCFC-124, results in the formation of trifluoroacetic acid (TFA). Concns. of TFA were detd. in pptn. and surface water samples collected in California and Nevada during 1996-1997. Terminal lake systems were found to have concns. 4-13 times higher than their calcd. yearly inputs, providing evidence for accumulation. The results support dry deposition as the primary contributor of TFA to surface waters in arid and semiarid environments. Pptn. samples obtained from three different locations contained 20.7-1530 ng/L with significantly higher concns. in fogwater (median = 689 ng/L) over rainwater (median = 63.7 ng/L). Elevated levels of TFA were obsd. for rainwater collected in Nevada (median = 136 ng/L) over those collected in California (median = 49.5 ng/L), indicating continual uptake and concn. as clouds move from a semiarid to arid climate. Thus several mechanisms exist, including evaporative concn., vapor-liq. phase partitioning, lowered washout vols. of atm. deposition water, and dry deposition, which may lead to elevated concns. of TFA in atm. and surface waters above levels expected from usual rainfall washout.
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  13. 13
    Freeling, F.; Björnsdotter, M. K. Assessing the Environmental Occurrence of the Anthropogenic Contaminant Trifluoroacetic Acid (TFA). Current Opinion in Green and Sustainable Chemistry 2023, 41, 100807  DOI: 10.1016/j.cogsc.2023.100807
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    Zhang, W.; Liang, Y. The Wide Presence of Fluorinated Compounds in Common Chemical Products and the Environment: A Review. Environmental Science and Pollution Research 2023, 30 (50), 108393– 108410,  DOI: 10.1007/s11356-023-30033-6
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    Pickard, H. M.; Criscitiello, A. S.; Persaud, D.; Spencer, C.; Muir, D. C. G.; Lehnherr, I.; Sharp, M. J.; De Silva, A. O.; Young, C. J. Ice Core Record of Persistent Short-Chain Fluorinated Alkyl Acids: Evidence of the Impact From Global Environmental Regulations. Geophys. Res. Lett. 2020, 47 (10).  DOI: 10.1029/2020GL087535 .
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    Brunn, H.; Arnold, G.; Körner, W.; Rippen, G.; Steinhäuser, K. G.; Valentin, I. PFAS: Forever Chemicals─Persistent, Bioaccumulative and Mobile. Reviewing the Status and the Need for Their Phase out and Remediation of Contaminated Sites. Environmental Sciences Europe 2023, 35 (1), 20,  DOI: 10.1186/s12302-023-00721-8
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    Dekant, W.; Dekant, R. Mammalian Toxicity of Trifluoroacetate and Assessment of Human Health Risks Due to Environmental Exposures. Arch. Toxicol. 2023, 97 (4), 1069– 1077,  DOI: 10.1007/s00204-023-03454-y
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    17
    Mammalian toxicity of trifluoroacetate and assessment of human health risks due to environmental exposures
    Dekant, Wolfgang; Dekant, Raphael
    Archives of Toxicology (2023), 97 (4), 1069-1077CODEN: ARTODN; ISSN:0340-5761. (Springer)
    Abstr.: While trifluoroacetic acid has limited tech. uses, the highly water-sol. trifluoroacetate (TFA) is reported to be present in water bodies at low concns. Most of the TFA in the environment is discussed to arise from natural processes, but also with the contribution from decompn. of environmental chems. The presence of TFA may result in human exposures. For hazard and risk assessment, the mammalian toxicity of TFA and human exposures are reviewed to assess the margin of exposures (MoE). The potential of TFA to induce acute toxicity is very low and oral repeated dose studies in rats have identified the liver as the target organ with mild liver hypertrophy as the lead effect. Biomarker analyses indicate that TFA is a weak peroxisome proliferator in rats. TFA administered to rats did not induce adverse effects in an extended one-generation study and in a developmental toxicity study or induce genotoxic responses. Based on recent levels of TFA in water and diet, MoEs for human exposures to TFA are well above 100 and do not indicate health risks.
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    Zheng, G.; Eick, S. M.; Salamova, A. Elevated Levels of Ultrashort- and Short-Chain Perfluoroalkyl Acids in US Homes and People. Environ. Sci. Technol. 2023, 57 (42), 15782– 15793,  DOI: 10.1021/acs.est.2c06715
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    18
    Elevated Levels of Ultrashort- and Short-Chain Perfluoroalkyl Acids in US Homes and People
    Zheng, Guomao; Eick, Stephanie M.; Salamova, Amina
    Environmental Science & Technology (2023), 57 (42), 15782-15793CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)
    Per- and polyfluoroalkyl substances (PFAS) make up a large group of fluorinated org. compds. extensively used in consumer products and industrial applications. Perfluorooctanesulfonic acid (PFOS) and perfluorooctanoic acid (PFOA), the two perfluoroalkyl acids (PFAAs) with 8 carbons in their structure, were phased out on a global scale because of their high environmental persistence and toxicity. As a result, shorter-chain PFAAs with \<8 carbons in their structure are being used as their replacements and are now widely detected in the environment, raising concerns about their effects on the environment and human health. In this study, 47 PFAAs and their precursors were measured in paired samples of dust and drinking water collected from residential homes in Indiana, United States, and in blood and urine samples collected from the residents of these homes. Ultrashort- (with 2 or 3 carbons [C2-C3]) and short-chain (with 4-7 carbons [C4-C7]) PFAAs were the most abundant in all four matrixes and constituted on av. 69-100% of the total PFAA concns. Specifically, trifluoroacetic acid (TFA, C2) and perfluoropropanoic acid (PFPrA, C3) were the predominant PFAA congeners in most of the samples. Significant pos. correlations (n = 81; r = 0.23-0.42; p < 0.05) were found between TFA, perfluorobutanoic acid (PFBA, C4) and perfluoroheptanoic acid (PFHpA, C7) concns. in dust or water and those in serum, suggesting dust ingestion and/or drinking water consumption as important exposure pathways for these compds. This study demonstrates that ultrashort- and short-chain PFAAs are now abundant in the indoor environment and in people and warrants further research on potential adverse health effects of these exposures.
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  19. 19
    Solomon, K. R.; Velders, G. J. M.; Wilson, S. R.; Madronich, S.; Longstreth, J.; Aucamp, P. J.; Bornman, J. F. Sources, Fates, Toxicity, and Risks of Trifluoroacetic Acid and Its Salts: Relevance to Substances Regulated under the Montreal and Kyoto Protocols. Journal of Toxicology and Environmental Health - Part B: Critical Reviews 2016, 19 (7), 289– 304,  DOI: 10.1080/10937404.2016.1175981
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    Garavagno, M. d. l. A.; Holland, R.; Khan, M. A. H.; Orr-Ewing, A. J.; Shallcross, D. E. Trifluoroacetic Acid: Toxicity, Sources, Sinks and Future Prospects. Sustainability 2024, 16 (6), 2382,  DOI: 10.3390/su16062382
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    Hanson, M. L.; Solomon, K. R. Haloacetic Acids in the Aquatic Environment. Part I: Macrophyte Toxicity. Environ. Pollut. 2004, 130 (3), 371– 383,  DOI: 10.1016/j.envpol.2003.12.016
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    Kwiatkowski, C. F.; Andrews, D. Q.; Birnbaum, L. S.; Bruton, T. A.; DeWitt, J. C.; Knappe, D. R. U.; Maffini, M. V.; Miller, M. F.; Pelch, K. E.; Reade, A.; Soehl, A.; Trier, X.; Venier, M.; Wagner, C. C.; Wang, Z.; Blum, A. Response to “Comment on Scientific Basis for Managing PFAS as a Chemical Class.. Environ. Sci. Technol. Lett. 2021, 8 (2), 195– 197,  DOI: 10.1021/acs.estlett.1c00049
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    Singh, R. R.; Papanastasiou, D. K. Comment on “Scientific Basis for Managing PFAS as a Chemical Class.. Environmental Science and Technology Letters 2021, 8 (2), 192– 194,  DOI: 10.1021/acs.estlett.0c00765
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    Arp, H. P. H.; Kühnel, D.; Rummel, C.; MacLeod, M.; Potthoff, A.; Reichelt, S.; Rojo-Nieto, E.; Schmitt-Jansen, M.; Sonnenberg, J.; Toorman, E.; Jahnke, A. Weathering Plastics as a Planetary Boundary Threat: Exposure, Fate, and Hazards. Environ. Sci. Technol. 2021, 55 (11), 7246– 7255,  DOI: 10.1021/acs.est.1c01512
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    24
    Weathering plastics as a planetary boundary threat: Exposure, fate, and hazards
    Arp, Hans Peter H.; Kuhnel, Dana; Rummel, Christoph; MacLeod, Matthew; Potthoff, Annegret; Reichelt, Sophia; Rojo-Nieto, Elisa; Schmitt-Jansen, Mechthild; Sonnenberg, Johanna; Toorman, Erik; Jahnke, Annika
    Environmental Science & Technology (2021), 55 (11), 7246-7255CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    We described in 2017 how weathering plastic litter in the marine environment fulfils two of three criteria to impose a planetary boundary threat related to "chem. pollution and the release of novel entities": planetary-scale exposure, which is not readily reversible. Whether marine plastics meet the third criterion, eliciting a disruptive impact on vital earth system processes, was uncertain. Since then, several important discoveries have been made to motivate a re-evaluation. A key issue is if weathering macroplastics, microplastics, nanoplastics, and their leachates have an inherently higher potential to elicit adverse effects than natural particles of the same size. We summarize novel findings related to weathering plastic in the context of the planetary boundary threat criteria that demonstrate increasing exposure, fate processes leading to poorly reversible pollution, and (eco)toxicol. hazards and their thresholds. We provide evidence that the third criterion could be fulfilled for weathering plastics in sensitive environments and therefore conclude that weathering plastics pose a planetary boundary threat. We suggest future research priorities to better understand (eco)toxicol. hazards modulated by increasing exposure and continuous weathering processes, to better parametrize the planetary boundary threshold for plastic pollution.
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  25. 25
    Persson, L. M.; Breitholtz, M.; Cousins, I. T.; De Wit, C. A.; MacLeod, M.; McLachlan, M. S. Confronting Unknown Planetary Boundary Threats from Chemical Pollution. Environ. Sci. Technol. 2013, 47 (22), 12619– 12622,  DOI: 10.1021/es402501c
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    Confronting Unknown Planetary Boundary Threats from Chemical Pollution
    Persson, Linn M.; Breitholtz, Magnus; Cousins, Ian T.; de Wit, Cynthia A.; MacLeod, Matthew; McLachlan, Michael S.
    Environmental Science & Technology (2013), 47 (22), 12619-12622CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Rockstroem et al. proposed a set of planetary boundaries that delimitate a safe operating space for humanity. One of the planetary boundaries is detd. by chem. pollution, however no clear definition was provided. Here, probably there is no single chem. pollution planetary boundary, but rather that many planetary boundary issues governed by chem. pollution exist. The authors identify three conditions that must be simultaneously met for chem. pollution to pose a planetary boundary threat. The authors then discuss approaches to identify chems. that could fulfill those conditions, and outline a proactive hazard identification strategy that considers long-range transport and the reversibility of chem. pollution.
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  26. 26
    MacLeod, M.; Breitholtz, M.; Cousins, I. T.; De Wit, C. A.; Persson, L. M.; Rudén, C.; McLachlan, M. S. Identifying Chemicals That Are Planetary Boundary Threats. Environ. Sci. Technol. 2014, 48 (19), 11057– 11063,  DOI: 10.1021/es501893m
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    26
    Identifying chemicals that are planetary boundary threats
    MacLeod, Matthew; Breitholtz, Magnus; Cousins, Ian T.; Wit, Cynthia A. de; Persson, Linn M.; Ruden, Christina; McLachlan, Michael S.
    Environmental Science & Technology (2014), 48 (19), 11057-11063CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Rockstr.ovrddot.om et al. proposed a set of planetary boundaries that delimit a "safe operating space for humanity". Many of the planetary boundaries that have so far been identified are detd. by chem. agents. Other chem. pollution-related planetary boundaries likely exist, but are currently unknown. A chem. poses an unknown planetary boundary threat if it simultaneously fulfills three conditions: (1) it has an unknown disruptive effect on a vital Earth system process; (2) the disruptive effect is not discovered until it is a problem at the global scale, and (3) the effect is not readily reversible. In this paper, we outline scenarios in which chems. could fulfill each of the three conditions, then use the scenarios as the basis to define chem. profiles that fit each scenario. The chem. profiles are defined in terms of the nature of the effect of the chem. and the nature of exposure of the environment to the chem. Prioritization of chems. in commerce against some of the profiles appears feasible, but there are considerable uncertainties and scientific challenges that must be addressed. Most challenging is prioritizing chems. for their potential to have a currently unknown effect on a vital Earth system process. We conclude that the most effective strategy currently available to identify chems. that are planetary boundary threats is prioritization against profiles defined in terms of environmental exposure combined with monitoring and study of the biogeochem. processes that underlie vital Earth system processes to identify currently unknown disruptive effects.
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  27. 27
    Cousins, I. T.; Johansson, J. H.; Salter, M. E.; Sha, B.; Scheringer, M. Outside the Safe Operating Space of a New Planetary Boundary for Per- and Polyfluoroalkyl Substances (PFAS). Environ. Sci. Technol. 2022, 56 (16), 11172– 11179,  DOI: 10.1021/acs.est.2c02765
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    27
    Outside the safe operating space of a new planetary boundary for per- and polyfluoroalkyl substances (PFAS)
    Cousins, Ian T.; Johansson, Jana H.; Salter, Matthew E.; Sha, Bo; Scheringer, Martin
    Environmental Science & Technology (2022), 56 (16), 11172-11179CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)
    A review. It is hypothesized that environmental contamination by per- and polyfluoroalkyl substances (PFAS) defines a sep. planetary boundary and that this boundary has been exceeded. This hypothesis is tested by comparing the levels of four selected perfluoroalkyl acids (PFAAs) (i.e., perfluorooctanesulfonic acid (PFOS), perfluorooctanoic acid (PFOA), perfluorohexanesulfonic acid (PFHxS), and perfluorononanoic acid (PFNA)) in various global environmental media (i.e., rainwater, soils, and surface waters) with recently proposed guideline levels. On the basis of the four PFAAs considered, it is concluded that (1) levels of PFOA and PFOS in rainwater often greatly exceed US Environmental Protection Agency (EPA) Lifetime Drinking Water Health Advisory levels and the sum of the aforementioned four PFAAs (Σ4 PFAS) in rainwater is often above Danish drinking water limit values also based on Σ4 PFAS; (2) levels of PFOS in rainwater are often above Environmental Quality Std. for Inland European Union Surface Water; and (3) atm. deposition also leads to global soils being ubiquitously contaminated and to be often above proposed Dutch guideline values. It is, therefore, concluded that the global spread of these four PFAAs in the atm. has led to the planetary boundary for chem. pollution being exceeded. Levels of PFAAs in atm. deposition are esp. poorly reversible because of the high persistence of PFAAs and their ability to continuously cycle in the hydrosphere, including on sea spray aerosols emitted from the oceans. Because of the poor reversibility of environmental exposure to PFAS and their assocd. effects, it is vitally important that PFAS uses and emissions are rapidly restricted.
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  28. 28
    Pike, K. A.; Edmiston, P. L.; Morrison, J. J.; Faust, J. A. Correlation Analysis of Perfluoroalkyl Substances in Regional U.S. Precipitation Events. Water Res. 2021, 190, 116685  DOI: 10.1016/j.watres.2020.116685
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    Correlation Analysis of Perfluoroalkyl Substances in Regional U.S. Precipitation Events
    Pike, Kyndal A.; Edmiston, Paul L.; Morrison, Jillian J.; Faust, Jennifer A.
    Water Research (2021), 190 (), 116685CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)
    Per- and polyfluoroalkyl substances (PFAS) are transported in the atm., leading to both wet and dry deposition to the surface. The concns. of 15 PFAS were measured at six locations in the Ohio-Indiana region of the U. S. during the summer of 2019 and compared to samples collected at a distant site in NW Wyoming. ΣPFAS concns. ranged from 50-850 ng L-1, with trifluoroacetic acid (TFA) being the dominant compd. (∼90%). Concns. of perfluorooctanoic acid (PFOA) and perfluorosulfonic acid (PFOS) were similar to amts. obsd. over the past 20 years, indicating persistence in the atm. despite regulatory action, and the newer species HFPO-DA (GenX) was also widely detected in rainwater. ANOVA modeling and correlation matrixes were used to det. assocn. of PFAS concns., location, and functional group and chain length. Statistically significant differences (p < 0.05) in PFAS profiles across sites sepd. by 10-100 km indicate that local point sources strongly contribute to wet deposition. This work introduces correlation plots for PFAS that allow rapid visual comparison of multi-analyte and multi-site data sets.
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  29. 29
    Freeling, F.; Behringer, D.; Heydel, F.; Scheurer, M.; Ternes, T. A.; Nödler, K. Trifluoroacetate in Precipitation: Deriving a Benchmark Data Set. Environ. Sci. Technol. 2020, 54 (18), 11210– 11219,  DOI: 10.1021/acs.est.0c02910
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    29
    Trifluoroacetate in precipitation: Deriving a benchmark data set
    Freeling, Finnian; Behringer, David; Heydel, Felix; Scheurer, Marco; Ternes, Thomas A.; Noedler, Karsten
    Environmental Science & Technology (2020), 54 (18), 11210-11219CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Although pptn. is considered to be the most important diffuse source of trifluoroacetate (TFA) to the nonmarine environment, information regarding the wet deposition of TFA as well as general data on the spatial and temporal variations in TFA concn. in pptn. is scarce. This is the first study to provide a comprehensive overview of the occurrence of TFA in pptn. by a systematic and nation-wide field monitoring campaign. In total, 1187 pptn. samples, which were collected over the course of 12 consecutive months at eight locations across Germany, were analyzed. The median, the estd. av., and the pptn.-weighted av. of the TFA concn. of all analyzed wet deposition samples were 0.210, 0.703, and 0.335μg/L, resp. For Germany, an annual wet deposition flux of 190μg/m2 or approx. 68 t was calcd. for the sampling period from Feb. 2018 to Jan. 2019. The campaign revealed a pronounced seasonality of the TFA concn. and wet deposition flux of collected samples. Correlation anal. suggested an enhanced transformation of TFA precursors in the troposphere in the summertime due to higher concns. of photochem. generated oxidants such as hydroxyl radicals, ultimately leading to an enhanced atm. deposition of TFA during summer.
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  30. 30
    Scheurer, M.; Nödler, K. Ultrashort-Chain Perfluoroalkyl Substance Trifluoroacetate (TFA) in Beer and Tea – An Unintended Aqueous Extraction. Food Chem. 2021, 351, 129304  DOI: 10.1016/j.foodchem.2021.129304
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    Ultrashort-chain perfluoroalkyl substance trifluoroacetate (TFA) in beer and tea - An unintended aqueous extraction
    Scheurer, Marco; Noedler, Karsten
    Food Chemistry (2021), 351 (), 129304CODEN: FOCHDJ; ISSN:0308-8146. (Elsevier Ltd.)
    Trifluoroacetate (TFA) is an ultrashort-chain perfluoroalkyl substance, which is ubiquitously present in the aq. environment. Due to its high mobility, it accumulates in plant material. The study presented here shows for the first time that TFA is a widely spread contaminant in beer and tea / herbal infusions. In 104 beer samples from 23 countries, TFA was detected up to 51μg/L with a median concn. of 6.1μg/L. An indicative brewing test and a correlation approach with potassium (K) indicate that the main source of TFA in beer is most likely the applied malt. It could be proven that the impact of the applied water is negligible in terms of TFA, which was supported by the anal. of numerous tap water samples from different countries. The unintended extn. of TFA was also demonstrated for tea / herbal infusions with a median concn. of 2.4μg/L.
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    The European Parliament and the Council of the European Union. Directive (EU) 2020/2184 of the European Parliament and of the Council of 16 December 2020 on the Quality of Water Intended for Human Consumption (Recast) (Text with EEA Relevance); EU, 2020; pp 1– 62. https://eur-lex.europa.eu/eli/dir/2020/2184/oj (accessed 2024–05–22).
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    GLOBAL 2000; Friends of the Earth Austria; Pesticide Action Network Europe (PAN Europe); Generations Futures. TFA in Water, Dirty PFAS Legacy Under the Radar ; 2024; pp 1– 23 https://www.pan-europe.info/resources/reports/2024/05/tfa-water-dirty-pfas-legacy-under-radar (accessed 2024–05–31).
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    Meier, S.; Brodmann, P.; Weber, S.; Moschet, C.; Gelmi, T.; Lacour, W.; Steinmann, J.. TRINKWASSERQUALITÄT BEZÜGLICH DER PFAS-RÜCKSTÄNDE , 2024; pp 6 https://www.aquaetgas.ch/wasser/trinkwasser/20240228_ag3_trinkwasserqualit%C3%A4t-bez%C3%BCglich-der-pfas-r%C3%BCckst%C3%A4nde/ (accessed 2024–08–20).
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    Wang, W.; Rhodes, G.; Ge, J.; Yu, X.; Li, H. Uptake and Accumulation of Per- and Polyfluoroalkyl Substances in Plants. Chemosphere 2020, 261, 127584  DOI: 10.1016/j.chemosphere.2020.127584
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    Uptake and accumulation of per- and polyfluoroalkyl substances in plants
    Wang, Wenfeng; Rhodes, Geoff; Ge, Jing; Yu, Xiangyang; Li, Hui
    Chemosphere (2020), 261 (), 127584CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
    Per- and polyfluoroalkyl substances (PFASs) are a class of persistent org. contaminants that are ubiquitous in the environment and have been found to be accumulated in agricultural products. Consumption of PFAS-contaminated agricultural products represents a feasible pathway for the trophic transfer of these toxic chems. along food chains/webs, leading to risks assocd. with human and animal health. Recently, studies on plant uptake and accumulation of PFASs have rapidly increased; consequently, a review to summarize the current knowledge and highlight future research is needed. Anal. of the publications indicates that a large variety of plant species can take up PFASs from the environment. Vegetables and grains are the most commonly investigated crops, with perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS) as the most studied PFASs. The potential sources of PFASs for plant uptake include industrial emissions, irrigation with contaminated water, land application of biosolids, leachates from landfill sites, and pesticide application. Root uptake is the predominant pathway for the accumulation of PFASs in agricultural crops, and uptake by plant aboveground portions from the ambient atm. could play a minor role in the overall PFAS accumulation. PFAS uptake by plants is influenced by physicochem. properties of compds. (e.g., perfluorocarbon chain length, head group functionality, water soly., and volatility), plant physiol. (e.g., transpiration rate, lipid and protein content), and abiotic factors (e.g., soil org. matters, pH, salinity, and temp.). Based on literature anal., the current knowledge gaps are identified, and future research prospects are suggested.
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    Ghisi, R.; Vamerali, T.; Manzetti, S. Accumulation of Perfluorinated Alkyl Substances (PFAS) in Agricultural Plants: A Review. Environ. Res. 2019, 169, 326– 341,  DOI: 10.1016/j.envres.2018.10.023
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    Accumulation of perfluorinated alkyl substances (PFAS) in agricultural plants: A review
    Ghisi, Rossella; Vamerali, Teofilo; Manzetti, Sergio
    Environmental Research (2019), 169 (), 326-341CODEN: ENVRAL; ISSN:0013-9351. (Elsevier)
    PFASs are a class of compds. that include perfluoroalkyl and polyfluoroalkyl substances, some of the most persistent pollutants still allowed - or only partially restricted - in several product fabrications and industrial applications worldwide. PFASs have been shown to interact with blood proteins and are suspected of causing a no. of pathol. responses, including cancer. Given this threat to living organisms, we carried out a broad review of possible sources of PFASs and their potential accumulation in agricultural plants, from where they can transfer to humans through the food chain. Anal. of the literature indicates a direct correlation between PFAS concns. in soil and bioaccumulation in plants. Furthermore, plant uptake largely changes with chain length, functional group, plant species and organ. Low accumulations of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS) have been found in peeled potatoes and cereal seeds, while short-chain compds. can accumulate at high levels in leafy vegetables and fruits. Significant variations in PFAS buildup in plants according to soil amendment are also found, suggesting a particular interaction with soil org. matter. Here, we identify a series of challenges that PFASs pose to the development of a safe agriculture for future generations.
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    Gredelj, A.; Polesel, F.; Trapp, S. Model-Based Analysis of the Uptake of Perfluoroalkyl Acids (PFAAs) from Soil into Plants. Chemosphere 2020, 244, 125534  DOI: 10.1016/j.chemosphere.2019.125534
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    Model-based analysis of the uptake of perfluoroalkyl acids (PFAAs) from soil into plants
    Gredelj, Andrea; Polesel, Fabio; Trapp, Stefan
    Chemosphere (2020), 244 (), 125534CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
    Perfluoroalkyl acids (PFAAs) bioaccumulate in crops, with uptake being particularly high for short-chain PFAAs that are constantly transported with transpiration water to aerial plant parts. Due to their amphiphilic surfactant nature and ionized state at environmental pH, predicting the partitioning behavior of PFAAs is difficult and subject to considerable uncertainty, making exptl. data highly desirable. Here, we applied a plant uptake model that combines advective flux with measured partition coeffs. to reproduce the set of empirically derived plant uptake and soil-partitioning data for nine PFAAs in red chicory, in order to improve the mechanistic understanding and provide new insights into the complex uptake processes. We introduced a new parameter for retarded uptake (R) to explain the slow transfer of PFAA across biomembranes of the root epidermis, which has led to low transpiration stream concn. factors (TSCFs) presented in literature so far. We estd. R values for PFAAs using exptl. data derived for red chicory and used the modified plant uptake model to simulate uptake of PFAA into other crops. Results show that this semi-empirical model predicted PFAAs transport to shoots and fruits with good accuracy based on exptl. root to soil concn. factors (RCFdw) and soil to water partition coeffs. (Kd) as well as estd. R values and plant-specific data for growth and transpiration. It can be concluded that the combination of rather low Kd with high RCFdw and the absence of any relevant loss are the reason for the obsd. excellent plant uptake of PFAAs.
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    Lesmeister, L.; Lange, F. T.; Breuer, J.; Biegel-Engler, A.; Giese, E.; Scheurer, M. Extending the Knowledge about PFAS Bioaccumulation Factors for Agricultural Plants – A Review. Sci. Total Environ. 2021, 766, 142640  DOI: 10.1016/j.scitotenv.2020.142640
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    Extending the knowledge about PFAS bioaccumulation factors for agricultural plants - A review
    Lesmeister, Lukas; Lange, Frank Thomas; Breuer, Joern; Biegel-Engler, Annegret; Giese, Evelyn; Scheurer, Marco
    Science of the Total Environment (2021), 766 (), 142640CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)
    A review. A main source of perfluoroalkyl and polyfluoroalkyl substances (PFASs) residues in agricultural plants is their uptake from contaminated soil. Bioaccumulation factors (BAFs) can be an important tool to derive recommendations for cultivation or handling of crops prior consumption. This review compiles >4500 soil-to-plant BAFs for 45 PFASs from 24 studies involving 27 genera of agricultural crops. Grasses (Poaceae) provided most BAFs with the highest no. of values for perfluorooctanoic acid and perfluorooctane sulfonic acid. Influencing factors on PFAS transfer like compd.-specific properties (hydrophobicity, chain length, functional group, etc.), plant species, compartments, and other boundary conditions are critically discussed. Throughout the literature, BAFs were higher for vegetative plant compartments than for reproductive and storage organs. Decreasing BAFs per addnl. perfluorinated carbon were clearly apparent for aboveground parts (up to 1.16 in grains) but not always for roots (partly down to zero). Combining all BAFs per single perfluoroalkyl carboxylic acid (C4-C14) and sulfonic acid (C4-C10), median log BAFs decreased by -0.25(±0.029) and -0.24(±0.013) per fluorinated carbon, resp. For the first time, the plant uptake of ultra-short-chain (≤ C3) perfluoroalkyl acids (PFAAs) was reviewed and showed a ubiquitous occurrence of trifluoroacetic acid in plants independent from the presence of other PFAAs. Based on identified knowledge gaps, it is suggested to focus on the uptake of precursors to PFAAs, PFAAs ≤C3, and addnl. emerging PFASs such as GenX or fluorinated ethers in future research. Studies regarding the uptake of PFASs by sugar cane, which accounts for about one fifth of the global crop prodn., are completely lacking and are also recommended. Furthermore, aq. soil leachates should be tested as an alternative to the solvent extn. of soils as a base for BAF calcns.
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    Scott, B. F.; Spencer, C.; Martin, J. W.; Barra, R.; Bootsma, H. A.; Jones, K. C.; Johnston, A. E.; Muir, D. C. G. Comparison of Haloacetic Acids in the Environment of the Northern and Southern Hemispheres. Environ. Sci. Technol. 2005, 39 (22), 8664– 8670,  DOI: 10.1021/es050118l
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    Comparison of Haloacetic Acids in the Environment of the Northern and Southern Hemispheres
    Scott, B. F.; Spencer, C.; Martin, J. W.; Barra, R.; Bootsma, H. A.; Jones, K. C.; Johnston, A. E.; Muir, D. C. G.
    Environmental Science and Technology (2005), 39 (22), 8664-8670CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Haloacetic acids (HAAs) are a family of compds. whose environmental concns. have been extensively studied, primarily in Europe. Depending on the compd., their sources are believed to be both natural and anthropogenic. To better understand possible sources and contribute to the knowledge of the global distribution of these compds., esp. between the Northern and Southern Hemispheres, samples of pptn., soils, and conifer needles were collected from Canada, Malawi, Chile, and the U.K. Pptn. samples exhibited highest HAA concns. in collections from Canada, and lowest in those from Malawi. Malawi samples contained measurable levels of monobromoacetic acid (MBA) (56 ng/L) unlike those from most other locations (<9 ng/L). Soil HAA concn. levels were highest in the U.K. (e.g., 7.3 ng/g av. TCA) and lowest in Malawi (0.8 ng/g av. TCA), with Chile having higher levels (4.8 ng/g av. TCA) than Canada (3 ng/g av. TCA). Malawi soils contained small amts. of MBA (2 ng/g), in common with the two most southern of the 11 Chilean sites. Anal. of soil cores (10-cm depth sliced at 1 cm) from sites in Malawi and Chile showed that trichloroacetic acid (TCA) generally declined with depth while mono- and dichloroacetic acid (MCA and DCA) showed no trend. MCA, DCA, and TCA concns. in archived U.K. Soil samples increased by factors of 2, 4, and 5-fold over 75 years while TFA showed no consistent trend. Monochloroacetic acid (MCA) was detected in pine needles collected from Malawi. U.K. Needle samples had the highest concns. of all chloroacetic acids (CAAs): MCA, 2-18 ng/g; dichloroacetic acid (DCA), 2-38 ng/g; and trichloroacetic acid (TCA), 28-190 ng/g. Conifer needles from Canada and Chile contained CAAs at levels ranging from <2 to 16 ng/g wet wt. Trifluoroacetic acid concns. generally declined with increasing elevation in the samples from the Rocky Mountains in western Canada. The results indicate that concns. of HAAs are greatest in the industrialized Northern Hemisphere but there are significant amts. of these compds. in the less industrialized Southern Hemisphere.
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    Lan, Z.; Yao, Y.; Xu, J. Y.; Chen, H.; Ren, C.; Fang, X.; Zhang, K.; Jin, L.; Hua, X.; Alder, A. C.; Wu, F.; Sun, H. Novel and Legacy Per- and Polyfluoroalkyl Substances (PFASs) in a Farmland Environment: Soil Distribution and Biomonitoring with Plant Leaves and Locusts. Environ. Pollut. 2020, 263, 114487  DOI: 10.1016/j.envpol.2020.114487
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    Novel and legacy per- and polyfluoroalkyl substances (PFASs) in a farmland environment: Soil distribution and biomonitoring with plant leaves and locusts
    Lan, Zhonghui; Yao, Yiming; Xu, JiaYao; Chen, Hao; Ren, Chao; Fang, Xiangguang; Zhang, Kai; Jin, Litao; Hua, Xia; Alder, Alfredo C.; Wu, Fengchang; Sun, Hongwen
    Environmental Pollution (Oxford, United Kingdom) (2020), 263 (Part_A), 114487CODEN: ENPOEK; ISSN:0269-7491. (Elsevier Ltd.)
    The occurrence of legacy and novel per- and polyfluoroalkyl substances (PFASs) in multiple matrixes from a farmland environment was investigated in the Beijing-Tianjin-Hebei core area of northern China. PFASs were ubiquitously detected in farmland soils, and the detection frequency of 6:2 chlorinated polyfluoroalkyl ether sulfonic acid (6:2 Cl-PFESA) was higher than that of perfluorooctane sulfonic acid (98% vs. 83%). Long-chain PFASs, including 6:2 Cl-PFESA, showed a centered distribution pattern around the metropolis of Tianjin, probably due to the local intensive industrial activity, while trifluoroacetic acid (TFA) showed a decreasing trend from the coast to the inland area. Other than soil, TFA was also found at higher levels than other longer-chain PFASs in dust, maize (Zea mays), poplar (Populus alba) leaf and locust (Locusta migratoria manilens) samples. Both poplar leaves and locusts can be used as promising biomonitoring targets for PFASs in farmland environments, and their accumulation potential corresponds with protein and lipid contents. Apart from being exposed to PFASs via food intake, locusts were likely exposed via uptake from soil and pptd. dust in farmland environments. The biomonitoring of locusts may be more relevant to insectivores, which is important to conducting a comprehensive ecol. risk assessment of farmland environments.
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    Cahill, T. M.; Thomas, C. M.; Schwarzbach, S. E.; Seiber, J. N. Accumulation of Trifluoroacetate in Seasonal Wetlands in California. Environ. Sci. Technol. 2001, 35 (5), 820– 825,  DOI: 10.1021/es0013982
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    Accumulation of trifluoroacetate in seasonal wetlands in California
    Cahill, Thomas M.; Thomas, Carmen M.; Schwarzbach, Steven E.; Seiber, James N.
    Environmental Science and Technology (2001), 35 (5), 820-825CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Trifluoroacetate (TFA, CF3COO-) is a stable and mildly phytotoxic breakdown product of several fluorinated org. compds. including the hydro(chloro)fluorocarbons (HFC/HCFCs) that have largely replaced the stratospheric ozone-depleting chlorofluorocarbons (CFCs). TFA enters aquatic ecosystems primarily through pptn. and has the potential to accumulate in water bodies with little or no outflow to the point where toxic concns. could be achieved. This study demonstrated that seasonal wetlands lacking outflow concd. TFA as they evapd. during the dry season. In addn., the TFA within the pools was retained between years, which may result in long-term TFA accumulation. Since plants acquire TFA from their growing media, the plants exposed to high aq. concns. of TFA within the pools had elevated TFA concns. with a median concn. of 279 ng/g dry wt. in their tissues as compared to 33 ng/g for species growing outside the pools. The highest TFA concns. in water, which occurred just prior to the pools drying up, were in the 2-10 μg/L range. These concns. are ≈190 or less than reported toxic concns. for the most sensitive species tested, but our evidence suggests that these concns. will increase with continued TFA deposition into the pools.
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    EU Reference Laboratories for Residues of Pesticides. EURL-SRM-Residue Findings Report , 2017; pp 1– 10. https://www.eurl-pesticides.eu/userfiles/file/eurlsrm/eurlsrm_residue-observation_tfa-dfa.pdf (accessed 2023–12–08).
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    van Hees, P.; Karlsson, P.; Bucuricova, L.; Olsman, H.; Yeung, L.. Trifluoroacetic Acid (TFA) and Trifluoromethane Sulphonic Acid (TFMS) in Juice and Fruit/Vegetable Purees , 2024; pp 1– 8. https://cdnmedia.eurofins.com/european-east/media/uxcnaa2c/eurofins_tfa_tfms_juice_24_final.pdf (accessed 2024–08–27).
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    Duan, Y.; Sun, H.; Yao, Y.; Meng, Y.; Li, Y. Distribution of Novel and Legacy Per-/Polyfluoroalkyl Substances in Serum and Its Associations with Two Glycemic Biomarkers among Chinese Adult Men and Women with Normal Blood Glucose Levels. Environ. Int. 2020, 134, 105295  DOI: 10.1016/j.envint.2019.105295
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    Distribution of novel and legacy per-/polyfluoroalkyl substances in serum and its associations with two glycemic biomarkers among Chinese adult men and women with normal blood glucose levels
    Duan, Yishuang; Sun, Hongwen; Yao, Yiming; Meng, Yue; Li, Yongcheng
    Environment International (2020), 134 (), 105295CODEN: ENVIDV; ISSN:0160-4120. (Elsevier Ltd.)
    In this study, fasting serum samples from 252 participants with age range from 19 to 87 years old were collected in Tianjin, China. A total of 21 target PFASs were detd. to analyze levels and distribution of novel and legacy PFASs in serum and to further evaluate the cross-sectional assocns. of serum PFAS concns. with two glycemic biomarkers (i.e., fasting glucose and glycated Hb (HbA1c)). 6:2 chlorinated PFAES (6:2 Cl-PFAES) and trifluoroacetic acid (TFA) were widely detected novel PFASs (greater than90%) with relatively high median concns. (8.64 ng/mL and 8.46 ng/mL, resp.), which were second only to the two dominant legacy PFASs, i.e., perfluorooctanoic acid (PFOA, 14.83 ng/mL) and perfluorooctane sulfonic acid (14.24 ng/mL). Furthermore, 1% increase in serum PFOA and perfluorononanoic acid (PFNA) was sep. significantly assocd. with 0.018% [95% confidence interval (CI): 0.004%, 0.033%] and 0.022% (95% CI: 0.007%, 0.037%) increment in fasting glucose levels. Similarly, 1% increase in serum perfluorohexanoic acid, PFNA, and perfluorohexane sulfonic acid was significantly assocd. with 0.030% (95% CI: 0.010%, 0.051%), 0.018% (95% CI: 0.003%, 0.033%), 0.007% (95% CI: 0.003%, 0.011%) increment in HbA1c levels, resp. These findings suggested that 6:2 Cl-PFAES and TFA showed greater contributions to PFASs in serum and supported an assocn. of exposure to PFASs with fasting glucose and HbA1c.
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    Arnot, J. A.; Gobas, F. A. A Review of Bioconcentration Factor (BCF) and Bioaccumulation Factor (BAF) Assessments for Organic Chemicals in Aquatic Organisms. Environmental Reviews 2006, 14 (4), 257– 297,  DOI: 10.1139/a06-005
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    A review of bioconcentration factor (BCF) and bioaccumulation factor (BAF) assessments for organic chemicals in aquatic organisms
    Arnot, Jon A.; Gobas, Frank A. P. C.
    Environmental Reviews (Ottawa, ON, Canada) (2006), 14 (4), 257-297CODEN: ENRVEH; ISSN:1181-8700. (National Research Council of Canada)
    A review. Bioaccumulation assessment is important in the scientific evaluation of risks that chems. may pose to humans and the environment and is a current focus of regulatory effort. The status of bioaccumulation evaluations for org. chems. in aquatic systems is reviewed to reduce uncertainty in bioaccumulation measurement, to provide quality data for assessment, and to assist in model development. A review of 392 scientific literature and database sources includes 5317 bioconcn. factor (BCF) and 1656 bioaccumulation factor (BAF) values measured for 842 org. chems. in 219 aquatic species. A data quality assessment finds that 45% of BCF values are subject to at least one major source of uncertainty and that measurement errors generally result in an underestimation of actual BCF values. A case study of org. chems. on the Canadian Domestic Substances List indicates that empirical data are available for less than 4% of the chems. that require evaluation and of these chems., 76% have less than three acceptable quality BCF or BAF values. Field BAFs tend to be greater than lab. BCFs emphasizing the importance of environmental measurement for reliable assessment; however, only 0.2% of current use org. chems. have BAF measurements. Key parameters influencing uncertainty and variability in BCF and BAF data are discussed using reviewed data and models. A crit. evaluation of representative BCF and BAF models in relation to existing measurements and regulatory criteria in Canada indicate the probability of Type n errors, i.e., false negatives or "misses", using BCF models for bioaccumulation assessment may be as high as 70.6% depending on the model. Recommendations for the selection of measured and modelled values used in bioaccumulation assessment are provided, and improvements for the science and regulatory criteria are proposed.
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    Lucas, K.; Gaines, L. G. T.; Paris-Davila, T.; Nylander-French, L. A. Occupational Exposure and Serum Levels of Per- and Polyfluoroalkyl Substances (PFAS): A Review. American Journal of Industrial Medicine 2023, 66 (5), 379– 392,  DOI: 10.1002/ajim.23454
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    Woodcock, A. The Montreal Protocol: Getting over the Finishing Line?. Lancet. 2009, 373 (9665), 705– 706,  DOI: 10.1016/S0140-6736(09)60418-9
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    Zhang, J.; Zhang, Y.; Li, J.; Hu, J.; Ye, P.; Zeng, Z. Monitoring of Trifluoroacetic Acid Concentration in Environmental Waters in China. Water Res. 2005, 39 (7), 1331– 1339,  DOI: 10.1016/j.watres.2004.12.043
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    Monitoring of trifluoroacetic acid concentration in environmental waters in China
    Zhang, Jianbo; Zhang, Ying; Li, Jinlong; Hu, Jianxin; Ye, Peng; Zeng, Zheng
    Water Research (2005), 39 (7), 1331-1339CODEN: WATRAG; ISSN:0043-1354. (Elsevier B.V.)
    It is critically important and extremely meaningful to det. the concn. of trifluoroacetic acid (TFA) in the environmental water in China. This will create background ref. for the effects of analyzing the extensive employment of the substitutes to CFCs in China. In this paper a set of anal. methods was described for use in monitoring of TFA concn. of environmental waters including collecting, pre-treatment measures, preserving, concg. and derivatization of samples from different kinds of environmental waters. The GC with elec. capture detector (ECD) and headspace auto sampler were used in the anal. The lowest detection limit of the instrument is 0.0004 ng Me trifluoroacetic acid (MTFA), and the lowest detected concn. with the method is 3.0 ng/mL TFA. TFA collected in various environmental water samples (including rainfall, inland surface water, groundwater, and wastewater) from 9 provinces and autonomous regions in China were detd. by applying the anal. methods created and defined in this work. The concns. of TFA in 9 rainfalls and 3 snowfalls through the period from 2000-2001 ranged from 25 to 220 ng/L, the TFA concn. in the inland surface water samples ranged from 4.7 to 221 ng/L, the concn. of TFA in groundwater samples collected in Beijing was 10 ng/L, and the TFA concn. in coastal water samples ranged from 4.2-190.1 ng/L.
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  48. 48
    Zhai, Z.; Wu, J.; Hu, X.; Li, L.; Guo, J.; Zhang, B.; Hu, J.; Zhang, J. A 17-Fold Increase of Trifluoroacetic Acid in Landscape Waters of Beijing, China during the Last Decade. Chemosphere 2015, 129, 110– 117,  DOI: 10.1016/j.chemosphere.2014.09.033
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    A 17-fold increase of trifluoroacetic acid in landscape waters of Beijing, China during the last decade
    Zhai, Zihan; Wu, Jing; Hu, Xia; Li, Li; Guo, Junyu; Zhang, Boya; Hu, Jianxin; Zhang, Jianbo
    Chemosphere (2015), 129 (), 110-117CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
    The concns. of trifluoroacetic acid (TFA) were measured in urban landscape waters, tap water and snows in Beijing, China in 2012. Compared with the 2002 measurements, a 17-fold increase from 23-98 ng L-1 to 345-828 ng L-1 was obsd. for TFA concns. in urban landscape waters, and an obvious increase from not detected (n.d.) to 155 ng L-1 occurred to TFA in tap water. By flux estn. between air and water interface, the remarkable increase of TFA was attributable to dry and wet deposition. The quant. water-air-sediment interaction (QWASI) model simulated TFAs in various environmental media and showed that, over 99% of TFA distributed in water bodies. Our results recommend that measures are needed to control the increase of TFA in China.
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    Cahill, T. M. Increases in Trifluoroacetate Concentrations in Surface Waters over Two Decades. Environ. Sci. Technol. 2022, 56 (13), 9428– 9434,  DOI: 10.1021/acs.est.2c01826
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    Increases in trifluoroacetate concentrations in surface waters over two decades
    Cahill, Thomas M.
    Environmental Science & Technology (2022), 56 (13), 9428-9434CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)
    Trifluoroacetate (TFA) is a persistent perfluorinated alkanoic acid anion that has many anthropogenic sources, with fluorocarbon refrigerants being a major one. After an initial burst of research in the late 1990s and early 2000s, research on this ubiquitous pollutant declined as atm. emissions of the precursor compds. grew rapidly. Thus, there is little contemporaneous information about the concns. of TFA in the environment and how they have changed over time. This research detd. the change in TFA concns. in streams by resampling a transect that was originally sampled in 1998. The transect was designed to det. the regional distribution of TFA both upwind and downwind of major metropolitan areas in Northern California as well as a set of globally remote sites in Alaska. The results showed that TFA concns. increased by an av. of 6-fold over the intervening 23 years, which resulted in a median concn. of 180 ng/L (range 21.3-2790). The highest concns. were found in streams immediately downwind of the San Francisco Bay Area, while substantially lower concns. were found in the upwind, regionally remote, and globally remote sites. The C3 to C5 perfluorinated alkanoic acids were also investigated, but they were rarely detected with this methodol.
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    Freeling, F.; Scheurer, M.; Koschorreck, J.; Hoffmann, G.; Ternes, T. A.; Nödler, K. Levels and Temporal Trends of Trifluoroacetate (TFA) in Archived Plants: Evidence for Increasing Emissions of Gaseous TFA Precursors over the Last Decades. Environ. Sci. Technol. Lett. 2022, 9 (5), 400– 405,  DOI: 10.1021/acs.estlett.2c00164
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    50
    Levels and Temporal Trends of Trifluoroacetate (TFA) in Archived Plants: Evidence for Increasing Emissions of Gaseous TFA Precursors over the Last Decades
    Freeling, Finnian; Scheurer, Marco; Koschorreck, Jan; Hoffmann, Gabriele; Ternes, Thomas A.; Noedler, Karsten
    Environmental Science & Technology Letters (2022), 9 (5), 400-405CODEN: ESTLCU; ISSN:2328-8930. (American Chemical Society)
    Trifluoroacetate (TFA) is a highly mobile and persistent compd. that occurs ubiquitously in the environment. Results from previous studies suggested an increase in the atm. deposition of TFA in the Northern Hemisphere starting in the 1990s. Due to its physicochem. properties, TFA can be efficiently taken up and accumulated by vascular plants. Consequently, plants could serve as a biomonitoring tool to evaluate the presence of TFA in the terrestrial environment. This is the first study which describes the concns. and temporal trends of TFA in biota by analyzing archived leaf samples of various tree species from the German Environmental Specimen Bank (observation period: 1989-2020). Samples from different locations of the same species were each in a similar concn. range. The highest concns. (up to ∼1000μg/kg dry wt.) were found in Lombardy poplar (Populus nigra 'Italica') leaves. A statistically significant pos. trend in the TFA concn. within the study period was found for most species/sites, which is likely the result of both bioaccumulation as well as increasing emissions of gaseous TFA precursors over the last three decades. These results contribute to the current discussion on the regulation of per- and polyfluoroalkyl substances (PFAS) to protect human and environmental health.
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    Wang, B.; Yao, Y.; Wang, Y.; Chen, H.; Sun, H. Per- and Polyfluoroalkyl Substances in Outdoor and Indoor Dust from Mainland China: Contributions of Unknown Precursors and Implications for Human Exposure. Environ. Sci. Technol. 2022, 56 (10), 6036– 6045,  DOI: 10.1021/acs.est.0c08242
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    Per- and polyfluoroalkyl substances in outdoor and indoor dust from mainland China: contributions of unknown precursors and implications for human exposure
    Wang, Bin; Yao, Yiming; Wang, Yu; Chen, Hao; Sun, Hongwen
    Environmental Science & Technology (2022), 56 (10), 6036-6045CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)
    Per- and polyfluoroalkyl substances (PFASs) were analyzed in outdoor (n = 101) and indoor dust (n = 43, 38 paired with outdoors) samples across mainland China. From 2013 to 2017, the median concn. of .sum.PFASs in outdoor dust tripled from 63 to 164 ng/g with an elevated contribution of trifluoroacetic acid and 6:2 fluorotelomer alc. In 2017, the indoor dust levels of .sum.PFASs were in the range 185-913 ng/g, which were generally higher than the outdoor dust levels (105-321 ng/g). Emerging PFASs were found at high median levels of 5.7-97 ng/g in both indoor and outdoor dust samples. As first revealed by the total oxidized precursors assay, unknown perfluoroalkyl acid (PFAA)-precursors contributed 37-67 mol % to the PFAS profiles in indoor dust samples. A great proportion of C8 PFAA-precursors were precursors for perfluorooctanesulfonic acid, while C6 and C4 PFAA-precursors were mostly fluorotelomer based. Furthermore, daily perfluorooctanoic acid (PFOA) equiv. intakes of PFAAs (C4-C12) mixts. via indoor dust were first estd. at 1.3-1.5 ng/kg b.w./d for toddlers at high scenarios, which exceeds the derived daily threshold of 0.63 ng/kg b.w./d. from the European Food Safety Authority (EFSA). On this basis, an underestimation of 56%-69% likely remains without considering potential risks due to the biotransformation of unknown PFAA-precursors.
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    European Chemicals Agency (ECHA). ECHA Registration Dossier for Trifluoroacetic Acid. https://echa.europa.eu/de/registration-dossier/-/registered-dossier/5203/7/1 (accessed 2023–12–15).
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    Scheurer, M.; Nödler, K.; Freeling, F.; Janda, J.; Happel, O.; Riegel, M.; Müller, U.; Storck, F. R.; Fleig, M.; Lange, F. T.; Brunsch, A.; Brauch, H. J. Small, Mobile, Persistent: Trifluoroacetate in the Water Cycle – Overlooked Sources, Pathways, and Consequences for Drinking Water Supply. Water Res. 2017, 126, 460– 471,  DOI: 10.1016/j.watres.2017.09.045
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    Small, mobile, persistent: Trifluoroacetate in the water cycle - Overlooked sources, pathways, and consequences for drinking water supply
    Scheurer, Marco; Noedler, Karsten; Freeling, Finnian; Janda, Joachim; Happel, Oliver; Riegel, Marcel; Mueller, Uwe; Storck, Florian Ruediger; Fleig, Michael; Lange, Frank Thomas; Brunsch, Andrea; Brauch, Heinz-Juergen
    Water Research (2017), 126 (), 460-471CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)
    Elevated concns. of trifluoroacetate (TFA) of more than 100 μg/L in a major German river led to the occurrence of more than 20 μg/L TFA in bank filtration based tap waters. Several spatially resolved monitoring programs were conducted and discharges from an industrial company were identified as the point source of TFA contamination. Treatment options for TFA removal were investigated at full-scale waterworks and in lab. batch tests. Commonly applied techniques like ozonation or granulated activated carbon filtration are inappropriate for TFA removal, whereas TFA was partly removed by ion exchange and completely retained by reverse osmosis. Further investigations identified wastewater treatment plants (WWTPs) as addnl. TFA dischargers into the aquatic environment. TFA was neither removed by biol. wastewater treatment, nor by a retention soil filter used for the treatment of combined sewer overflows. WWTP influents can even bear a TFA formation potential, when appropriate CF3-contg. precursors are present. Biol. degrdn. and ozonation batch expts. with chems. of different classes (flurtamone, fluopyram, tembotrione, flufenacet, fluoxetine, sitagliptine and 4:2 fluorotelomer sulfonate) proved that there are yet overlooked sources and pathways of TFA, which need to be addressed in the future.
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    Scott, B. F.; Macdonald, R. W.; Kannan, K.; Fisk, A.; Witter, A.; Yamashita, N.; Durham, L.; Spencer, C.; Muir, D. C. G. Trifluoroacetate Profiles in the Arctic, Atlantic, and Pacific Oceans. Environ. Sci. Technol. 2005, 39 (17), 6555– 6560,  DOI: 10.1021/es047975u
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    Trifluoroacetate Profiles in the Arctic, Atlantic, and Pacific Oceans
    Scott, B. F.; MacDonald, R. W.; Kannan, K.; Fisk, A.; Witter, A.; Yamashita, N.; Durham, L.; Spencer, C.; Muir, D. C. G.
    Environmental Science and Technology (2005), 39 (17), 6555-6560CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    A series of depth profiles was collected at 22 sites in the Arctic, North and South Atlantic, and Pacific Oceans to det. spatial patterns for trifluoroacetate (TFA) concns. in the marine environment and to study possible natural sources of TFA. Profiles were also taken over underwater vents in the North and South Pacific and the Mediterranean Sea. At the profile sites, TFA was from <10 ng/L in the Pacific Ocean to >150 ng/L in the Atlantic Ocean. Samples from the Canada Basin of the Arctic Ocean exhibited variable TFA concns. (60-160 ng/L) down to 700 m. Below this depth, in water with 14C ages exceeding 1000 yr, the TFA concns. were const. (150 ng/L). Water returning to the Atlantic through the Canadian Arctic Archipelago had const. high TFA values. Profiles from the Northern Atlantic exhibited high values at all depths but were more consistent in the Western Atlantic. The northwestern Pacific Ocean surface profile sites exhibited low TFA concns. in the top 100 m increasing to a max. of 60 ng/L with depth. Samples from the South Pacific Ocean site had generally low values with a few depths (>800 m) having concns. of ≥50 ng/L. To det. if underwater vents could contribute to the TFA concns. in the oceans, profiles were taken over three vents in the Pacific and Mediterranean Oceans. The results suggest that some deep-sea vents may be natural sources of TFA.
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    Frank, H.; Christoph, E. H.; Holm-Hansen, O.; Bullister, J. L. Trifluoroacetate in Ocean Waters. Environ. Sci. Technol. 2002, 36 (1), 12– 15,  DOI: 10.1021/es0101532
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    Trifluoroacetate in Ocean Waters
    Frank, Hartmut; Christoph, Eugen H.; Holm-Hansen, Osmund; Bullister, John L.
    Environmental Science and Technology (2002), 36 (1), 12-15CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Trifluoroacetate (TFA) is a ubiquitous xenochem. presently increasing in concn. in some environmental compartments, esp. in the plant biomass of industrialized countries. Direct anthropogenic emissions of TFA are probably low, and the major anthropogenic sources are most likely various TFA precursors. As TFA has been found in ocean waters from remote locations, the question arose as to whether it is also a naturally occurring environmental chem. Detn. of the depth dependence of TFA in the ocean water column should shed some light on this question. However, in environmental anal. studies, the risk of systematic errors can be high and may lead to wrong conclusions. Therefore, special attention has been paid to the fact that TFA is a common atm. pollutant in the urban environment and that contributions from sampling, storage, and transport potentially lead to artificially high TFA values. The results of the ocean water sampling campaigns indicate that TFA is a naturally occurring chem., homogeneously distributed in ocean waters of all ages with a concn. of about 200 ng/L.
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    Zhang, L.; Sun, H.; Wang, Q.; Chen, H.; Yao, Y.; Zhao, Z.; Alder, A. C. Uptake Mechanisms of Perfluoroalkyl Acids with Different Carbon Chain Lengths (C2-C8) by Wheat (Triticum Acstivnm L.). Sci. Total Environ. 2019, 654, 19– 27,  DOI: 10.1016/j.scitotenv.2018.10.443
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    Uptake mechanisms of perfluoroalkyl acids with different carbon chain lengths (C2-C8) by wheat (Triticum aestivum L.)
    Zhang, Lu; Sun, Hongwen; Wang, Qi; Chen, Hao; Yao, Yiming; Zhao, Zhen; Alder, Alfredo C.
    Science of the Total Environment (2019), 654 (), 19-27CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)
    Org. compds. could be taken up by plants via different pathways, depending on chem. properties and biol. species, which is important for the risk assessment and risk control. To investigate the transport pathways of perfluoroalkyl acids (PFAAs) by wheat (Triticum acstivnm L.), the uptake of five perfluoroalkyl carboxylic acids (PFCAs): TFA (C2), PFPrA (C3), PFBA (C4), PFHxA (C6), PFOA (C8), and a perfluoroalkyl sulfonic acid: PFOS (C8) were studied using hydroponic expts. Various inhibitors including a metabolic inhibitor (Na3VO4), two anion channel blockers (9-AC, DIDS), and two aquaporin inhibitors (AgNO3, glycerol) were examd. The wheat root and shoot showed different concn. trends with the carbon chain length of PFAAs. The uptake of TFA was inhibited by Na3VO4 and 9-AC whereas PFPrA was inhibited by Na3VO4, AgNO3 and 9-AC. For the other four PFAAs, only Na3VO4 was effective. These results together with the result of concn.-dependent uptake, which followed the Michaelis-Menten model, indicate that the uptake of PFAAs by wheat is mainly an energy-dependent active process mediated by carriers. For the ultra-short chain PFCAs (C2 and C3), aquaporins and anion channels may also be involved. A competition between TFA and PFPrA was detd. during the plant uptake but no competition was obsd. between these two shorter chain analogs with other analogs, neither between PFBA and PFHxA, PFBA and PFBS, PFOA and PFOS.
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    Costello, M. C. S.; Lee, L. S. Sources, Fate, and Plant Uptake in Agricultural Systems of Per- and Polyfluoroalkyl Substances. Curr. Pollut Rep 2024, 10, 799– 819,  DOI: 10.1007/s40726-020-00168-y
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    Munoz, G.; Mercier, L.; Duy, S. V.; Liu, J.; Sauvé, S.; Houde, M. Bioaccumulation and Trophic Magnification of Emerging and Legacy Per- and Polyfluoroalkyl Substances (PFAS) in a St. Lawrence River Food Web. Environ. Pollut. 2022, 309, 119739  DOI: 10.1016/j.envpol.2022.119739
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    Bioaccumulation and trophic magnification of emerging and legacy per- and polyfluoroalkyl substances (PFAS) in a St. Lawrence River food web
    Munoz, Gabriel; Mercier, Laurie; Duy, Sung Vo; Liu, Jinxia; Sauve, Sebastien; Houde, Magali
    Environmental Pollution (Oxford, United Kingdom) (2022), 309 (), 119739CODEN: ENPOEK; ISSN:0269-7491. (Elsevier Ltd.)
    Research on per- and polyfluoroalkyl substances (PFAS) in freshwater ecosystems has focused primarily on legacy compds. and little is still known on the presence of emerging PFAS. Here, we investigated the occurrence of 60 anionic, zwitterionic, and cationic PFAS in a food web of the St. Lawrence River (Quebec, Canada) near a major metropolitan area. Water, sediments, aquatic vegetation, invertebrates, and 14 fish species were targeted for anal. Levels of perfluorobutanoic acid (PFBA) in river water exceeded those of perfluorooctanoic acid (PFOA) or perfluorooctane sulfonate (PFOS), and a zwitterionic betaine was obsd. for the first time in the St.Lawrence River. The highest mean PFAS concns. were obsd. for the benthopelagic top predator Smallmouth bass (Micropterus dolomieu, Σ60PFAS ∼ 92± 34 ng/g wet wt. whole-body) and the lowest for aquatic plants (0.52-2.3 ng/g). Up to 33 PFAS were detected in biotic samples, with frequent occurrences of emerging PFAS such as perfluorobutane sulfonamide (FBSA) and perfluoroethyl cyclohexane sulfonate (PFECHS), while targeted ether-PFAS all remained undetected. PFOS and long-chain perfluorocarboxylates (C10-C13 PFCAs) dominated the contamination profiles in biota except for insects where PFBA was predominant. Gammarids, molluscs, and insects also had frequent detections of PFOA and fluorotelomer sulfonates, an important distinction with fish and presumably due to different metab. Based on bioaccumulation factors >5000 and trophic magnification factors >1, long-chain (C10-C13) PFCAs, PFOS, perfluorodecane sulfonate, and perfluorooctane sulfonamide qualified as very bioaccumulative and biomagnifying. Newly monitored PFAS such as FBSA and PFECHS were biomagnified but moderately bioaccumulative, while PFOA was biodiluted.
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    Haukås, M.; Berger, U.; Hop, H.; Gulliksen, B.; Gabrielsen, G. W. Bioaccumulation of Per- and Polyfluorinated Alkyl Substances (PFAS) in Selected Species from the Barents Sea Food Web. Environ. Pollut. 2007, 148 (1), 360– 371,  DOI: 10.1016/j.envpol.2006.09.021
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    Bioaccumulation of per- and polyfluorinated alkyl substances (PFAS) in selected species from the Barents Sea food web
    Haukas, Marianne; Berger, Urs; Hop, Haakon; Gulliksen, Bjorn; Gabrielsen, Geir W.
    Environmental Pollution (Amsterdam, Netherlands) (2007), 148 (1), 360-371CODEN: ENPOEK; ISSN:0269-7491. (Elsevier B.V.)
    The present study reports concns. and biomagnification potential of per- and polyfluorinated alkyl substances (PFAS) in species from the Barents Sea food web. The examd. species included sea ice amphipod (Gammarus wilkitzkii), polar cod (Boreogadus saida), black guillemot (Cepphus grylle) and glaucous gull (Larus hyperboreus). These were analyzed for PFAS, polychlorinated biphenyls (PCBs), dichlorodiphenyltrichloroethanes (DDTs) and polybrominated di-Ph ethers (PBDEs). Perfluorooctane sulfonate (PFOS) was the predominant of the detected PFAS. Trophic levels and food web transfer of PFAS were detd. using stable nitrogen isotopes (δ 15N). No correlation was found between PFOS concns. and trophic level within species. However, a non-linear relationship was established when the entire food web was analyzed. Biomagnification factors displayed values >1 for perfluorohexane sulfonate (PFHxS), perfluorononanoic acid (PFNA), PFOS and ΣPFAS(7). Multivariate analyses showed that the degree of trophic transfer of PFAS is similar to that of PCB, DDT and PBDE, despite their accumulation through different pathways.
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    Drew, R.; Hagen, T. G.; Champness, D. Accumulation of PFAS by Livestock – Determination of Transfer Factors from Water to Serum for Cattle and Sheep in Australia. Food Additives & Contaminants: Part A 2021, 38 (11), 1897– 1913,  DOI: 10.1080/19440049.2021.1942562
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    Ghisi, R.; Vamerali, T.; Manzetti, S. Accumulation of Perfluorinated Alkyl Substances (PFAS) in Agricultural Plants: A Review. Environ. Res. 2019, 169, 326– 341,  DOI: 10.1016/j.envres.2018.10.023
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    Accumulation of perfluorinated alkyl substances (PFAS) in agricultural plants: A review
    Ghisi, Rossella; Vamerali, Teofilo; Manzetti, Sergio
    Environmental Research (2019), 169 (), 326-341CODEN: ENVRAL; ISSN:0013-9351. (Elsevier)
    PFASs are a class of compds. that include perfluoroalkyl and polyfluoroalkyl substances, some of the most persistent pollutants still allowed - or only partially restricted - in several product fabrications and industrial applications worldwide. PFASs have been shown to interact with blood proteins and are suspected of causing a no. of pathol. responses, including cancer. Given this threat to living organisms, we carried out a broad review of possible sources of PFASs and their potential accumulation in agricultural plants, from where they can transfer to humans through the food chain. Anal. of the literature indicates a direct correlation between PFAS concns. in soil and bioaccumulation in plants. Furthermore, plant uptake largely changes with chain length, functional group, plant species and organ. Low accumulations of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS) have been found in peeled potatoes and cereal seeds, while short-chain compds. can accumulate at high levels in leafy vegetables and fruits. Significant variations in PFAS buildup in plants according to soil amendment are also found, suggesting a particular interaction with soil org. matter. Here, we identify a series of challenges that PFASs pose to the development of a safe agriculture for future generations.
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    Mikkonen, A. T.; Martin, J.; Upton, R. N.; Moenning, J.-L.; Numata, J.; Taylor, M. P.; Roberts, M. S.; Mackenzie, L. Dynamic Exposure and Body Burden Models for Per- and Polyfluoroalkyl Substances (PFAS) Enable Management of Food Safety Risks in Cattle. Environ. Int. 2023, 180, 108218  DOI: 10.1016/j.envint.2023.108218
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    Salierno, G. On the Chemical Pathways Influencing the Effective Global Warming Potential of Commercial Hydrofluoroolefin Gases. ChemSusChem 2024, 1– 20,  DOI: 10.1002/cssc.202400280
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    Russell, M. H.; Hoogeweg, G.; Webster, E. M.; Ellis, D. A.; Waterland, R. L.; Hoke, R. A. TFA from HFO-1234yf: Accumulation and Aquatic Risk in Terminal Water Bodies. Environ. Toxicol. Chem. 2012, 31 (9), 1957– 1965,  DOI: 10.1002/etc.1925
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    TFA from HFO-1234yf: accumulation and aquatic risk in terminal water bodies
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    Environmental Toxicology and Chemistry (2012), 31 (9), 1957-1965CODEN: ETOCDK; ISSN:0730-7268. (Wiley-Blackwell)
    A next-generation mobile automobile air conditioning (MAC) refrigerant, HFO-1234yf (CF3CF=CH2), is being developed with improved environmental characteristics. In the atm., it ultimately forms trifluoroacetic acid (TFA(A); CF3COOH), which is subsequently scavenged by atm. pptn. and deposited on land and water as trifluoroacetate (TFA; CF3COO-). Trifluoroacetate is environmentally stable and has the potential to accumulate in terminal water bodies, i.e., aquatic systems receiving inflow but with little or no outflow and with high evapn. rates. Previous studies estd. HFO-1234yf emission rates and modeled its deposition concns. and TFA rates throughout North America. This work used multi-media and geog. information system-based modeling to assess potential TFA concns. in terminal water bodies over extended periods. After 10 years of emissions, predicted TFA concns. in North American terminal water bodies were estd. to be from current background concns. (0.01-0.22 μg/L) to 1-6 μg/L. After 50 years of continuous emissions, aquatic concns. of 1-15 μg/L are predicted, with extreme concns. of 50-200 μg/L in settings such as the Sonoran Desert along the California/Arizona border. Based on the relative insensitivity of aquatic organisms to TFA, predicted TFA concns. in terminal water bodies are not expected to impair aquatic systems, even considering potential emissions over extended periods.
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    Getting in control of persistent, mobile and toxic (PMT) and very persistent and very mobile (vPvM) substances to protect water resources: strategies from diverse perspectives
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    Environmental Sciences Europe (2022), 34 (1), 22CODEN: ESENCT; ISSN:2190-4715. (Springer)
    Safe and clean drinking water is essential for human life. Persistent, mobile and toxic (PMT) substances and/or very persistent and very mobile (vPvM) substances are an important group of substances for which addnl. measures to protect water resources may be needed to avoid neg. environmental and human health effects. PMT/vPvM substances do not sufficiently biodegrade in the environment, they can travel long distances with water and are toxic (those that are PMT substances) to the environment and/or human health. PMT/vPvM substance research and regulation is arguably in its infancy and in order to get in control of these substances the following (non-exhaustive list of) knowledge gaps should to be addressed: environmental occurrence; the suitability of currently available anal. methods; the effectiveness and availability of treatment technologies; the ability of regional governance and industrial stewardship to contribute to safe drinking water while supporting innovation; the ways in which policies and regulations can be used most effectively to govern these substances; and, the identification of safe and sustainable alternatives. The work is the outcome of the third PMT workshop, held in March 2021, that brought together diverse scientists, regulators, NGOs, and representatives from the water sector and the chem. sector, all concerned with protecting the quality of our water resources. The online workshop was attended by over 700 people. The knowledge gaps above were discussed in the presentations given and the attendees were invited to provide their opinions about knowledge gaps related to PMT/vPvM substance research and regulation. Strategies to closing the knowledge, tech. and practical gaps to get in control of PMT/vPvM substances can be rooted in the Chems. Strategy for Sustainability Towards a Toxic Free Environment from the European Commission, as well as recent advances in the research and industrial stewardship. Key to closing these gaps are: (i) advancing remediation and removal strategies for PMT/vPvM substances that are already in the environment, however this is not an effective long-term strategy; (ii) clear and harmonized definitions of PMT/vPvM substances across diverse European and international legislations; (iii) ensuring wider availability of anal. methods and ref. stds.; (iv) addressing data gaps related to persistence, mobility and toxicity of chem. substances, particularly transformation products and those within complex substance mixts.; and (v) advancing monitoring and risk assessment tools for stewardship and regulatory compliance. The two most effective ways to get in control were identified to be source control through risk governance efforts, and enhancing market incentives for alternatives to PMT/vPvM substances by using safe and sustainable by design strategies.
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    Cost Optimization of Osmotically Assisted Reverse Osmosis
    Bartholomew, Timothy V.; Siefert, Nicholas S.; Mauter, Meagan S.
    Environmental Science & Technology (2018), 52 (20), 11813-11821CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    We develop a nonlinear optimization model to identify min. cost designs for osmotically assisted reverse osmosis (OARO), a multistaged membrane-based process for desalinating high-salinity brines. The optimization model enables comprehensive evaluation of a complex process configuration and operational decision space that includes nonlinear process performance and implicit relationships among membrane stages, saline sweep cycles, and makeup, purge, and recycle streams. The objective function minimizes cost, rather than energy or capital expenditures, to accurately account for the trade-offs in capital and operational expenses inherent in multistaged membrane processes. Generally, we find that cost-optimal OARO processes minimize the no. of stages, eliminate the use of saline makeup streams, purge from the first sweep cycle, and successively decrease stage membrane area and sweep flow rates. The optimal OARO configuration for treating feed salinities of 50-125 g/L total dissolved solids with water recoveries between 30-70% results in costs less than or equal to $6 per m3 of product water. Sensitivity anal. suggests that future research to minimize OARO costs should focus on minimizing the membrane structural parameter while maximizing the membrane burst pressure and reducing the membrane unit cost.
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    Kim, J.; Park, K.; Yang, D. R.; Hong, S. A Comprehensive Review of Energy Consumption of Seawater Reverse Osmosis Desalination Plants. Appl. Energy 2019, 254, 113652  DOI: 10.1016/j.apenergy.2019.113652
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    A comprehensive review of energy consumption of seawater reverse osmosis desalination plants
    Kim, Jungbin; Park, Kiho; Yang, Dae Ryook; Hong, Seungkwan
    Applied Energy (2019), 254 (), 113652CODEN: APENDX; ISSN:0306-2619. (Elsevier Ltd.)
    A review. High specific energy consumption (SEC) is the main barrier for the expansion of seawater reverse osmosis (SWRO). Therefore, the main objective of current SWRO research is to lower the SEC of SWRO plants. However, SEC of SWRO plants has not been systemically explored or analyzed, despite the need for information to develop appropriate strategies to reduce SEC. Therefore, this study aims to review and analyze SWRO plants for a comprehensive understanding of their SEC. First, trends in SWRO application are investigated using more than 70 datasets on large-scale SWRO. The anal. explains the increasing no. of large-size SWRO plants, the SEC redn. by isobaric energy recovery devices (ERDs), and the use of different SWRO configurations to meet the energy and quality requirements. Factors assocd. with SEC (i.e., feed conditions, target conditions, and equipment efficiency) are also analyzed. High salinity increases energy demand, whereas the temp. effect on energy consumption is not entirely clear. High-efficiency ERDs and pumps can reduce SEC, but overall SEC cannot be explained by these factors alone. SEC is also affected by target water quality and quantity. Moreover, specific SWRO designs can improve the system to efficiently achieve the established goals. Furthermore, future directions to develop low-energy SWRO plants are discussed.
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    The Future of Seawater Desalination: Energy, Technology, and the Environment
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    A review. In recent years, numerous large-scale seawater desalination plants were built in water-stressed countries to augment available water resources, and construction of new desalination plants is expected to increase in the near future. Despite major advancements in desalination technologies, seawater desalination is still more energy intensive compared to conventional technologies for the treatment of fresh water. There are also concerns about the potential environmental impacts of large-scale seawater desalination plants. Here, the authors review the possible redns. in energy demand by state-of-the-art seawater desalination technologies, the potential role of advanced materials and innovative technologies in improving performance, and the sustainability of desalination as a technol. soln. to global water shortages.
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    Photolytic dissocn. of atm. CFCl3 and CF2Cl2 gives Cl which destroys the O3 layer. The halomethanes may remain at altitudes of 20-40 km for 40-150 yr and will reach satn. values of 10-30 times the present levels.
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    Holland, R.; Khan, M. A. H.; Driscoll, I.; Chhantyal-Pun, R.; Derwent, R. G.; Taatjes, C. A.; Orr-Ewing, A. J.; Percival, C. J.; Shallcross, D. E. Investigation of the Production of Trifluoroacetic Acid from Two Halocarbons, HFC-134a and HFO-1234yf and Its Fates Using a Global Three-Dimensional Chemical Transport Model. ACS Earth Space Chem. 2021, 5 (4), 849– 857,  DOI: 10.1021/acsearthspacechem.0c00355
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    Investigation of the production of trifluoroacetic acid from two halocarbons, HFC-134a and HFO-1234yf and its fates using a global three-dimensional chemical transport model
    Holland, Rayne; Khan, M. Anwar H.; Driscoll, Isabel; Chhantyal-Pun, Rabi; Derwent, Richard G.; Taatjes, Craig A.; Orr-Ewing, Andrew J.; Percival, Carl J.; Shallcross, Dudley E.
    ACS Earth and Space Chemistry (2021), 5 (4), 849-857CODEN: AESCCQ; ISSN:2472-3452. (American Chemical Society)
    Trifluoroacetic acid (TFA), a highly sol. and stable org. acid, is photochem. produced by certain anthropogenically emitted halocarbons such as HFC-134a and HFO-1234yf. Both these halocarbons are used as refrigerants in the automobile industry, and the high global warming potential of HFC-134a has promoted regulation of its use. Industries are transitioning to the use of HFO-1234yf as a more environmentally friendly alternative. We investigated the environmental effects of this change and found a 33-fold increase in the global burden of TFA from an annual value of 65 tonnes formed from the 2015 emissions of HFC-134a to a value of 2220 tonnes formed from an equiv. emission of HFO-1234yf. The percentage increase in surface TFA concns. resulting from the switch from HFC-134a to HFO-1234yf remains substantial with an increase of up to 250-fold across Europe. The increase in emissions greater than the current emission scenario of HFO-1234yf is likely to result in significant TFA burden as the atm. is not able to disperse and deposit relevant oxidn. products. The Criegee intermediate initiated loss process of TFA reduces the surface level atm. lifetime of TFA by up to 5 days (from 7 days to 2 days) in tropical forested regions.
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    Xie, G.; Cui, J.; Zhai, Z.; Zhang, J. Distribution Characteristics of Trifluoroacetic Acid in the Environments Surrounding Fluorochemical Production Plants in Jinan, China. Environmental Science and Pollution Research 2020, 27 (1), 983– 991,  DOI: 10.1007/s11356-019-06689-4
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    Distribution characteristics of trifluoroacetic acid in the environments surrounding fluorochemical production plants in Jinan, China
    Xie, Guiying; Cui, Jia'nan; Zhai, Zihan; Zhang, Jianbo
    Environmental Science and Pollution Research (2020), 27 (1), 983-991CODEN: ESPLEC; ISSN:0944-1344. (Springer)
    Trifluoroacetic acid (TFA) is a ubiquitous and extremely stable contaminant in the ambient environment and may be discharged during fluorochem. prodn. processes. However, the impacts of fluorochem. prodn. on surrounding areas have seldom been evaluated. We focused on Jinan, the capital of Shandong Province, China, and measured TFA levels in water, soil, and air samples. Our results showed that the av. TFA concns. in flowing water bodies were lower than those in landscape water bodies. The av. TFA concns. in soils were significantly higher than the background concn. As for atm. TFA levels, the mean concns. in the gas phase were higher than those in the particle phase, and av. daytime levels were slightly higher than nighttime levels. In addn., the quotient method was used to assess the ecol. risk of TFA in water in Jinan. The ratio of pollutant environmental concn. to predicted no-effect concn. (PEC/PNEC) for TFA was greater than 1, indicating that TFA does potentially damage the aquatic ecosystem of Jinan. Our findings suggest that TFA pollution around fluoride prodn. plants is a serious problem and that actions are required to avoid exacerbating the local ecol. and environmental risks of TFA.
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    The Aqueous Photolysis of TFM and Related Trifluoromethylphenols. An Alternate Source of Trifluoroacetic Acid in the Environment
    Ellis, David A.; Mabury, Scott A.
    Environmental Science and Technology (2000), 34 (4), 632-637CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    The lampricide 3-trifluoromethyl-4-nitrophenol (TFM) is added annually to the Great Lakes (∼50,000 Kg/yr), with treatment concns. 1-14 mg/L at source. TFM was shown to undergo photohydrolytic degrdn., at 365 nm and under actinic radiation, to produce trifluoroacetic acid (TFA). A mechanistic study for the prodn. of TFA from TFM was conducted, and the structural parameters assocd. with the prodn. of TFA from trifluoromethylated phenols were studied. It was found that the yield of TFA depended on the nature of the trifluoromethylated phenol. The nature of the substituents, the substitution pattern, and the pH strongly effected the photolytic half-life of the parent compd. and the yield of TFA. The half-life of TFM at 365 nm was 22 h (pH 9) and yielded 5.1% TFA, and 91.7 h at pH 7, yielding 17.8% TFA. Converting the nitro substituent of TFM to an amino group caused a decrease in the half-life to 2.3 min and yielded 11% TFA. The mechanism for the prodn. of TFA from TFM was deduced from the pH dependence and the effect of altering substituents on the trifluoromethylphenol. Ultimately, the formation of trifluoromethylquinone led to the quant. prodn. of TFA.
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    Joudan, S.; Gauthier, J.; Mabury, S. A.; Young, C. J. Aqueous Leaching of Ultrashort-Chain PFAS from (Fluoro)Polymers: Targeted and Nontargeted Analysis. Environ. Sci. Technol. Lett. 2024, 11 (3), 237– 242,  DOI: 10.1021/acs.estlett.3c00797
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    Cui, J.; Guo, J.; Zhai, Z.; Zhang, J. The Contribution of Fluoropolymer Thermolysis to Trifluoroacetic Acid (TFA) in Environmental Media. Chemosphere 2019, 222, 637– 644,  DOI: 10.1016/j.chemosphere.2019.01.174
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    The contribution of fluoropolymer thermolysis to trifluoroacetic acid (TFA) in environmental media
    Cui, Jia-nan; Guo, Junyu; Zhai, Zihan; Zhang, Jianbo
    Chemosphere (2019), 222 (), 637-644CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
    The source of trifluoroacetic acid (TFA) has long been a controversial issue. Fluoropolymer thermolysis is expected to be a potential anthropogenic source except for CFC alternatives. However, its TFA yield and contributions have rarely been reported more recently. In this study, we investigated the thermal properties of three kinds of fluoropolymers, including poly (vinylidene fluoride-co-hexafluropropylene) (PVDF-HFP), poly (vinylidene fluoride-co-chlorotrifluoroethylene) (PVDF-CTFE) and poly (tetrafluoroethylene) (PTFE). A lab. simulation expt. was then performed to analyze the TFA levels in the thermolysis products and hence to examine the TFA yields of these fluoropolymers. Thermolysis of these fluoropolymers occurred in the temp. ranges from ∼400°C to ∼650°C, with the peak wt. loss rate at around 550-600°C. TFA could be produced through fluoropolymer thermolysis when being heated to 500°C and above. Av. TFA yields of PTFE, PVDF-HFP and PVDF-CTFE were 1.2%, 0.9% and 0.3%, resp. Furthermore, the contribution of fluoropolymer thermolysis and CFC alternatives to rainwater TFA in Beijing, China was evaluated by using a Two-Box model. The degrdn. of fluoropolymers and HCFCs/HFCs could explain 37.9-43.4 ng L-1 rainwater TFA in Beijing in 2014. The thermolysis of fluoropolymers contributed 0.6-6.1 ng L-1 of rainwater TFA, accounting for 1.6-14.0% of the TFA burden from all the precursors which were considered here.
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    Martin, J. W.; Franklin, J.; Hanson, M. L.; Solomon, K. R.; Mabury, S. A.; Ellis, D. A.; Scott, B. F.; Muir, D. C. G. Detection of Chlorodifluoroacetic Acid in Precipitation: A Possible Product of Fluorocarbon Degradation. Environ. Sci. Technol. 2000, 34 (2), 274– 281,  DOI: 10.1021/es990935j
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    Detection of Chlorodifluoroacetic Acid in Precipitation: A Possible Product of Fluorocarbon Degradation
    Martin, Jonathan W.; Franklin, James; Hanson, Mark L.; Solomon, Keith R.; Mabury, Scott A.; Ellis, David A.; Scott, Brian F.; Muir, Derek C. G.
    Environmental Science and Technology (2000), 34 (2), 274-281CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    Chlorodifluoroacetic acid (CDFA) was detected in rain and snow samples from various regions of Canada. Routine quant. anal. was performed using an in-situ derivatization technique that allowed CDFA detn. by gas chromatog.-mass spectrometry of its anilide deriv. Validation of environmental CDFA was provided by strong anionic exchange chromatog. and detection by 19F NMR. CDFA concns. were <7.1-170 ng/L among all samples analyzed. Monthly vol.-weighted CDFA concns. in rain samples showed a seasonal trend between June and Nov. 1998, peaking in late summer and decreasing in fall for Guelph and Toronto sites. Preliminary toxicity tests with the aquatic macrophytes, Myriophyllum sibiricum and Myriophyllum spicatum, suggested CDFA does not represent a risk of acute toxicity to these aquatic macrophytes at current environmental concns. A degrdn. study suggested CDFA is recalcitrant to biotic and abiotic degrdn. relative to dichloroacetic acid (DCA) and may accumulate in the aquatic environment. Based on existing exptl. data, it is postulated that CDFA is a degrdn. product of CFC-113, and, to a lesser extent, HCFC-142b. If CFC-113 is a source, its O3 depletion potential may be lower than previously assumed.
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  92. 92
    Sun, M.; Cui, J.; Guo, J.; Zhai, Z.; Zuo, P.; Zhang, J. Fluorochemicals Biodegradation as a Potential Source of Trifluoroacetic Acid (TFA) to the Environment. Chemosphere 2020, 254, 126894  DOI: 10.1016/j.chemosphere.2020.126894
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    92
    Fluorochemicals biodegradation as a potential source of trifluoroacetic acid (TFA) to the environment
    Sun, Mei; Cui, Jia'nan; Guo, Junyu; Zhai, Zihan; Zuo, Peng; Zhang, Jianbo
    Chemosphere (2020), 254 (), 126894CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
    The anthropogenic release of trifluoroacetic acid (TFA) into the environmental media is not limited to photochem. oxidn. of CFC alternatives and industrial emissions. Biol. degrdn. of some fluorochems. is expected to be a potential TFA source. For the first time, we assess if the potential precursors [6:2 fluorotelomer alc. (6:2 FTOH), 4:2 fluorotelomer alc. (4:2 FTOH), acrinathrin, trifluralin, and 2-(trifluoromethyl)acrylic acid (TFMAA)] can be biol. degraded to TFA. Results show that 6:2 FTOH was terminally transformed to 5:3 polyfluorinated acid (5:3 FTCA; 12.5 mol%), perfluorohexanoic acid (PFHxA; 2.0 mol%), perfluoropentanoic acid (PFPeA; 1.6 mol%), perfluorobutyric acid (PFBA; 1.7 mol%), and TFA (2.3 mol%) by day 32 in the landfill soil microbial culture system. 4:2 FTOH could remove multiple -CF2 groups by microorganisms and produce PFPeA (2.6 mol%), PFBA (17.4 mol%), TFA (7.8 mol%). Furthermore, we basically analyzed the biodegrdn. contribution of short-chain FTOH as raw material residuals in com. products to the TFA burden in the environmental media. We est. global emission of 3.9-47.3 tonnes of TFA in the period from 1961 to 2019, and project 3.8-46.4 tonnes to be emitted from 2020 to 2040 via the pathway of 4:2 and 6:2 FTOH biodegrdn. (0.6-7.1 and 0.6-7.0 tonnes in China, resp.). Direct evidence of the expts. indicates that biodegrdn. of fluorochems. is an overlooked source of TFA and there are still some unspecified mech. of TFA prodn. pathways.
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    Björnsdotter, M. K.; Yeung, L. W. Y.; Kärrman, A.; Jogsten, I. E. Ultra-Short-Chain Perfluoroalkyl Acids Including Trifluoromethane Sulfonic Acid in Water Connected to Known and Suspected Point Sources in Sweden. Environ. Sci. Technol. 2019, 53 (19), 11093– 11101,  DOI: 10.1021/acs.est.9b02211
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    93
    Ultra-Short-Chain Perfluoroalkyl Acids Including Trifluoromethane Sulfonic Acid in Water Connected to Known and Suspected Point Sources in Sweden
    Bjornsdotter Maria K; Yeung Leo W Y; Karrman Anna; Jogsten Ingrid Ericson
    Environmental science & technology (2019), 53 (19), 11093-11101 ISSN:.
    Data presenting the environmental occurrence of ultra-short-chain perfluoroalkyl acids (PFAAs) are scarce and little is known about the potential sources. In this study, ultra-short-chain PFAAs were analyzed in water connected to potential point sources using supercritical fluid chromatography coupled with tandem mass spectrometry. Samples (n = 34) were collected in connection with firefighting training sites, landfills, and a hazardous waste management facility. Ultra-short-chain PFAAs were detected in all samples at concentrations up to 84 000 ng/L (.sum.C1-C3), representing up to 69% of the concentration of 29 per- and polyfluoroalkyl substances (PFASs). Trifluoroacetic acid (TFA), perfluoropropanoic acid (PFPrA), trifluoromethane sulfonic acid (TFMS), perfluoroethane sulfonic acid (PFEtS), and perfluoropropane sulfonic acid (PFPrS) were detected at concentrations up to 14 000, 53 000, 940, 1700, and 15 000 ng/L, respectively. Principal component analysis suggests that TFA is associated with landfills. PFPrS was associated with samples collected close to the source at all types of sites included in this study. These findings reveal the presence of high concentrations of ultra-short-chain PFAAs released into the environment from various sources and emphasize the large fraction of ultra-short-chain PFAAs to the total concentration of PFASs in water.
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    Wang, B.; Yao, Y.; Chen, H.; Chang, S.; Tian, Y.; Sun, H. Per- and Polyfluoroalkyl Substances and the Contribution of Unknown Precursors and Short-Chain (C2–C3) Perfluoroalkyl Carboxylic Acids at Solid Waste Disposal Facilities. Sci. Total Environ. 2020, 705, 135832  DOI: 10.1016/j.scitotenv.2019.135832
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    94
    Per- and polyfluoroalkyl substances and contribution of unknown precursors and short-chain (C2-C3) perfluoroalkyl carboxylic acids at solid waste disposal facilities
    Wang, Bin; Yao, Yiming; Chen, Hao; Chang, Shuai; Tian, Ying; Sun, Hongwen
    Science of the Total Environment (2020), 705 (), 135832CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)
    The emission of per- and polyfluoroalkyl substances (PFASs) from municipal solid wastes (MSW) disposal raises concerns for their potential of long-term release and risks. In this study, the occurrence of PFASs was investigated in ambient air and leachate from seven MSW disposal facilities including three landfills, two incineration plants, and two MSW transfer stations in Tianjin, China. Mass loads of PFASs (≥C4) released to the atm. were estd. at 0.007-0.97 kg/y/site, which were much lower than those to leachate (0.04-1.3 kg/y/site), while emission to the atm. at landfills was more considerable. With total oxidizable precursor (TOP) assay, unknown C4-C12 perfluoroalkyl acids (PFAAs)-precursors were found contributing 10-97 mol% in leachate and accounting for addnl. 15%-43% mass loads. Using IC-Ba/Ag/H cartridges, trifluoroacetic acid (C2) and perfluoropropionic acid (C3) were recovered in leachate for TOP assay (62%-78%) and detd. at dominant levels of 19-81μg/L, which accounted for mass loads of 0.08-2.6 kg/y/site. Unknown C2-C3 PFAA-precursors contributed 12-93 mol% with mass loads of 0.10-3.0 kg/y/site. Overall, unknown C2-C12 PFAA-precursors remained contributing 0.35-68 mol% in biochem. treated leachate. This study emphasizes that the profiles of unknown PFAA-precursors released during MSW disposal are to be identified, which is essential for their environmental risk assessment.
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    Tsou, K.; Antell, E.; Duan, Y.; Olivares, C. I.; Yi, S.; Alvarez-Cohen, L.; Sedlak, D. L. Improved Total Oxidizable Precursor Assay for Quantifying Polyfluorinated Compounds Amenable to Oxidative Conversion to Perfluoroalkyl Carboxylic Acids. ACS ES&T Water 2023, 3 (9), 2996– 3003,  DOI: 10.1021/acsestwater.3c00224
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    Joudan, S.; De Silva, A. O.; Young, C. J. Insufficient Evidence for the Existence of Natural Trifluoroacetic Acid. Environ. Sci. Process Impacts 2021, 23 (11), 1641– 1649,  DOI: 10.1039/D1EM00306B
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    Insufficient evidence for the existence of natural trifluoroacetic acid
    Joudan, Shira; De Silva, Amila O.; Young, Cora J.
    Environmental Science: Processes & Impacts (2021), 23 (11), 1641-1649CODEN: ESPICZ; ISSN:2050-7895. (Royal Society of Chemistry)
    Trifluoroacetic acid (TFA) is a persistent and mobile pollutant that is present ubiquitously in the environment. As a result of a few studies reporting its presence in pre-industrial samples and a purported unaccounted source, TFA is often claimed to exist naturally. Here, we examine the evidence for natural TFA by: (i) critically evaluating measurements of TFA in pre-industrial samples; (ii) examg. the likelihood of TFA formation by hypothesized mechanisms; (iii) exploring other potential TFA sources to the deep ocean; and (iv) examg. global budgets of TFA. We conclude that the presence of TFA in the deep ocean and lack of closed TFA budget is not sufficient evidence that TFA occurs naturally, esp. without a reasonable mechanism of formation. We argue the paradigm of natural TFA should no longer be carried forward.
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    Ellis, D. A.; Mabury, S. A.; Martin, J. W.; Muir, D. C. G. Thermolysis of Fluoropolymers as a Potential Source of Halogenated Organic Acids in the Environment. Nature 2001, 412 (6844), 321– 324,  DOI: 10.1038/35085548
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    Thermolysis of fluoropolymers as a potential source of halogenated organic acids in the environment
    Ellis, David A.; Mabury, Scott A.; Martin, Jonathan W.; Muir, Derek C. G.
    Nature (London, United Kingdom) (2001), 412 (6844), 321-324CODEN: NATUAS; ISSN:0028-0836. (Nature Publishing Group)
    Following the introduction of hydrochlorofluorocarbon (HCFCs) and hydrofluorocarbon (HFCs) gases as replacements for the ozone-destroying chlorofluorocarbons (CFCs), it has been discovered that HCFCs/HFCs can degrade in the atm. to produce trifluoroacetic acid, a compd. with no known loss mechanisms in the environment, and higher concns. in natural waters have been shown to be mildly phytotoxic. Present environmental levels of trifluooracetic acid are not accounted by HCFC/HFC degrdn. alone. Here we report that thermolysis of fluorinated polymers, such as the com. polymers Teflon and Kel-F, can also produce trifluoroacetate and the similar compd. chlorodifluoroacetate. This can occur either directly, or indirectly via products that are known to degrade to these haloacetates in the atm. The environmental significance of these findings is confirmed by modeling, which indicates that the thermolysis of fluoropolymers in industrial and consumer high-temp. applications (ovens, non-stick cooking utensils and combustion engines) is likely to be a significant source of trifluoroacetate in urban rainwater (∼25 ngL-1, as estd. for Toronto). Thermolysis also leads to longer chain polyfluoro- and/or polychlorofluoro-(C3-C14) carboxylic acids which may be equally persistent. Some of these products have recently been linked with possible adverse health and environmental impacts and are being phased out of the US market. Furthermore, we detected CFCs and fluorocarbons-groups that can destroy ozone and act as greenhouse gases, resp.-among the other thermal degrdn. products, suggesting that continued use of fluoropolymers may also exacerbate stratospheric ozone-depletion and global warming.
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    Duchesne, A. L.; Brown, J. K.; Patch, D. J.; Major, D.; Weber, K. P.; Gerhard, J. I. Remediation of PFAS-Contaminated Soil and Granular Activated Carbon by Smoldering Combustion. Environ. Sci. Technol. 2020, 54 (19), 12631– 12640,  DOI: 10.1021/acs.est.0c03058
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    Remediation of PFAS-contaminated soil and granular activated carbon by smoldering combustion
    Duchesne, Alexandra L.; Brown, Joshua K.; Patch, David J.; Major, David; Weber, Kela P.; Gerhard, Jason I.
    Environmental Science & Technology (2020), 54 (19), 12631-12640CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    This study explored smoldering combustion for remediating polyfluoroalkyl substance (PFAS)-impacted granular activated carbon (GAC) and PFAS-contaminated soil. GAC, both fresh and PFAS-loaded, was employed as the supplemental fuel supporting smoldering in mixts. with sand (≈175 mg PFAS/kg GAC-sand), with PFAS-spiked, lab.-constructed soil (≈4 mg PFAS/kg soil), and with a PFAS-impacted field soil (≈0.2 mg PFAS/kg soil). The fate of PFAS and fluorine was quantified with soil and emission analyses, including targeted PFAS and suspect screening as well as hydrogen fluoride and total fluorine. Results demonstrated that exceeding 35 g GAC/kg soil resulted in self-sustained smoldering with temps. exceeding 900°C. Post-treatment PFAS concns. of the treated soil were near (2 expts.) or below (7 expts.) detection limits (0.0004 mg/kg). Further, 44% of the initial PFAS on GAC underwent full destruction, compared to 16% of the PFAS on soil. Less than 1% of the initial PFAS contamination on GAC or soil was emitted as PFAS in the quantifiable anal. suite. Results suggest that the rest were emitted as altered, shorter-chain PFAS and volatile fluorinated compds., which were scrubbed effectively with GAC. Total org. fluorine anal. proved useful for PFAS-loaded GAC in sand; however, analyzing soils suffered from interference from non-PFAS. Overall, this study demonstrated that smoldering has significant potential as an effective remediation technique for PFAS-impacted soils and PFAS-laden GAC.
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    Trang, B.; Li, Y.; Xue, X.-S.; Ateia, M.; Houk, K. N.; Dichtel, W. R. Low-Temperature Mineralization of Perfluorocarboxylic Acids. Science (1979) 2022, 377 (6608), 839– 845,  DOI: 10.1126/science.abm8868
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    Nödler, K.; Scheurer, M. Substances from Multiple Sources (SMS): The Presence of Multiple Primary and Secondary Sources of Persistent and Mobile Organic Contaminants Is an Upcoming Challenge for the Drinking Water Sector and Regulatory Frameworks. Environ. Sci. Technol. 2019, 53 (19), 11061– 11062,  DOI: 10.1021/acs.est.9b05168
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    Hanson, M. L.; Madronich, S.; Solomon, K.; Sulbaek Andersen, M. P.; Wallington, T. J. Trifluoroacetic Acid in the Environment: Consensus, Gaps, and Next Steps. Environ. Toxicol. Chem. 2024, 43 (10), 2091– 2093,  DOI: 10.1002/etc.5963
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    Madronich, S.; Sulzberger, B.; Longstreth, J. D.; Schikowski, T.; Andersen, M. P. S.; Solomon, K. R.; Wilson, S. R. Changes in Tropospheric Air Quality Related to the Protection of Stratospheric Ozone in a Changing Climate. Photochemical & Photobiological Sciences 2023, 22 (5), 1129– 1176,  DOI: 10.1007/s43630-023-00369-6
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    Felizeter, S.; McLachlan, M. S.; De Voogt, P. Root Uptake and Translocation of Perfluorinated Alkyl Acids by Three Hydroponically Grown Crops. J. Agric. Food Chem. 2014, 62 (15), 3334– 3342,  DOI: 10.1021/jf500674j
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    Root uptake and translocation of perfluorinated alkyl acids by three hydroponically grown crops
    Felizeter, Sebastian; McLachlan, Michael S.; De Voogt, Pim
    Journal of Agricultural and Food Chemistry (2014), 62 (15), 3334-3342CODEN: JAFCAU; ISSN:0021-8561. (American Chemical Society)
    Tomato, cabbage, and zucchini plants were grown hydroponically in a greenhouse. They were exposed to 14 perfluorinated alkyl acids (PFAAs) at four different concns. via the nutrient soln. At maturity the plants were harvested, and the roots, stems, leaves, twigs (where applicable), and edible parts (tomatoes, cabbage head, zucchinis) were analyzed sep. Uptake and transfer factors were calcd. for all plant parts to assess PFAA translocation and distribution within the plants. Root concn. factors were highest for long-chain PFAAs (>C11) in all three plant species, but these chems. were not found in the edible parts. All other PFAAs were present in all above-ground plant parts, with transpiration stream concn. factors (TSCFs) of 0.05-0.25. These PFAAs are taken up with the transpiration stream and accumulate primarily in the leaves. Although some systematic differences were obsd., overall their uptake from nutrient soln. to roots and their further distribution within the plants were similar between plant species and among PFAAs.
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    Felizeter, S.; McLachlan, M. S.; De Voogt, P. Uptake of Perfluorinated Alkyl Acids by Hydroponically Grown Lettuce (Lactuca Sativa). Environ. Sci. Technol. 2012, 46 (21), 11735– 11743,  DOI: 10.1021/es302398u
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    112
    Uptake of Perfluorinated Alkyl Acids by Hydroponically Grown Lettuce (Lactuca sativa)
    Felizeter, Sebastian; McLachlan, Michael. S.; de Voogt, Pim
    Environmental Science & Technology (2012), 46 (21), 11735-11743CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
    An uptake study was carried out to assess the potential human exposure to perfluorinated alkyl acids (PFAAs) through the ingestion of vegetables. Lettuce (Lactuca sativa) was grown in PFAA-spiked nutrient solns. at four different concns., ranging from 10 ng/L to 10 μg/L. Eleven perfluorinated carboxylic acids (PFCAs) and three perfluorinated sulfonic acids (PFSAs) were analyzed by HPLC-MS/MS. At the end of the expt., the major part of the total mass of each of the PFAAs (except the short-chain, C4-C7, PFCAs) taken up by plants appeared to be retained in the nonedible part, viz. the roots. Root concn. factors (RCF), foliage/root concn. factors (FRCF), and transpiration stream concn. factors (TSCF) were calcd. For the long chained PFAAs, RCF values were highest, whereas FRCF were lowest. This indicates that uptake by roots is likely governed by sorption of PFAAs to lipid-rich root solids. Translocation from roots to shoots is restricted and highly depending on the hydrophobicity of the compds. Although the TSCF show that longer-chain PFCAs (e.g., perfluorododecanoic acid) get better transferred from the nutrient soln. to the foliage than shorter-chain PFCAs (e.g., perfluoroheptanoic acid), the major fraction of longer-chain PFCAs is found in roots due to addnl. adsorption from the spiked soln. Due to the strong electron-withdrawing effect of the fluorine atoms the role of the neg. charge of the dissocd. PFAAs is likely insignificant.
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    Gredelj, A.; Nicoletto, C.; Polesello, S.; Ferrario, C.; Valsecchi, S.; Lava, R.; Barausse, A.; Zanon, F.; Palmeri, L.; Guidolin, L.; Bonato, M. Uptake and Translocation of Perfluoroalkyl Acids (PFAAs) in Hydroponically Grown Red Chicory (Cichorium Intybus L.): Growth and Developmental Toxicity, Comparison with Growth in Soil and Bioavailability Implications. Science of The Total Environment 2020, 720, 137333  DOI: 10.1016/j.scitotenv.2020.137333
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    Hubert, M.; Arp, H. P. H.; Hansen, M. C.; Castro, G.; Meyn, T.; Asimakopoulos, A. G.; Hale, S. E. Influence of Grain Size, Organic Carbon and Organic Matter Residue Content on the Sorption of per- and Polyfluoroalkyl Substances in Aqueous Film Forming Foam Contaminated Soils - Implications for Remediation Using Soil Washing. Science of The Total Environment 2023, 875, 162668  DOI: 10.1016/j.scitotenv.2023.162668
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  • Abstract

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    Figure 1

    Figure 1. Comparison of TFA concentrations detected in different media summarized as before 2010 (green) and after 2010 (in red). Reported values of maximum concentrations found in the literature review are shown as vertical bars and mean values of reported monitoring means and medians are shown with overlapping dots. Numbers indicating the number of summarized individual data points are shown above the corresponding bars. In cases of either green or red bars and dots missing, data were not available for the given media and/or time frame. For air concentrations before 2010 only two studies were available, one of which reported only mean measured concentrations (see Table S1 for the full data set and Figure S3 for air data presented as concentrations from individual studies).

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    Hans Peter H. Arp

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    Hans Peter H. Arp, NGI, is an environmental chemist interested in how fundamental aspects of physical chemistry can be utilized as applied tools for understanding and preventing pollution exposure. His projects focus on designing solutions through policy mechanisms, chemical properties, interdisciplinary collaboration, and sustainable technologies to enable the circular economy and help create a zero-pollution society. He holds a PhD from ETH Zürich (2008) and a professorship at the Norwegian University of Science and Technology (since 2018). He is an Associate Editor for the journal Environmental Science: Processes and Impacts (since 2024).

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      Multimedia Distribution and Transfer of Per- and Polyfluoroalkyl Substances (PFAS) Surrounding Two Fluorochemical Manufacturing Facilities in Fuxin, China
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      Distribution and dry deposition of alternative and legacy perfluoroalkyl and polyfluoroalkyl substances in the air above the Bohai and Yellow Seas, China
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      A total of 26 alternative and legacy perfluoroalkyl and polyfluoroalkyl substances (PFASs) were investigated in air collected above the Bohai and Yellow Seas during a research cruise between June 28 and July 15, 2016. .sum.PFAS concns. ranged from 70 pg m-3 to 430 pg m-3 (mean 230 ± 100 pg m-3). Trifluoroacetic acid (TFA, mean 120 ± 80 pg m-3) and 8:2 fluorotelomer alc. (8:2 FTOH, mean 34 ± 46 pg m-3) were the predominating compds. of ionizable PFASs (i-PFASs) and neutral PFASs (n-PFASs), resp. The contributions of C4 and C6 i-PFASs were higher than those of C8 i-PFASs. Alternative substances, such as chlorinated 6:2 polyfluoroalkyl ether sulfonic acids (Cl-6:2 PFESA, mean 1.6 ± 1.2 pg m-3) and diPAPs (mean 1.6 ± 1.3 pg m-3), were only detected on the filter. The distribution coeff. of 10:2 FTOH was higher than 8:2 FTOH, which could be explained by the length of the carbon chain. The gas phase dry deposition velocities were simulated, and the values ranged from 0.08 ± 0.12 cm s-1 to 0.85 ± 0.28 cm s-1. For i-PFASs and diPAPs, the estd. fluxes of the particle phase were higher than those of the gas phase. For n-PFASs and TFA, the gas phase deposition played a key role. The .sum.PFASs dry deposition fluxes were 11-290 ng (m2 d)-1 (mean 72 ± 67 ng (m2 d)-1). The measurement of the concns. in the gas and particle phases simultaneously provided a more comprehensive understanding of PFAS behaviors in air.
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    7. 7
      Jordan, A.; Frank, H. Trifluoroacetate in the Environment. Evidence for Sources Other than HFC/HCFCs. Environ. Sci. Technol. 1999, 33 (4), 522– 527,  DOI: 10.1021/es980674y
      7
      Trifluoroacetate in the Environment. Evidence for Sources Other Than HFC/HCFCs
      Jordan, Armin; Frank, Hartmut
      Environmental Science and Technology (1999), 33 (4), 522-527CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      The partly halogenated C2-hydro(chloro)fluorocarbons (HFC, HCFC) 1,1,1-trifluoro-2,2-dichloroethane (HCFC-123), 1,1,1,2-tetrafluoro-2-chloroethane (HCFC-124), and 1,1,1,2-tetrafluoroethane (HFC-134a) are CFC substitutes found at increasing levels in the atm. Trifluoroacetate (TFA) is an atm. degrdn. product of these compds. and due to its persistence its potential accumulation in some aquatic ecosystems is a matter of environmental concern. This study was undertaken to det. the present-days base level of environmental TFA and whether model calcns. are in line with the actual data. Av. levels of ∼120 ng/L as predicted for the year 2010 are found in rain in Germany already, slightly higher than in rain collected in Switzerland or Nevada. In the major rivers in Germany, TFA is present at av. concns. of 140 ng/L. In air, levels of 45-60 pg/m3 have been found in Central Europe. Between Mar. 1995 and Sept. 1996, a period of substantial increase in atm. HFC-134a mixing ratio, the TFA concns. in air and pptn. did not significantly increase. TFA is absent in old groundwater samples and river water from remote locations, concns. are low. These data suggest that the total TFA in both compartments exceeds the formation potential of currently known sources, that TFA in atm. and rain is regionally assocd. with industrial or population d., and that other unresolved sources must contribute to the present concns.
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    8. 8
      Berends, A. G.; Boutonnet, J. C.; De Rooij, C. G.; Thompson, R. S. Toxicity of Trifluoroacetate to Aquatic Organisms. Environ. Toxicol. Chem. 1999, 18 (5), 1053– 1059,  DOI: 10.1002/etc.5620180533
      8
      Toxicity of trifluoroacetate to aquatic organisms
      Berends, Albert G.; Boutonnet, Jean Charles; de Rooij, Christ G.; Thompson, Roy S.
      Environmental Toxicology and Chemistry (1999), 18 (5), 1053-1059CODEN: ETOCDK; ISSN:0730-7268. (SETAC Press)
      As a result of the atm. degrdn. of several hydrofluorocarbons and hydrochlorofluorocarbons, trifluoroacetate (TFA) will be formed. Through pptn., TFA will enter aquatic ecosystems. To evaluate the impact on the aquatic environment, an aquatic toxicity testing program was carried out with sodium trifluoroacetate (NaTFA). During acute toxicity tests, no effects of NaTFA on water fleas (Daphnia magna) and zebra fish (Danio rerio) were found at a concn. of 1200 mg/L. A 7-d study with duckweed (Lemna gibba G3) revealed a NOEC of 300 mg/L. On the basis of the results of five toxicity tests with Selenastrum capricornutum, we detd. a NOEC of 0.12 mg/L. However, algal toxicity tests with NaTFA and Chlorella vulgaris, Scenedesmus subspicatus, Chlamydomonas reinhardtii, Dunaliella tertiolecta, Euglena gracilis, Phaeodactylum tricornutum, Navicula pelliculosa, Skeletonema costatum, Anabaena flos-aquae, and Microcystis aeruginosa resulted in EC50 values that were all higher than 100 mg/L. The toxicity of TFA to S. capricornutum could be due to metabolic defluorination to monofluoroacetate (MFA), which is known to inhibit the citric acid cycle. A toxicity test with MFA and S. capricornutum revealed it to be about three orders of magnitude more toxic than TFA. However, a bioactivation study revealed that defluorination of TFA was less than 4%. On the other hand, S. capricornutum exposed to a toxic concn. of NaTFA showed a recovery of growth when citric acid was added, suggesting that TFA (or a metabolite of TFA) interferes with the citric acid cycle. A recovery of the growth of S. capricornutum was also found when TFA was removed from the test solns. Therefore, TFA should be considered algistatic and not algicidic for S. capricornutum. On the basis of the combined results of the lab. tests and a previously reported semi-field study, we can consider a TFA concn. of 0.10 mg/L as safe for the aquatic ecosystem.
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    9. 9
      Boutonnet, J. C.; Bingham, P.; Calamari, D.; Rooij, C. de; Franklin, J.; Kawano, T.; Libre, J.-M.; McCul-loch, A.; Malinverno, G.; Odom, J. M.; Rusch, G. M.; Smythe, K.; Sobolev, I.; Thompson, R.; Tiedje, J. M. Environmental Risk Assessment of Trifluoroacetic Acid. Human and Ecological Risk Assessment: An International Journal 1999, 5 (1), 59– 124,  DOI: 10.1080/10807039991289644
      9
      Environmental risk assessment of trifluoroacetic acid
      Boutonnet, Jean Charles; Bingham, Pauline; Calamari, Davide; De Rooij, Christ; Franklin, James; Kawano, Toshihiko; Libre, Jean-Marie; McCulloch, Archie; Malinverno, Giuseppe; Odom, J. Martin; Rusch, George M.; Smythe, Katie; Sobolev, Igor; Thompson, Roy; Tiedje, James M.
      Human and Ecological Risk Assessment (1999), 5 (1), 59-124CODEN: HERAFR; ISSN:1080-7039. (CRC Press LLC)
      A review and discussion with many refs. The Montreal Protocol was developed in 1987 in response to concerns that the chlorofluorocarbons (CFCs) were releasing chlorine into the stratosphere and that this chlorine was causing a depletion of stratospheric ozone over Antarctica. This international agreement called for a phase out of these CFCs. Industry initiated a major effort to find replacements that are safe when properly used and safe to the environment. The toxicol. and environmental fate of these first generation replacements has been studied extensively. It was detd. that the new substances break down in the environment to give predominantly carbon dioxide, water and inorg. salts of chlorine and fluorine. The only exception is that some substances also break down to yield trifluoroacetic acid (HTFA), a substance resistant to further degrdn. Recognizing this, industry embarked on a research and assessment program to study the potential effects of trifluoroacetate (TFA) on the environment and to investigate possible degrdn. pathways. The results of these recently completed studies are summarized below and described in further detail in this paper. Trifluoroacetic acid is a strong org. acid with a pKa of 0.23. It is miscible with water and its low octanol/water partition coeff. (log Pow = -2.1) indicates no potential to bioaccumulate. Industrial use is limited and environmental releases are very low. Some addnl. TFA will be formed from the breakdown of a few halogenated hydrocarbons, most notably HFC-134a (CF3CH2F), HCFC-124 (CF3CHFCl), and HCFC-123 (CF3CHCl2). As these substances have only been produced in limited com. quantities, their contribution to environmental levels has been minimal. Surprisingly, environmental measurements in many of diverse locations show existing levels of 100 to 300 ng·l-1 in water with one site (Dead Sea) having a level of 6400 ng·l-1. These levels cannot be accounted for based on current atm. sources and imply a long-term, possibly pre-industrial source. Generally, soil retention of TFA is poor although soils with high levels of org. matter have been shown to have a greater affinity for TFA when contrasted to soils with low levels of org. matter. This appears to be an adsorption phenomenon, not irreversible binding. Therefore, TFA will not be retained in soil, but will ultimately enter the aq. compartment. Modeling of emission rates and subsequent conversion rates for precursors has led to ests. of max. levels of TFA in rain water in the region of 0.1 μg·l-1 in the year 2020. TFA is resistant to both oxidative and reductive degrdn. While there had been speculation regarding the possibility of TFA being degraded into monofluoroacetic acid (MFA), the rate of breakdown of MFA is so much higher than for TFA that any MFA formed would rapidly degrade. Therefore, there would be no buildup of MFA regardless of the levels of TFA present in the environment. Although highly resistant to microbial degrdn., there have been two reports of TFA degrdn. under anaerobic conditions. In the first study, natural sediments reduced TFA. However, even though this work was done in replicate, the investigators and others were unable to reproduce it in subsequent studies. In the second study, radiolabeled TFA was removed from a mixed anaerobic in vitro microcosm. Limited evidence of decarboxylation has also been reported for two strains of bacteria grown under highly specific conditions. TFA was not biodegraded in a semi-continuous activated sludge test even with prolonged incubation (up to 84 days). TFA does not accumulate significantly in lower aquatic life forms such as bacteria, small invertebrates, oligochaete worms and some aquatic plants including Lemna gibba (duckweed). Some bioaccumulation was obsd. in terrestrial higher plants, such as sunflower and wheat. This result appeared to be related to uptake with water and then concn. due to transpiration water loss. When transferred to clean hydroponic media, some elimination of TFA was seen. Also, more than 80% of the TFA in leaves was found to be water extractable, suggesting that no significant metab. of TFA had occurred. At an exposure level of 1200 mg·l-1 of sodium trifluoroacetate (NaTFA) - corresponding to 1000 mg·l-1 HTFA - no effects were seen on either Brachydanio rerio (a fish) or Daphnia magna (a water flea). With duckweed, mild effects were seen on frond increase and wt. increase at the same exposure level. At a concn. of 300 mg·l-1 no effects were obsd. Toxicity tests were conducted with 11 species of algae. For ten of these species the EC50 was greater than 100 mg·l-1. In Selenastrum capricornutum the no-effect level was 0.12 mg·l-1. At higher levels the effect was reversible. The reason for the unique sensitivity of this strain is unknown, but a recovery of the growth rate was seen when citric acid was added. This could imply a competitive inhibition of the citric acid cycle. The effect of TFA on seed germination and plant growth has been evaluated with a wide variety of plants. Application of NaTFA at 1000 mg·l-1 to seeds of sunflower, cabbage, lettuce, tomato, mung bean, soy bean, wheat, corn, oats and rice did not affect germination. Foliar application of a soln. of 100 mg·l-1 of NaTFA to field grown plants did not affect growth of sunflower, soya, wheat, maize, oilseed rape, rice and plantain. When plantain, wheat (varieties Katepwa and Hanno) and soya were grown in hydroponic systems contg. NaTFA, no effects were seen on plantain at 32 mg·l-1, on wheat (Katepwa) and soya at 1 mg·l-1, or on wheat (Hanno) at 10 mg·l-1; some effects on growth were seen at, resp., 100 mg·l-1, 5 mg·l-1, 5 mg·l-1, and 10 mg·l-1 and above. TFA is not metabolized in mammalian systems to any great extent. It is the major final metabolite of halothane, HCFC-123 and HCFC-124. The half-life of TFA in humans is 16 h. As expected, the acute oral toxicity of the free acid is higher than the one of the sodium salt. The inhalation LC50 (2 h exposure) for mice was 13.5 mg·l-1 (2900 ppm) and for rats it was 10 mg·l-1 (2140 ppm). Thus, TFA is considered to have low inhalation toxicity. The irritation threshold for humans was 54 ppm. As one would expect of a strong acid, it is a severe irritant to the skin and eye. When conjugated with protein, it has been shown to elicit an immunol. reaction; however, it is unlikely that TFA itself would elicit a sensitization response. Repeat administration of aq. solns. have shown that TFA can cause increased liver wt. and induction of peroxisomes. Relative to the doses (0.5% in diet or 150 mg·kg-1·day-1 by gavage) the effects are mild. In a series of Ames assays, TFA was reported to be non-mutagenic. Its carcinogenic potential has not been evaluated. Although TFA was shown to accumulate in amniotic fluid following exposure of pregnant animals to high levels of halothane (1200 ppm), no fetal effects were seen. Likewise, a reprodn. study that involved exposure of animals to halothane at levels up to 4000 ppm for 4 h per day, 7 days per wk, resulted in no adverse effects. Given the high levels of halothane exposure, it is unlikely that environmental TFA is a reproductive or developmental hazard. Overall the toxicity of TFA has been evaluated in stream mesocosms, algae, higher plants, fish, animals and humans. It has been found to be of very low toxicity in all of these systems. The lowest threshold for any effects was the reversible effect on growth of one strain of algae, Selenastrum capricornutum, which was seen at 0.12 mg·l-1. There is a 1000-fold difference between the no-effect concn. and the projected environmental levels of TFA from HFCs and HCFCs (0.0001 mg·l-1). Based on available data, one can conclude that environmental levels of TFA resulting from the breakdown of alternative fluorocarbons do not pose a threat to the environment.
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    10. 10
      Likens, G. E.; Tartowski, S. L.; Berger, T. W.; Richey, D. G.; Driscoll, C. T.; Frank, H. G.; Klein, A. Transport and Fate of Trifluoroacetate in Upland Forest and Wetland Ecosystems. Proc. Natl. Acad. Sci. U.S.A. 1997, 94 (9), 4499– 4503,  DOI: 10.1073/pnas.94.9.4499
      There is no corresponding record for this reference.
    11. 11
      Standley, L. J.; Bott, T. L. Trifluoroacetate, an Atmospheric Breakdown Product of Hydrofluorocarbon Refrigerants: Biomolecular Fate in Aquatic Organisms. Environ. Sci. Technol. 1998, 32 (4), 469– 475,  DOI: 10.1021/es970161b
      11
      Trifluoroacetate, an Atmospheric Breakdown Product of Hydrofluorocarbon Refrigerants: Biomolecular Fate in Aquatic Organisms
      Standley, Laurel J.; Bott, Thomas L.
      Environmental Science and Technology (1998), 32 (4), 469-475CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Aquatic organisms were monitored for their ability to incorporate trifluoroacetate (TFA), an atm. breakdown product of HFC and HCFC refrigerants contg. a trifluoromethyl moiety. Because of the structural similarity of TFA to acetate, a biochem. intermediate and microbial nutrient, we suspected that organisms might use the fluorinated compd. to synthesize biomols. such as lipids and acetylated proteins. We exposed aquatic organisms (microbial communities, oligochaetes, macroinvertebrates, Callitriche sp., Lemna sp., and Impatiens capensis) to radioactive TFA ([14C]F3COOH) and examd. them for distribution of radiolabel in different classes of biomols. The most label was found in oligochaetes and I. capensis leaves at 3 and 6 μg/g (as TFA), resp., with the greatest proportion found in the protein fraction for each sample type. Aerobic microorganisms incorporated only a small fraction of the label (a few nanograms per g as TFA), and the greatest proportion of label occurred in cell wall material. We have demonstrated that selected aquatic organisms spanning a range of trophic levels incorporated the xenobiotic TFA into their biomol. fractions so that it was no longer extd. as TFA and thus was metabolically transformed.
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    12. 12
      Wujcik, C. E.; Cahill, T. M.; Seiber, J. N. Determination of Trifluoroacetic Acid in 1996–1997 Precipitation and Surface Waters in California and Nevada. Environ. Sci. Technol. 1999, 33 (10), 1747– 1751,  DOI: 10.1021/es980697c
      12
      Determination of Trifluoroacetic Acid in 1996-1997 Precipitation and Surface Waters in California and Nevada
      Wujcik, Chad E.; Cahill, Thomas M.; Seiber, James N.
      Environmental Science and Technology (1999), 33 (10), 1747-1751CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      The atm. degrdn. of three chlorofluorocarbon (CFC) replacement compds., namely HFC-134a, HCFC-123, and HCFC-124, results in the formation of trifluoroacetic acid (TFA). Concns. of TFA were detd. in pptn. and surface water samples collected in California and Nevada during 1996-1997. Terminal lake systems were found to have concns. 4-13 times higher than their calcd. yearly inputs, providing evidence for accumulation. The results support dry deposition as the primary contributor of TFA to surface waters in arid and semiarid environments. Pptn. samples obtained from three different locations contained 20.7-1530 ng/L with significantly higher concns. in fogwater (median = 689 ng/L) over rainwater (median = 63.7 ng/L). Elevated levels of TFA were obsd. for rainwater collected in Nevada (median = 136 ng/L) over those collected in California (median = 49.5 ng/L), indicating continual uptake and concn. as clouds move from a semiarid to arid climate. Thus several mechanisms exist, including evaporative concn., vapor-liq. phase partitioning, lowered washout vols. of atm. deposition water, and dry deposition, which may lead to elevated concns. of TFA in atm. and surface waters above levels expected from usual rainfall washout.
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    13. 13
      Freeling, F.; Björnsdotter, M. K. Assessing the Environmental Occurrence of the Anthropogenic Contaminant Trifluoroacetic Acid (TFA). Current Opinion in Green and Sustainable Chemistry 2023, 41, 100807  DOI: 10.1016/j.cogsc.2023.100807
      There is no corresponding record for this reference.
    14. 14
      Zhang, W.; Liang, Y. The Wide Presence of Fluorinated Compounds in Common Chemical Products and the Environment: A Review. Environmental Science and Pollution Research 2023, 30 (50), 108393– 108410,  DOI: 10.1007/s11356-023-30033-6
      There is no corresponding record for this reference.
    15. 15
      Pickard, H. M.; Criscitiello, A. S.; Persaud, D.; Spencer, C.; Muir, D. C. G.; Lehnherr, I.; Sharp, M. J.; De Silva, A. O.; Young, C. J. Ice Core Record of Persistent Short-Chain Fluorinated Alkyl Acids: Evidence of the Impact From Global Environmental Regulations. Geophys. Res. Lett. 2020, 47 (10).  DOI: 10.1029/2020GL087535 .
      There is no corresponding record for this reference.
    16. 16
      Brunn, H.; Arnold, G.; Körner, W.; Rippen, G.; Steinhäuser, K. G.; Valentin, I. PFAS: Forever Chemicals─Persistent, Bioaccumulative and Mobile. Reviewing the Status and the Need for Their Phase out and Remediation of Contaminated Sites. Environmental Sciences Europe 2023, 35 (1), 20,  DOI: 10.1186/s12302-023-00721-8
      There is no corresponding record for this reference.
    17. 17
      Dekant, W.; Dekant, R. Mammalian Toxicity of Trifluoroacetate and Assessment of Human Health Risks Due to Environmental Exposures. Arch. Toxicol. 2023, 97 (4), 1069– 1077,  DOI: 10.1007/s00204-023-03454-y
      17
      Mammalian toxicity of trifluoroacetate and assessment of human health risks due to environmental exposures
      Dekant, Wolfgang; Dekant, Raphael
      Archives of Toxicology (2023), 97 (4), 1069-1077CODEN: ARTODN; ISSN:0340-5761. (Springer)
      Abstr.: While trifluoroacetic acid has limited tech. uses, the highly water-sol. trifluoroacetate (TFA) is reported to be present in water bodies at low concns. Most of the TFA in the environment is discussed to arise from natural processes, but also with the contribution from decompn. of environmental chems. The presence of TFA may result in human exposures. For hazard and risk assessment, the mammalian toxicity of TFA and human exposures are reviewed to assess the margin of exposures (MoE). The potential of TFA to induce acute toxicity is very low and oral repeated dose studies in rats have identified the liver as the target organ with mild liver hypertrophy as the lead effect. Biomarker analyses indicate that TFA is a weak peroxisome proliferator in rats. TFA administered to rats did not induce adverse effects in an extended one-generation study and in a developmental toxicity study or induce genotoxic responses. Based on recent levels of TFA in water and diet, MoEs for human exposures to TFA are well above 100 and do not indicate health risks.
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    18. 18
      Zheng, G.; Eick, S. M.; Salamova, A. Elevated Levels of Ultrashort- and Short-Chain Perfluoroalkyl Acids in US Homes and People. Environ. Sci. Technol. 2023, 57 (42), 15782– 15793,  DOI: 10.1021/acs.est.2c06715
      18
      Elevated Levels of Ultrashort- and Short-Chain Perfluoroalkyl Acids in US Homes and People
      Zheng, Guomao; Eick, Stephanie M.; Salamova, Amina
      Environmental Science & Technology (2023), 57 (42), 15782-15793CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)
      Per- and polyfluoroalkyl substances (PFAS) make up a large group of fluorinated org. compds. extensively used in consumer products and industrial applications. Perfluorooctanesulfonic acid (PFOS) and perfluorooctanoic acid (PFOA), the two perfluoroalkyl acids (PFAAs) with 8 carbons in their structure, were phased out on a global scale because of their high environmental persistence and toxicity. As a result, shorter-chain PFAAs with \<8 carbons in their structure are being used as their replacements and are now widely detected in the environment, raising concerns about their effects on the environment and human health. In this study, 47 PFAAs and their precursors were measured in paired samples of dust and drinking water collected from residential homes in Indiana, United States, and in blood and urine samples collected from the residents of these homes. Ultrashort- (with 2 or 3 carbons [C2-C3]) and short-chain (with 4-7 carbons [C4-C7]) PFAAs were the most abundant in all four matrixes and constituted on av. 69-100% of the total PFAA concns. Specifically, trifluoroacetic acid (TFA, C2) and perfluoropropanoic acid (PFPrA, C3) were the predominant PFAA congeners in most of the samples. Significant pos. correlations (n = 81; r = 0.23-0.42; p < 0.05) were found between TFA, perfluorobutanoic acid (PFBA, C4) and perfluoroheptanoic acid (PFHpA, C7) concns. in dust or water and those in serum, suggesting dust ingestion and/or drinking water consumption as important exposure pathways for these compds. This study demonstrates that ultrashort- and short-chain PFAAs are now abundant in the indoor environment and in people and warrants further research on potential adverse health effects of these exposures.
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    19. 19
      Solomon, K. R.; Velders, G. J. M.; Wilson, S. R.; Madronich, S.; Longstreth, J.; Aucamp, P. J.; Bornman, J. F. Sources, Fates, Toxicity, and Risks of Trifluoroacetic Acid and Its Salts: Relevance to Substances Regulated under the Montreal and Kyoto Protocols. Journal of Toxicology and Environmental Health - Part B: Critical Reviews 2016, 19 (7), 289– 304,  DOI: 10.1080/10937404.2016.1175981
      There is no corresponding record for this reference.
    20. 20
      Garavagno, M. d. l. A.; Holland, R.; Khan, M. A. H.; Orr-Ewing, A. J.; Shallcross, D. E. Trifluoroacetic Acid: Toxicity, Sources, Sinks and Future Prospects. Sustainability 2024, 16 (6), 2382,  DOI: 10.3390/su16062382
      There is no corresponding record for this reference.
    21. 21
      Hanson, M. L.; Solomon, K. R. Haloacetic Acids in the Aquatic Environment. Part I: Macrophyte Toxicity. Environ. Pollut. 2004, 130 (3), 371– 383,  DOI: 10.1016/j.envpol.2003.12.016
      There is no corresponding record for this reference.
    22. 22
      Kwiatkowski, C. F.; Andrews, D. Q.; Birnbaum, L. S.; Bruton, T. A.; DeWitt, J. C.; Knappe, D. R. U.; Maffini, M. V.; Miller, M. F.; Pelch, K. E.; Reade, A.; Soehl, A.; Trier, X.; Venier, M.; Wagner, C. C.; Wang, Z.; Blum, A. Response to “Comment on Scientific Basis for Managing PFAS as a Chemical Class.. Environ. Sci. Technol. Lett. 2021, 8 (2), 195– 197,  DOI: 10.1021/acs.estlett.1c00049
      There is no corresponding record for this reference.
    23. 23
      Singh, R. R.; Papanastasiou, D. K. Comment on “Scientific Basis for Managing PFAS as a Chemical Class.. Environmental Science and Technology Letters 2021, 8 (2), 192– 194,  DOI: 10.1021/acs.estlett.0c00765
      There is no corresponding record for this reference.
    24. 24
      Arp, H. P. H.; Kühnel, D.; Rummel, C.; MacLeod, M.; Potthoff, A.; Reichelt, S.; Rojo-Nieto, E.; Schmitt-Jansen, M.; Sonnenberg, J.; Toorman, E.; Jahnke, A. Weathering Plastics as a Planetary Boundary Threat: Exposure, Fate, and Hazards. Environ. Sci. Technol. 2021, 55 (11), 7246– 7255,  DOI: 10.1021/acs.est.1c01512
      24
      Weathering plastics as a planetary boundary threat: Exposure, fate, and hazards
      Arp, Hans Peter H.; Kuhnel, Dana; Rummel, Christoph; MacLeod, Matthew; Potthoff, Annegret; Reichelt, Sophia; Rojo-Nieto, Elisa; Schmitt-Jansen, Mechthild; Sonnenberg, Johanna; Toorman, Erik; Jahnke, Annika
      Environmental Science & Technology (2021), 55 (11), 7246-7255CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      We described in 2017 how weathering plastic litter in the marine environment fulfils two of three criteria to impose a planetary boundary threat related to "chem. pollution and the release of novel entities": planetary-scale exposure, which is not readily reversible. Whether marine plastics meet the third criterion, eliciting a disruptive impact on vital earth system processes, was uncertain. Since then, several important discoveries have been made to motivate a re-evaluation. A key issue is if weathering macroplastics, microplastics, nanoplastics, and their leachates have an inherently higher potential to elicit adverse effects than natural particles of the same size. We summarize novel findings related to weathering plastic in the context of the planetary boundary threat criteria that demonstrate increasing exposure, fate processes leading to poorly reversible pollution, and (eco)toxicol. hazards and their thresholds. We provide evidence that the third criterion could be fulfilled for weathering plastics in sensitive environments and therefore conclude that weathering plastics pose a planetary boundary threat. We suggest future research priorities to better understand (eco)toxicol. hazards modulated by increasing exposure and continuous weathering processes, to better parametrize the planetary boundary threshold for plastic pollution.
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    25. 25
      Persson, L. M.; Breitholtz, M.; Cousins, I. T.; De Wit, C. A.; MacLeod, M.; McLachlan, M. S. Confronting Unknown Planetary Boundary Threats from Chemical Pollution. Environ. Sci. Technol. 2013, 47 (22), 12619– 12622,  DOI: 10.1021/es402501c
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      Confronting Unknown Planetary Boundary Threats from Chemical Pollution
      Persson, Linn M.; Breitholtz, Magnus; Cousins, Ian T.; de Wit, Cynthia A.; MacLeod, Matthew; McLachlan, Michael S.
      Environmental Science & Technology (2013), 47 (22), 12619-12622CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Rockstroem et al. proposed a set of planetary boundaries that delimitate a safe operating space for humanity. One of the planetary boundaries is detd. by chem. pollution, however no clear definition was provided. Here, probably there is no single chem. pollution planetary boundary, but rather that many planetary boundary issues governed by chem. pollution exist. The authors identify three conditions that must be simultaneously met for chem. pollution to pose a planetary boundary threat. The authors then discuss approaches to identify chems. that could fulfill those conditions, and outline a proactive hazard identification strategy that considers long-range transport and the reversibility of chem. pollution.
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    26. 26
      MacLeod, M.; Breitholtz, M.; Cousins, I. T.; De Wit, C. A.; Persson, L. M.; Rudén, C.; McLachlan, M. S. Identifying Chemicals That Are Planetary Boundary Threats. Environ. Sci. Technol. 2014, 48 (19), 11057– 11063,  DOI: 10.1021/es501893m
      26
      Identifying chemicals that are planetary boundary threats
      MacLeod, Matthew; Breitholtz, Magnus; Cousins, Ian T.; Wit, Cynthia A. de; Persson, Linn M.; Ruden, Christina; McLachlan, Michael S.
      Environmental Science & Technology (2014), 48 (19), 11057-11063CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Rockstr.ovrddot.om et al. proposed a set of planetary boundaries that delimit a "safe operating space for humanity". Many of the planetary boundaries that have so far been identified are detd. by chem. agents. Other chem. pollution-related planetary boundaries likely exist, but are currently unknown. A chem. poses an unknown planetary boundary threat if it simultaneously fulfills three conditions: (1) it has an unknown disruptive effect on a vital Earth system process; (2) the disruptive effect is not discovered until it is a problem at the global scale, and (3) the effect is not readily reversible. In this paper, we outline scenarios in which chems. could fulfill each of the three conditions, then use the scenarios as the basis to define chem. profiles that fit each scenario. The chem. profiles are defined in terms of the nature of the effect of the chem. and the nature of exposure of the environment to the chem. Prioritization of chems. in commerce against some of the profiles appears feasible, but there are considerable uncertainties and scientific challenges that must be addressed. Most challenging is prioritizing chems. for their potential to have a currently unknown effect on a vital Earth system process. We conclude that the most effective strategy currently available to identify chems. that are planetary boundary threats is prioritization against profiles defined in terms of environmental exposure combined with monitoring and study of the biogeochem. processes that underlie vital Earth system processes to identify currently unknown disruptive effects.
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    27. 27
      Cousins, I. T.; Johansson, J. H.; Salter, M. E.; Sha, B.; Scheringer, M. Outside the Safe Operating Space of a New Planetary Boundary for Per- and Polyfluoroalkyl Substances (PFAS). Environ. Sci. Technol. 2022, 56 (16), 11172– 11179,  DOI: 10.1021/acs.est.2c02765
      27
      Outside the safe operating space of a new planetary boundary for per- and polyfluoroalkyl substances (PFAS)
      Cousins, Ian T.; Johansson, Jana H.; Salter, Matthew E.; Sha, Bo; Scheringer, Martin
      Environmental Science & Technology (2022), 56 (16), 11172-11179CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)
      A review. It is hypothesized that environmental contamination by per- and polyfluoroalkyl substances (PFAS) defines a sep. planetary boundary and that this boundary has been exceeded. This hypothesis is tested by comparing the levels of four selected perfluoroalkyl acids (PFAAs) (i.e., perfluorooctanesulfonic acid (PFOS), perfluorooctanoic acid (PFOA), perfluorohexanesulfonic acid (PFHxS), and perfluorononanoic acid (PFNA)) in various global environmental media (i.e., rainwater, soils, and surface waters) with recently proposed guideline levels. On the basis of the four PFAAs considered, it is concluded that (1) levels of PFOA and PFOS in rainwater often greatly exceed US Environmental Protection Agency (EPA) Lifetime Drinking Water Health Advisory levels and the sum of the aforementioned four PFAAs (Σ4 PFAS) in rainwater is often above Danish drinking water limit values also based on Σ4 PFAS; (2) levels of PFOS in rainwater are often above Environmental Quality Std. for Inland European Union Surface Water; and (3) atm. deposition also leads to global soils being ubiquitously contaminated and to be often above proposed Dutch guideline values. It is, therefore, concluded that the global spread of these four PFAAs in the atm. has led to the planetary boundary for chem. pollution being exceeded. Levels of PFAAs in atm. deposition are esp. poorly reversible because of the high persistence of PFAAs and their ability to continuously cycle in the hydrosphere, including on sea spray aerosols emitted from the oceans. Because of the poor reversibility of environmental exposure to PFAS and their assocd. effects, it is vitally important that PFAS uses and emissions are rapidly restricted.
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    28. 28
      Pike, K. A.; Edmiston, P. L.; Morrison, J. J.; Faust, J. A. Correlation Analysis of Perfluoroalkyl Substances in Regional U.S. Precipitation Events. Water Res. 2021, 190, 116685  DOI: 10.1016/j.watres.2020.116685
      28
      Correlation Analysis of Perfluoroalkyl Substances in Regional U.S. Precipitation Events
      Pike, Kyndal A.; Edmiston, Paul L.; Morrison, Jillian J.; Faust, Jennifer A.
      Water Research (2021), 190 (), 116685CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)
      Per- and polyfluoroalkyl substances (PFAS) are transported in the atm., leading to both wet and dry deposition to the surface. The concns. of 15 PFAS were measured at six locations in the Ohio-Indiana region of the U. S. during the summer of 2019 and compared to samples collected at a distant site in NW Wyoming. ΣPFAS concns. ranged from 50-850 ng L-1, with trifluoroacetic acid (TFA) being the dominant compd. (∼90%). Concns. of perfluorooctanoic acid (PFOA) and perfluorosulfonic acid (PFOS) were similar to amts. obsd. over the past 20 years, indicating persistence in the atm. despite regulatory action, and the newer species HFPO-DA (GenX) was also widely detected in rainwater. ANOVA modeling and correlation matrixes were used to det. assocn. of PFAS concns., location, and functional group and chain length. Statistically significant differences (p < 0.05) in PFAS profiles across sites sepd. by 10-100 km indicate that local point sources strongly contribute to wet deposition. This work introduces correlation plots for PFAS that allow rapid visual comparison of multi-analyte and multi-site data sets.
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    29. 29
      Freeling, F.; Behringer, D.; Heydel, F.; Scheurer, M.; Ternes, T. A.; Nödler, K. Trifluoroacetate in Precipitation: Deriving a Benchmark Data Set. Environ. Sci. Technol. 2020, 54 (18), 11210– 11219,  DOI: 10.1021/acs.est.0c02910
      29
      Trifluoroacetate in precipitation: Deriving a benchmark data set
      Freeling, Finnian; Behringer, David; Heydel, Felix; Scheurer, Marco; Ternes, Thomas A.; Noedler, Karsten
      Environmental Science & Technology (2020), 54 (18), 11210-11219CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Although pptn. is considered to be the most important diffuse source of trifluoroacetate (TFA) to the nonmarine environment, information regarding the wet deposition of TFA as well as general data on the spatial and temporal variations in TFA concn. in pptn. is scarce. This is the first study to provide a comprehensive overview of the occurrence of TFA in pptn. by a systematic and nation-wide field monitoring campaign. In total, 1187 pptn. samples, which were collected over the course of 12 consecutive months at eight locations across Germany, were analyzed. The median, the estd. av., and the pptn.-weighted av. of the TFA concn. of all analyzed wet deposition samples were 0.210, 0.703, and 0.335μg/L, resp. For Germany, an annual wet deposition flux of 190μg/m2 or approx. 68 t was calcd. for the sampling period from Feb. 2018 to Jan. 2019. The campaign revealed a pronounced seasonality of the TFA concn. and wet deposition flux of collected samples. Correlation anal. suggested an enhanced transformation of TFA precursors in the troposphere in the summertime due to higher concns. of photochem. generated oxidants such as hydroxyl radicals, ultimately leading to an enhanced atm. deposition of TFA during summer.
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    30. 30
      Scheurer, M.; Nödler, K. Ultrashort-Chain Perfluoroalkyl Substance Trifluoroacetate (TFA) in Beer and Tea – An Unintended Aqueous Extraction. Food Chem. 2021, 351, 129304  DOI: 10.1016/j.foodchem.2021.129304
      30
      Ultrashort-chain perfluoroalkyl substance trifluoroacetate (TFA) in beer and tea - An unintended aqueous extraction
      Scheurer, Marco; Noedler, Karsten
      Food Chemistry (2021), 351 (), 129304CODEN: FOCHDJ; ISSN:0308-8146. (Elsevier Ltd.)
      Trifluoroacetate (TFA) is an ultrashort-chain perfluoroalkyl substance, which is ubiquitously present in the aq. environment. Due to its high mobility, it accumulates in plant material. The study presented here shows for the first time that TFA is a widely spread contaminant in beer and tea / herbal infusions. In 104 beer samples from 23 countries, TFA was detected up to 51μg/L with a median concn. of 6.1μg/L. An indicative brewing test and a correlation approach with potassium (K) indicate that the main source of TFA in beer is most likely the applied malt. It could be proven that the impact of the applied water is negligible in terms of TFA, which was supported by the anal. of numerous tap water samples from different countries. The unintended extn. of TFA was also demonstrated for tea / herbal infusions with a median concn. of 2.4μg/L.
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    31. 31
      The European Parliament and the Council of the European Union. Directive (EU) 2020/2184 of the European Parliament and of the Council of 16 December 2020 on the Quality of Water Intended for Human Consumption (Recast) (Text with EEA Relevance); EU, 2020; pp 1– 62. https://eur-lex.europa.eu/eli/dir/2020/2184/oj (accessed 2024–05–22).
      There is no corresponding record for this reference.
    32. 32
      GLOBAL 2000; Friends of the Earth Austria; Pesticide Action Network Europe (PAN Europe); Generations Futures. TFA in Water, Dirty PFAS Legacy Under the Radar ; 2024; pp 1– 23 https://www.pan-europe.info/resources/reports/2024/05/tfa-water-dirty-pfas-legacy-under-radar (accessed 2024–05–31).
      There is no corresponding record for this reference.
    33. 33
      Meier, S.; Brodmann, P.; Weber, S.; Moschet, C.; Gelmi, T.; Lacour, W.; Steinmann, J.. TRINKWASSERQUALITÄT BEZÜGLICH DER PFAS-RÜCKSTÄNDE , 2024; pp 6 https://www.aquaetgas.ch/wasser/trinkwasser/20240228_ag3_trinkwasserqualit%C3%A4t-bez%C3%BCglich-der-pfas-r%C3%BCckst%C3%A4nde/ (accessed 2024–08–20).
      There is no corresponding record for this reference.
    34. 34
      Wang, W.; Rhodes, G.; Ge, J.; Yu, X.; Li, H. Uptake and Accumulation of Per- and Polyfluoroalkyl Substances in Plants. Chemosphere 2020, 261, 127584  DOI: 10.1016/j.chemosphere.2020.127584
      34
      Uptake and accumulation of per- and polyfluoroalkyl substances in plants
      Wang, Wenfeng; Rhodes, Geoff; Ge, Jing; Yu, Xiangyang; Li, Hui
      Chemosphere (2020), 261 (), 127584CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
      Per- and polyfluoroalkyl substances (PFASs) are a class of persistent org. contaminants that are ubiquitous in the environment and have been found to be accumulated in agricultural products. Consumption of PFAS-contaminated agricultural products represents a feasible pathway for the trophic transfer of these toxic chems. along food chains/webs, leading to risks assocd. with human and animal health. Recently, studies on plant uptake and accumulation of PFASs have rapidly increased; consequently, a review to summarize the current knowledge and highlight future research is needed. Anal. of the publications indicates that a large variety of plant species can take up PFASs from the environment. Vegetables and grains are the most commonly investigated crops, with perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS) as the most studied PFASs. The potential sources of PFASs for plant uptake include industrial emissions, irrigation with contaminated water, land application of biosolids, leachates from landfill sites, and pesticide application. Root uptake is the predominant pathway for the accumulation of PFASs in agricultural crops, and uptake by plant aboveground portions from the ambient atm. could play a minor role in the overall PFAS accumulation. PFAS uptake by plants is influenced by physicochem. properties of compds. (e.g., perfluorocarbon chain length, head group functionality, water soly., and volatility), plant physiol. (e.g., transpiration rate, lipid and protein content), and abiotic factors (e.g., soil org. matters, pH, salinity, and temp.). Based on literature anal., the current knowledge gaps are identified, and future research prospects are suggested.
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    35. 35
      Ghisi, R.; Vamerali, T.; Manzetti, S. Accumulation of Perfluorinated Alkyl Substances (PFAS) in Agricultural Plants: A Review. Environ. Res. 2019, 169, 326– 341,  DOI: 10.1016/j.envres.2018.10.023
      35
      Accumulation of perfluorinated alkyl substances (PFAS) in agricultural plants: A review
      Ghisi, Rossella; Vamerali, Teofilo; Manzetti, Sergio
      Environmental Research (2019), 169 (), 326-341CODEN: ENVRAL; ISSN:0013-9351. (Elsevier)
      PFASs are a class of compds. that include perfluoroalkyl and polyfluoroalkyl substances, some of the most persistent pollutants still allowed - or only partially restricted - in several product fabrications and industrial applications worldwide. PFASs have been shown to interact with blood proteins and are suspected of causing a no. of pathol. responses, including cancer. Given this threat to living organisms, we carried out a broad review of possible sources of PFASs and their potential accumulation in agricultural plants, from where they can transfer to humans through the food chain. Anal. of the literature indicates a direct correlation between PFAS concns. in soil and bioaccumulation in plants. Furthermore, plant uptake largely changes with chain length, functional group, plant species and organ. Low accumulations of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS) have been found in peeled potatoes and cereal seeds, while short-chain compds. can accumulate at high levels in leafy vegetables and fruits. Significant variations in PFAS buildup in plants according to soil amendment are also found, suggesting a particular interaction with soil org. matter. Here, we identify a series of challenges that PFASs pose to the development of a safe agriculture for future generations.
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    36. 36
      Gredelj, A.; Polesel, F.; Trapp, S. Model-Based Analysis of the Uptake of Perfluoroalkyl Acids (PFAAs) from Soil into Plants. Chemosphere 2020, 244, 125534  DOI: 10.1016/j.chemosphere.2019.125534
      36
      Model-based analysis of the uptake of perfluoroalkyl acids (PFAAs) from soil into plants
      Gredelj, Andrea; Polesel, Fabio; Trapp, Stefan
      Chemosphere (2020), 244 (), 125534CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
      Perfluoroalkyl acids (PFAAs) bioaccumulate in crops, with uptake being particularly high for short-chain PFAAs that are constantly transported with transpiration water to aerial plant parts. Due to their amphiphilic surfactant nature and ionized state at environmental pH, predicting the partitioning behavior of PFAAs is difficult and subject to considerable uncertainty, making exptl. data highly desirable. Here, we applied a plant uptake model that combines advective flux with measured partition coeffs. to reproduce the set of empirically derived plant uptake and soil-partitioning data for nine PFAAs in red chicory, in order to improve the mechanistic understanding and provide new insights into the complex uptake processes. We introduced a new parameter for retarded uptake (R) to explain the slow transfer of PFAA across biomembranes of the root epidermis, which has led to low transpiration stream concn. factors (TSCFs) presented in literature so far. We estd. R values for PFAAs using exptl. data derived for red chicory and used the modified plant uptake model to simulate uptake of PFAA into other crops. Results show that this semi-empirical model predicted PFAAs transport to shoots and fruits with good accuracy based on exptl. root to soil concn. factors (RCFdw) and soil to water partition coeffs. (Kd) as well as estd. R values and plant-specific data for growth and transpiration. It can be concluded that the combination of rather low Kd with high RCFdw and the absence of any relevant loss are the reason for the obsd. excellent plant uptake of PFAAs.
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    37. 37
      Lesmeister, L.; Lange, F. T.; Breuer, J.; Biegel-Engler, A.; Giese, E.; Scheurer, M. Extending the Knowledge about PFAS Bioaccumulation Factors for Agricultural Plants – A Review. Sci. Total Environ. 2021, 766, 142640  DOI: 10.1016/j.scitotenv.2020.142640
      37
      Extending the knowledge about PFAS bioaccumulation factors for agricultural plants - A review
      Lesmeister, Lukas; Lange, Frank Thomas; Breuer, Joern; Biegel-Engler, Annegret; Giese, Evelyn; Scheurer, Marco
      Science of the Total Environment (2021), 766 (), 142640CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)
      A review. A main source of perfluoroalkyl and polyfluoroalkyl substances (PFASs) residues in agricultural plants is their uptake from contaminated soil. Bioaccumulation factors (BAFs) can be an important tool to derive recommendations for cultivation or handling of crops prior consumption. This review compiles >4500 soil-to-plant BAFs for 45 PFASs from 24 studies involving 27 genera of agricultural crops. Grasses (Poaceae) provided most BAFs with the highest no. of values for perfluorooctanoic acid and perfluorooctane sulfonic acid. Influencing factors on PFAS transfer like compd.-specific properties (hydrophobicity, chain length, functional group, etc.), plant species, compartments, and other boundary conditions are critically discussed. Throughout the literature, BAFs were higher for vegetative plant compartments than for reproductive and storage organs. Decreasing BAFs per addnl. perfluorinated carbon were clearly apparent for aboveground parts (up to 1.16 in grains) but not always for roots (partly down to zero). Combining all BAFs per single perfluoroalkyl carboxylic acid (C4-C14) and sulfonic acid (C4-C10), median log BAFs decreased by -0.25(±0.029) and -0.24(±0.013) per fluorinated carbon, resp. For the first time, the plant uptake of ultra-short-chain (≤ C3) perfluoroalkyl acids (PFAAs) was reviewed and showed a ubiquitous occurrence of trifluoroacetic acid in plants independent from the presence of other PFAAs. Based on identified knowledge gaps, it is suggested to focus on the uptake of precursors to PFAAs, PFAAs ≤C3, and addnl. emerging PFASs such as GenX or fluorinated ethers in future research. Studies regarding the uptake of PFASs by sugar cane, which accounts for about one fifth of the global crop prodn., are completely lacking and are also recommended. Furthermore, aq. soil leachates should be tested as an alternative to the solvent extn. of soils as a base for BAF calcns.
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    38. 38
      Scott, B. F.; Spencer, C.; Martin, J. W.; Barra, R.; Bootsma, H. A.; Jones, K. C.; Johnston, A. E.; Muir, D. C. G. Comparison of Haloacetic Acids in the Environment of the Northern and Southern Hemispheres. Environ. Sci. Technol. 2005, 39 (22), 8664– 8670,  DOI: 10.1021/es050118l
      38
      Comparison of Haloacetic Acids in the Environment of the Northern and Southern Hemispheres
      Scott, B. F.; Spencer, C.; Martin, J. W.; Barra, R.; Bootsma, H. A.; Jones, K. C.; Johnston, A. E.; Muir, D. C. G.
      Environmental Science and Technology (2005), 39 (22), 8664-8670CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Haloacetic acids (HAAs) are a family of compds. whose environmental concns. have been extensively studied, primarily in Europe. Depending on the compd., their sources are believed to be both natural and anthropogenic. To better understand possible sources and contribute to the knowledge of the global distribution of these compds., esp. between the Northern and Southern Hemispheres, samples of pptn., soils, and conifer needles were collected from Canada, Malawi, Chile, and the U.K. Pptn. samples exhibited highest HAA concns. in collections from Canada, and lowest in those from Malawi. Malawi samples contained measurable levels of monobromoacetic acid (MBA) (56 ng/L) unlike those from most other locations (<9 ng/L). Soil HAA concn. levels were highest in the U.K. (e.g., 7.3 ng/g av. TCA) and lowest in Malawi (0.8 ng/g av. TCA), with Chile having higher levels (4.8 ng/g av. TCA) than Canada (3 ng/g av. TCA). Malawi soils contained small amts. of MBA (2 ng/g), in common with the two most southern of the 11 Chilean sites. Anal. of soil cores (10-cm depth sliced at 1 cm) from sites in Malawi and Chile showed that trichloroacetic acid (TCA) generally declined with depth while mono- and dichloroacetic acid (MCA and DCA) showed no trend. MCA, DCA, and TCA concns. in archived U.K. Soil samples increased by factors of 2, 4, and 5-fold over 75 years while TFA showed no consistent trend. Monochloroacetic acid (MCA) was detected in pine needles collected from Malawi. U.K. Needle samples had the highest concns. of all chloroacetic acids (CAAs): MCA, 2-18 ng/g; dichloroacetic acid (DCA), 2-38 ng/g; and trichloroacetic acid (TCA), 28-190 ng/g. Conifer needles from Canada and Chile contained CAAs at levels ranging from <2 to 16 ng/g wet wt. Trifluoroacetic acid concns. generally declined with increasing elevation in the samples from the Rocky Mountains in western Canada. The results indicate that concns. of HAAs are greatest in the industrialized Northern Hemisphere but there are significant amts. of these compds. in the less industrialized Southern Hemisphere.
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    39. 39
      Lan, Z.; Yao, Y.; Xu, J. Y.; Chen, H.; Ren, C.; Fang, X.; Zhang, K.; Jin, L.; Hua, X.; Alder, A. C.; Wu, F.; Sun, H. Novel and Legacy Per- and Polyfluoroalkyl Substances (PFASs) in a Farmland Environment: Soil Distribution and Biomonitoring with Plant Leaves and Locusts. Environ. Pollut. 2020, 263, 114487  DOI: 10.1016/j.envpol.2020.114487
      39
      Novel and legacy per- and polyfluoroalkyl substances (PFASs) in a farmland environment: Soil distribution and biomonitoring with plant leaves and locusts
      Lan, Zhonghui; Yao, Yiming; Xu, JiaYao; Chen, Hao; Ren, Chao; Fang, Xiangguang; Zhang, Kai; Jin, Litao; Hua, Xia; Alder, Alfredo C.; Wu, Fengchang; Sun, Hongwen
      Environmental Pollution (Oxford, United Kingdom) (2020), 263 (Part_A), 114487CODEN: ENPOEK; ISSN:0269-7491. (Elsevier Ltd.)
      The occurrence of legacy and novel per- and polyfluoroalkyl substances (PFASs) in multiple matrixes from a farmland environment was investigated in the Beijing-Tianjin-Hebei core area of northern China. PFASs were ubiquitously detected in farmland soils, and the detection frequency of 6:2 chlorinated polyfluoroalkyl ether sulfonic acid (6:2 Cl-PFESA) was higher than that of perfluorooctane sulfonic acid (98% vs. 83%). Long-chain PFASs, including 6:2 Cl-PFESA, showed a centered distribution pattern around the metropolis of Tianjin, probably due to the local intensive industrial activity, while trifluoroacetic acid (TFA) showed a decreasing trend from the coast to the inland area. Other than soil, TFA was also found at higher levels than other longer-chain PFASs in dust, maize (Zea mays), poplar (Populus alba) leaf and locust (Locusta migratoria manilens) samples. Both poplar leaves and locusts can be used as promising biomonitoring targets for PFASs in farmland environments, and their accumulation potential corresponds with protein and lipid contents. Apart from being exposed to PFASs via food intake, locusts were likely exposed via uptake from soil and pptd. dust in farmland environments. The biomonitoring of locusts may be more relevant to insectivores, which is important to conducting a comprehensive ecol. risk assessment of farmland environments.
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    40. 40
      Cahill, T. M.; Thomas, C. M.; Schwarzbach, S. E.; Seiber, J. N. Accumulation of Trifluoroacetate in Seasonal Wetlands in California. Environ. Sci. Technol. 2001, 35 (5), 820– 825,  DOI: 10.1021/es0013982
      40
      Accumulation of trifluoroacetate in seasonal wetlands in California
      Cahill, Thomas M.; Thomas, Carmen M.; Schwarzbach, Steven E.; Seiber, James N.
      Environmental Science and Technology (2001), 35 (5), 820-825CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Trifluoroacetate (TFA, CF3COO-) is a stable and mildly phytotoxic breakdown product of several fluorinated org. compds. including the hydro(chloro)fluorocarbons (HFC/HCFCs) that have largely replaced the stratospheric ozone-depleting chlorofluorocarbons (CFCs). TFA enters aquatic ecosystems primarily through pptn. and has the potential to accumulate in water bodies with little or no outflow to the point where toxic concns. could be achieved. This study demonstrated that seasonal wetlands lacking outflow concd. TFA as they evapd. during the dry season. In addn., the TFA within the pools was retained between years, which may result in long-term TFA accumulation. Since plants acquire TFA from their growing media, the plants exposed to high aq. concns. of TFA within the pools had elevated TFA concns. with a median concn. of 279 ng/g dry wt. in their tissues as compared to 33 ng/g for species growing outside the pools. The highest TFA concns. in water, which occurred just prior to the pools drying up, were in the 2-10 μg/L range. These concns. are ≈190 or less than reported toxic concns. for the most sensitive species tested, but our evidence suggests that these concns. will increase with continued TFA deposition into the pools.
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    41. 41
      EU Reference Laboratories for Residues of Pesticides. EURL-SRM-Residue Findings Report , 2017; pp 1– 10. https://www.eurl-pesticides.eu/userfiles/file/eurlsrm/eurlsrm_residue-observation_tfa-dfa.pdf (accessed 2023–12–08).
      There is no corresponding record for this reference.
    42. 42
      van Hees, P.; Karlsson, P.; Bucuricova, L.; Olsman, H.; Yeung, L.. Trifluoroacetic Acid (TFA) and Trifluoromethane Sulphonic Acid (TFMS) in Juice and Fruit/Vegetable Purees , 2024; pp 1– 8. https://cdnmedia.eurofins.com/european-east/media/uxcnaa2c/eurofins_tfa_tfms_juice_24_final.pdf (accessed 2024–08–27).
      There is no corresponding record for this reference.
    43. 43
      Duan, Y.; Sun, H.; Yao, Y.; Meng, Y.; Li, Y. Distribution of Novel and Legacy Per-/Polyfluoroalkyl Substances in Serum and Its Associations with Two Glycemic Biomarkers among Chinese Adult Men and Women with Normal Blood Glucose Levels. Environ. Int. 2020, 134, 105295  DOI: 10.1016/j.envint.2019.105295
      43
      Distribution of novel and legacy per-/polyfluoroalkyl substances in serum and its associations with two glycemic biomarkers among Chinese adult men and women with normal blood glucose levels
      Duan, Yishuang; Sun, Hongwen; Yao, Yiming; Meng, Yue; Li, Yongcheng
      Environment International (2020), 134 (), 105295CODEN: ENVIDV; ISSN:0160-4120. (Elsevier Ltd.)
      In this study, fasting serum samples from 252 participants with age range from 19 to 87 years old were collected in Tianjin, China. A total of 21 target PFASs were detd. to analyze levels and distribution of novel and legacy PFASs in serum and to further evaluate the cross-sectional assocns. of serum PFAS concns. with two glycemic biomarkers (i.e., fasting glucose and glycated Hb (HbA1c)). 6:2 chlorinated PFAES (6:2 Cl-PFAES) and trifluoroacetic acid (TFA) were widely detected novel PFASs (greater than90%) with relatively high median concns. (8.64 ng/mL and 8.46 ng/mL, resp.), which were second only to the two dominant legacy PFASs, i.e., perfluorooctanoic acid (PFOA, 14.83 ng/mL) and perfluorooctane sulfonic acid (14.24 ng/mL). Furthermore, 1% increase in serum PFOA and perfluorononanoic acid (PFNA) was sep. significantly assocd. with 0.018% [95% confidence interval (CI): 0.004%, 0.033%] and 0.022% (95% CI: 0.007%, 0.037%) increment in fasting glucose levels. Similarly, 1% increase in serum perfluorohexanoic acid, PFNA, and perfluorohexane sulfonic acid was significantly assocd. with 0.030% (95% CI: 0.010%, 0.051%), 0.018% (95% CI: 0.003%, 0.033%), 0.007% (95% CI: 0.003%, 0.011%) increment in HbA1c levels, resp. These findings suggested that 6:2 Cl-PFAES and TFA showed greater contributions to PFASs in serum and supported an assocn. of exposure to PFASs with fasting glucose and HbA1c.
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    44. 44
      Arnot, J. A.; Gobas, F. A. A Review of Bioconcentration Factor (BCF) and Bioaccumulation Factor (BAF) Assessments for Organic Chemicals in Aquatic Organisms. Environmental Reviews 2006, 14 (4), 257– 297,  DOI: 10.1139/a06-005
      44
      A review of bioconcentration factor (BCF) and bioaccumulation factor (BAF) assessments for organic chemicals in aquatic organisms
      Arnot, Jon A.; Gobas, Frank A. P. C.
      Environmental Reviews (Ottawa, ON, Canada) (2006), 14 (4), 257-297CODEN: ENRVEH; ISSN:1181-8700. (National Research Council of Canada)
      A review. Bioaccumulation assessment is important in the scientific evaluation of risks that chems. may pose to humans and the environment and is a current focus of regulatory effort. The status of bioaccumulation evaluations for org. chems. in aquatic systems is reviewed to reduce uncertainty in bioaccumulation measurement, to provide quality data for assessment, and to assist in model development. A review of 392 scientific literature and database sources includes 5317 bioconcn. factor (BCF) and 1656 bioaccumulation factor (BAF) values measured for 842 org. chems. in 219 aquatic species. A data quality assessment finds that 45% of BCF values are subject to at least one major source of uncertainty and that measurement errors generally result in an underestimation of actual BCF values. A case study of org. chems. on the Canadian Domestic Substances List indicates that empirical data are available for less than 4% of the chems. that require evaluation and of these chems., 76% have less than three acceptable quality BCF or BAF values. Field BAFs tend to be greater than lab. BCFs emphasizing the importance of environmental measurement for reliable assessment; however, only 0.2% of current use org. chems. have BAF measurements. Key parameters influencing uncertainty and variability in BCF and BAF data are discussed using reviewed data and models. A crit. evaluation of representative BCF and BAF models in relation to existing measurements and regulatory criteria in Canada indicate the probability of Type n errors, i.e., false negatives or "misses", using BCF models for bioaccumulation assessment may be as high as 70.6% depending on the model. Recommendations for the selection of measured and modelled values used in bioaccumulation assessment are provided, and improvements for the science and regulatory criteria are proposed.
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    45. 45
      Lucas, K.; Gaines, L. G. T.; Paris-Davila, T.; Nylander-French, L. A. Occupational Exposure and Serum Levels of Per- and Polyfluoroalkyl Substances (PFAS): A Review. American Journal of Industrial Medicine 2023, 66 (5), 379– 392,  DOI: 10.1002/ajim.23454
      There is no corresponding record for this reference.
    46. 46
      Woodcock, A. The Montreal Protocol: Getting over the Finishing Line?. Lancet. 2009, 373 (9665), 705– 706,  DOI: 10.1016/S0140-6736(09)60418-9
      There is no corresponding record for this reference.
    47. 47
      Zhang, J.; Zhang, Y.; Li, J.; Hu, J.; Ye, P.; Zeng, Z. Monitoring of Trifluoroacetic Acid Concentration in Environmental Waters in China. Water Res. 2005, 39 (7), 1331– 1339,  DOI: 10.1016/j.watres.2004.12.043
      47
      Monitoring of trifluoroacetic acid concentration in environmental waters in China
      Zhang, Jianbo; Zhang, Ying; Li, Jinlong; Hu, Jianxin; Ye, Peng; Zeng, Zheng
      Water Research (2005), 39 (7), 1331-1339CODEN: WATRAG; ISSN:0043-1354. (Elsevier B.V.)
      It is critically important and extremely meaningful to det. the concn. of trifluoroacetic acid (TFA) in the environmental water in China. This will create background ref. for the effects of analyzing the extensive employment of the substitutes to CFCs in China. In this paper a set of anal. methods was described for use in monitoring of TFA concn. of environmental waters including collecting, pre-treatment measures, preserving, concg. and derivatization of samples from different kinds of environmental waters. The GC with elec. capture detector (ECD) and headspace auto sampler were used in the anal. The lowest detection limit of the instrument is 0.0004 ng Me trifluoroacetic acid (MTFA), and the lowest detected concn. with the method is 3.0 ng/mL TFA. TFA collected in various environmental water samples (including rainfall, inland surface water, groundwater, and wastewater) from 9 provinces and autonomous regions in China were detd. by applying the anal. methods created and defined in this work. The concns. of TFA in 9 rainfalls and 3 snowfalls through the period from 2000-2001 ranged from 25 to 220 ng/L, the TFA concn. in the inland surface water samples ranged from 4.7 to 221 ng/L, the concn. of TFA in groundwater samples collected in Beijing was 10 ng/L, and the TFA concn. in coastal water samples ranged from 4.2-190.1 ng/L.
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    48. 48
      Zhai, Z.; Wu, J.; Hu, X.; Li, L.; Guo, J.; Zhang, B.; Hu, J.; Zhang, J. A 17-Fold Increase of Trifluoroacetic Acid in Landscape Waters of Beijing, China during the Last Decade. Chemosphere 2015, 129, 110– 117,  DOI: 10.1016/j.chemosphere.2014.09.033
      48
      A 17-fold increase of trifluoroacetic acid in landscape waters of Beijing, China during the last decade
      Zhai, Zihan; Wu, Jing; Hu, Xia; Li, Li; Guo, Junyu; Zhang, Boya; Hu, Jianxin; Zhang, Jianbo
      Chemosphere (2015), 129 (), 110-117CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
      The concns. of trifluoroacetic acid (TFA) were measured in urban landscape waters, tap water and snows in Beijing, China in 2012. Compared with the 2002 measurements, a 17-fold increase from 23-98 ng L-1 to 345-828 ng L-1 was obsd. for TFA concns. in urban landscape waters, and an obvious increase from not detected (n.d.) to 155 ng L-1 occurred to TFA in tap water. By flux estn. between air and water interface, the remarkable increase of TFA was attributable to dry and wet deposition. The quant. water-air-sediment interaction (QWASI) model simulated TFAs in various environmental media and showed that, over 99% of TFA distributed in water bodies. Our results recommend that measures are needed to control the increase of TFA in China.
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    49. 49
      Cahill, T. M. Increases in Trifluoroacetate Concentrations in Surface Waters over Two Decades. Environ. Sci. Technol. 2022, 56 (13), 9428– 9434,  DOI: 10.1021/acs.est.2c01826
      49
      Increases in trifluoroacetate concentrations in surface waters over two decades
      Cahill, Thomas M.
      Environmental Science & Technology (2022), 56 (13), 9428-9434CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)
      Trifluoroacetate (TFA) is a persistent perfluorinated alkanoic acid anion that has many anthropogenic sources, with fluorocarbon refrigerants being a major one. After an initial burst of research in the late 1990s and early 2000s, research on this ubiquitous pollutant declined as atm. emissions of the precursor compds. grew rapidly. Thus, there is little contemporaneous information about the concns. of TFA in the environment and how they have changed over time. This research detd. the change in TFA concns. in streams by resampling a transect that was originally sampled in 1998. The transect was designed to det. the regional distribution of TFA both upwind and downwind of major metropolitan areas in Northern California as well as a set of globally remote sites in Alaska. The results showed that TFA concns. increased by an av. of 6-fold over the intervening 23 years, which resulted in a median concn. of 180 ng/L (range 21.3-2790). The highest concns. were found in streams immediately downwind of the San Francisco Bay Area, while substantially lower concns. were found in the upwind, regionally remote, and globally remote sites. The C3 to C5 perfluorinated alkanoic acids were also investigated, but they were rarely detected with this methodol.
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    50. 50
      Freeling, F.; Scheurer, M.; Koschorreck, J.; Hoffmann, G.; Ternes, T. A.; Nödler, K. Levels and Temporal Trends of Trifluoroacetate (TFA) in Archived Plants: Evidence for Increasing Emissions of Gaseous TFA Precursors over the Last Decades. Environ. Sci. Technol. Lett. 2022, 9 (5), 400– 405,  DOI: 10.1021/acs.estlett.2c00164
      50
      Levels and Temporal Trends of Trifluoroacetate (TFA) in Archived Plants: Evidence for Increasing Emissions of Gaseous TFA Precursors over the Last Decades
      Freeling, Finnian; Scheurer, Marco; Koschorreck, Jan; Hoffmann, Gabriele; Ternes, Thomas A.; Noedler, Karsten
      Environmental Science & Technology Letters (2022), 9 (5), 400-405CODEN: ESTLCU; ISSN:2328-8930. (American Chemical Society)
      Trifluoroacetate (TFA) is a highly mobile and persistent compd. that occurs ubiquitously in the environment. Results from previous studies suggested an increase in the atm. deposition of TFA in the Northern Hemisphere starting in the 1990s. Due to its physicochem. properties, TFA can be efficiently taken up and accumulated by vascular plants. Consequently, plants could serve as a biomonitoring tool to evaluate the presence of TFA in the terrestrial environment. This is the first study which describes the concns. and temporal trends of TFA in biota by analyzing archived leaf samples of various tree species from the German Environmental Specimen Bank (observation period: 1989-2020). Samples from different locations of the same species were each in a similar concn. range. The highest concns. (up to ∼1000μg/kg dry wt.) were found in Lombardy poplar (Populus nigra 'Italica') leaves. A statistically significant pos. trend in the TFA concn. within the study period was found for most species/sites, which is likely the result of both bioaccumulation as well as increasing emissions of gaseous TFA precursors over the last three decades. These results contribute to the current discussion on the regulation of per- and polyfluoroalkyl substances (PFAS) to protect human and environmental health.
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    51. 51
      Wang, B.; Yao, Y.; Wang, Y.; Chen, H.; Sun, H. Per- and Polyfluoroalkyl Substances in Outdoor and Indoor Dust from Mainland China: Contributions of Unknown Precursors and Implications for Human Exposure. Environ. Sci. Technol. 2022, 56 (10), 6036– 6045,  DOI: 10.1021/acs.est.0c08242
      51
      Per- and polyfluoroalkyl substances in outdoor and indoor dust from mainland China: contributions of unknown precursors and implications for human exposure
      Wang, Bin; Yao, Yiming; Wang, Yu; Chen, Hao; Sun, Hongwen
      Environmental Science & Technology (2022), 56 (10), 6036-6045CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)
      Per- and polyfluoroalkyl substances (PFASs) were analyzed in outdoor (n = 101) and indoor dust (n = 43, 38 paired with outdoors) samples across mainland China. From 2013 to 2017, the median concn. of .sum.PFASs in outdoor dust tripled from 63 to 164 ng/g with an elevated contribution of trifluoroacetic acid and 6:2 fluorotelomer alc. In 2017, the indoor dust levels of .sum.PFASs were in the range 185-913 ng/g, which were generally higher than the outdoor dust levels (105-321 ng/g). Emerging PFASs were found at high median levels of 5.7-97 ng/g in both indoor and outdoor dust samples. As first revealed by the total oxidized precursors assay, unknown perfluoroalkyl acid (PFAA)-precursors contributed 37-67 mol % to the PFAS profiles in indoor dust samples. A great proportion of C8 PFAA-precursors were precursors for perfluorooctanesulfonic acid, while C6 and C4 PFAA-precursors were mostly fluorotelomer based. Furthermore, daily perfluorooctanoic acid (PFOA) equiv. intakes of PFAAs (C4-C12) mixts. via indoor dust were first estd. at 1.3-1.5 ng/kg b.w./d for toddlers at high scenarios, which exceeds the derived daily threshold of 0.63 ng/kg b.w./d. from the European Food Safety Authority (EFSA). On this basis, an underestimation of 56%-69% likely remains without considering potential risks due to the biotransformation of unknown PFAA-precursors.
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    52. 52
      European Chemicals Agency (ECHA). ECHA Registration Dossier for Trifluoroacetic Acid. https://echa.europa.eu/de/registration-dossier/-/registered-dossier/5203/7/1 (accessed 2023–12–15).
      There is no corresponding record for this reference.
    53. 53
      Scheurer, M.; Nödler, K.; Freeling, F.; Janda, J.; Happel, O.; Riegel, M.; Müller, U.; Storck, F. R.; Fleig, M.; Lange, F. T.; Brunsch, A.; Brauch, H. J. Small, Mobile, Persistent: Trifluoroacetate in the Water Cycle – Overlooked Sources, Pathways, and Consequences for Drinking Water Supply. Water Res. 2017, 126, 460– 471,  DOI: 10.1016/j.watres.2017.09.045
      53
      Small, mobile, persistent: Trifluoroacetate in the water cycle - Overlooked sources, pathways, and consequences for drinking water supply
      Scheurer, Marco; Noedler, Karsten; Freeling, Finnian; Janda, Joachim; Happel, Oliver; Riegel, Marcel; Mueller, Uwe; Storck, Florian Ruediger; Fleig, Michael; Lange, Frank Thomas; Brunsch, Andrea; Brauch, Heinz-Juergen
      Water Research (2017), 126 (), 460-471CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)
      Elevated concns. of trifluoroacetate (TFA) of more than 100 μg/L in a major German river led to the occurrence of more than 20 μg/L TFA in bank filtration based tap waters. Several spatially resolved monitoring programs were conducted and discharges from an industrial company were identified as the point source of TFA contamination. Treatment options for TFA removal were investigated at full-scale waterworks and in lab. batch tests. Commonly applied techniques like ozonation or granulated activated carbon filtration are inappropriate for TFA removal, whereas TFA was partly removed by ion exchange and completely retained by reverse osmosis. Further investigations identified wastewater treatment plants (WWTPs) as addnl. TFA dischargers into the aquatic environment. TFA was neither removed by biol. wastewater treatment, nor by a retention soil filter used for the treatment of combined sewer overflows. WWTP influents can even bear a TFA formation potential, when appropriate CF3-contg. precursors are present. Biol. degrdn. and ozonation batch expts. with chems. of different classes (flurtamone, fluopyram, tembotrione, flufenacet, fluoxetine, sitagliptine and 4:2 fluorotelomer sulfonate) proved that there are yet overlooked sources and pathways of TFA, which need to be addressed in the future.
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    54. 54
      Scott, B. F.; Macdonald, R. W.; Kannan, K.; Fisk, A.; Witter, A.; Yamashita, N.; Durham, L.; Spencer, C.; Muir, D. C. G. Trifluoroacetate Profiles in the Arctic, Atlantic, and Pacific Oceans. Environ. Sci. Technol. 2005, 39 (17), 6555– 6560,  DOI: 10.1021/es047975u
      54
      Trifluoroacetate Profiles in the Arctic, Atlantic, and Pacific Oceans
      Scott, B. F.; MacDonald, R. W.; Kannan, K.; Fisk, A.; Witter, A.; Yamashita, N.; Durham, L.; Spencer, C.; Muir, D. C. G.
      Environmental Science and Technology (2005), 39 (17), 6555-6560CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      A series of depth profiles was collected at 22 sites in the Arctic, North and South Atlantic, and Pacific Oceans to det. spatial patterns for trifluoroacetate (TFA) concns. in the marine environment and to study possible natural sources of TFA. Profiles were also taken over underwater vents in the North and South Pacific and the Mediterranean Sea. At the profile sites, TFA was from <10 ng/L in the Pacific Ocean to >150 ng/L in the Atlantic Ocean. Samples from the Canada Basin of the Arctic Ocean exhibited variable TFA concns. (60-160 ng/L) down to 700 m. Below this depth, in water with 14C ages exceeding 1000 yr, the TFA concns. were const. (150 ng/L). Water returning to the Atlantic through the Canadian Arctic Archipelago had const. high TFA values. Profiles from the Northern Atlantic exhibited high values at all depths but were more consistent in the Western Atlantic. The northwestern Pacific Ocean surface profile sites exhibited low TFA concns. in the top 100 m increasing to a max. of 60 ng/L with depth. Samples from the South Pacific Ocean site had generally low values with a few depths (>800 m) having concns. of ≥50 ng/L. To det. if underwater vents could contribute to the TFA concns. in the oceans, profiles were taken over three vents in the Pacific and Mediterranean Oceans. The results suggest that some deep-sea vents may be natural sources of TFA.
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    55. 55
      Frank, H.; Christoph, E. H.; Holm-Hansen, O.; Bullister, J. L. Trifluoroacetate in Ocean Waters. Environ. Sci. Technol. 2002, 36 (1), 12– 15,  DOI: 10.1021/es0101532
      55
      Trifluoroacetate in Ocean Waters
      Frank, Hartmut; Christoph, Eugen H.; Holm-Hansen, Osmund; Bullister, John L.
      Environmental Science and Technology (2002), 36 (1), 12-15CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Trifluoroacetate (TFA) is a ubiquitous xenochem. presently increasing in concn. in some environmental compartments, esp. in the plant biomass of industrialized countries. Direct anthropogenic emissions of TFA are probably low, and the major anthropogenic sources are most likely various TFA precursors. As TFA has been found in ocean waters from remote locations, the question arose as to whether it is also a naturally occurring environmental chem. Detn. of the depth dependence of TFA in the ocean water column should shed some light on this question. However, in environmental anal. studies, the risk of systematic errors can be high and may lead to wrong conclusions. Therefore, special attention has been paid to the fact that TFA is a common atm. pollutant in the urban environment and that contributions from sampling, storage, and transport potentially lead to artificially high TFA values. The results of the ocean water sampling campaigns indicate that TFA is a naturally occurring chem., homogeneously distributed in ocean waters of all ages with a concn. of about 200 ng/L.
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    56. 56
      Zhang, L.; Sun, H.; Wang, Q.; Chen, H.; Yao, Y.; Zhao, Z.; Alder, A. C. Uptake Mechanisms of Perfluoroalkyl Acids with Different Carbon Chain Lengths (C2-C8) by Wheat (Triticum Acstivnm L.). Sci. Total Environ. 2019, 654, 19– 27,  DOI: 10.1016/j.scitotenv.2018.10.443
      56
      Uptake mechanisms of perfluoroalkyl acids with different carbon chain lengths (C2-C8) by wheat (Triticum aestivum L.)
      Zhang, Lu; Sun, Hongwen; Wang, Qi; Chen, Hao; Yao, Yiming; Zhao, Zhen; Alder, Alfredo C.
      Science of the Total Environment (2019), 654 (), 19-27CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)
      Org. compds. could be taken up by plants via different pathways, depending on chem. properties and biol. species, which is important for the risk assessment and risk control. To investigate the transport pathways of perfluoroalkyl acids (PFAAs) by wheat (Triticum acstivnm L.), the uptake of five perfluoroalkyl carboxylic acids (PFCAs): TFA (C2), PFPrA (C3), PFBA (C4), PFHxA (C6), PFOA (C8), and a perfluoroalkyl sulfonic acid: PFOS (C8) were studied using hydroponic expts. Various inhibitors including a metabolic inhibitor (Na3VO4), two anion channel blockers (9-AC, DIDS), and two aquaporin inhibitors (AgNO3, glycerol) were examd. The wheat root and shoot showed different concn. trends with the carbon chain length of PFAAs. The uptake of TFA was inhibited by Na3VO4 and 9-AC whereas PFPrA was inhibited by Na3VO4, AgNO3 and 9-AC. For the other four PFAAs, only Na3VO4 was effective. These results together with the result of concn.-dependent uptake, which followed the Michaelis-Menten model, indicate that the uptake of PFAAs by wheat is mainly an energy-dependent active process mediated by carriers. For the ultra-short chain PFCAs (C2 and C3), aquaporins and anion channels may also be involved. A competition between TFA and PFPrA was detd. during the plant uptake but no competition was obsd. between these two shorter chain analogs with other analogs, neither between PFBA and PFHxA, PFBA and PFBS, PFOA and PFOS.
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    57. 57
      Costello, M. C. S.; Lee, L. S. Sources, Fate, and Plant Uptake in Agricultural Systems of Per- and Polyfluoroalkyl Substances. Curr. Pollut Rep 2024, 10, 799– 819,  DOI: 10.1007/s40726-020-00168-y
      There is no corresponding record for this reference.
    58. 58
      Munoz, G.; Mercier, L.; Duy, S. V.; Liu, J.; Sauvé, S.; Houde, M. Bioaccumulation and Trophic Magnification of Emerging and Legacy Per- and Polyfluoroalkyl Substances (PFAS) in a St. Lawrence River Food Web. Environ. Pollut. 2022, 309, 119739  DOI: 10.1016/j.envpol.2022.119739
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      Bioaccumulation and trophic magnification of emerging and legacy per- and polyfluoroalkyl substances (PFAS) in a St. Lawrence River food web
      Munoz, Gabriel; Mercier, Laurie; Duy, Sung Vo; Liu, Jinxia; Sauve, Sebastien; Houde, Magali
      Environmental Pollution (Oxford, United Kingdom) (2022), 309 (), 119739CODEN: ENPOEK; ISSN:0269-7491. (Elsevier Ltd.)
      Research on per- and polyfluoroalkyl substances (PFAS) in freshwater ecosystems has focused primarily on legacy compds. and little is still known on the presence of emerging PFAS. Here, we investigated the occurrence of 60 anionic, zwitterionic, and cationic PFAS in a food web of the St. Lawrence River (Quebec, Canada) near a major metropolitan area. Water, sediments, aquatic vegetation, invertebrates, and 14 fish species were targeted for anal. Levels of perfluorobutanoic acid (PFBA) in river water exceeded those of perfluorooctanoic acid (PFOA) or perfluorooctane sulfonate (PFOS), and a zwitterionic betaine was obsd. for the first time in the St.Lawrence River. The highest mean PFAS concns. were obsd. for the benthopelagic top predator Smallmouth bass (Micropterus dolomieu, Σ60PFAS ∼ 92± 34 ng/g wet wt. whole-body) and the lowest for aquatic plants (0.52-2.3 ng/g). Up to 33 PFAS were detected in biotic samples, with frequent occurrences of emerging PFAS such as perfluorobutane sulfonamide (FBSA) and perfluoroethyl cyclohexane sulfonate (PFECHS), while targeted ether-PFAS all remained undetected. PFOS and long-chain perfluorocarboxylates (C10-C13 PFCAs) dominated the contamination profiles in biota except for insects where PFBA was predominant. Gammarids, molluscs, and insects also had frequent detections of PFOA and fluorotelomer sulfonates, an important distinction with fish and presumably due to different metab. Based on bioaccumulation factors >5000 and trophic magnification factors >1, long-chain (C10-C13) PFCAs, PFOS, perfluorodecane sulfonate, and perfluorooctane sulfonamide qualified as very bioaccumulative and biomagnifying. Newly monitored PFAS such as FBSA and PFECHS were biomagnified but moderately bioaccumulative, while PFOA was biodiluted.
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    59. 59
      Haukås, M.; Berger, U.; Hop, H.; Gulliksen, B.; Gabrielsen, G. W. Bioaccumulation of Per- and Polyfluorinated Alkyl Substances (PFAS) in Selected Species from the Barents Sea Food Web. Environ. Pollut. 2007, 148 (1), 360– 371,  DOI: 10.1016/j.envpol.2006.09.021
      59
      Bioaccumulation of per- and polyfluorinated alkyl substances (PFAS) in selected species from the Barents Sea food web
      Haukas, Marianne; Berger, Urs; Hop, Haakon; Gulliksen, Bjorn; Gabrielsen, Geir W.
      Environmental Pollution (Amsterdam, Netherlands) (2007), 148 (1), 360-371CODEN: ENPOEK; ISSN:0269-7491. (Elsevier B.V.)
      The present study reports concns. and biomagnification potential of per- and polyfluorinated alkyl substances (PFAS) in species from the Barents Sea food web. The examd. species included sea ice amphipod (Gammarus wilkitzkii), polar cod (Boreogadus saida), black guillemot (Cepphus grylle) and glaucous gull (Larus hyperboreus). These were analyzed for PFAS, polychlorinated biphenyls (PCBs), dichlorodiphenyltrichloroethanes (DDTs) and polybrominated di-Ph ethers (PBDEs). Perfluorooctane sulfonate (PFOS) was the predominant of the detected PFAS. Trophic levels and food web transfer of PFAS were detd. using stable nitrogen isotopes (δ 15N). No correlation was found between PFOS concns. and trophic level within species. However, a non-linear relationship was established when the entire food web was analyzed. Biomagnification factors displayed values >1 for perfluorohexane sulfonate (PFHxS), perfluorononanoic acid (PFNA), PFOS and ΣPFAS(7). Multivariate analyses showed that the degree of trophic transfer of PFAS is similar to that of PCB, DDT and PBDE, despite their accumulation through different pathways.
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    60. 60
      Drew, R.; Hagen, T. G.; Champness, D. Accumulation of PFAS by Livestock – Determination of Transfer Factors from Water to Serum for Cattle and Sheep in Australia. Food Additives & Contaminants: Part A 2021, 38 (11), 1897– 1913,  DOI: 10.1080/19440049.2021.1942562
      There is no corresponding record for this reference.
    61. 61
      Ghisi, R.; Vamerali, T.; Manzetti, S. Accumulation of Perfluorinated Alkyl Substances (PFAS) in Agricultural Plants: A Review. Environ. Res. 2019, 169, 326– 341,  DOI: 10.1016/j.envres.2018.10.023
      61
      Accumulation of perfluorinated alkyl substances (PFAS) in agricultural plants: A review
      Ghisi, Rossella; Vamerali, Teofilo; Manzetti, Sergio
      Environmental Research (2019), 169 (), 326-341CODEN: ENVRAL; ISSN:0013-9351. (Elsevier)
      PFASs are a class of compds. that include perfluoroalkyl and polyfluoroalkyl substances, some of the most persistent pollutants still allowed - or only partially restricted - in several product fabrications and industrial applications worldwide. PFASs have been shown to interact with blood proteins and are suspected of causing a no. of pathol. responses, including cancer. Given this threat to living organisms, we carried out a broad review of possible sources of PFASs and their potential accumulation in agricultural plants, from where they can transfer to humans through the food chain. Anal. of the literature indicates a direct correlation between PFAS concns. in soil and bioaccumulation in plants. Furthermore, plant uptake largely changes with chain length, functional group, plant species and organ. Low accumulations of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS) have been found in peeled potatoes and cereal seeds, while short-chain compds. can accumulate at high levels in leafy vegetables and fruits. Significant variations in PFAS buildup in plants according to soil amendment are also found, suggesting a particular interaction with soil org. matter. Here, we identify a series of challenges that PFASs pose to the development of a safe agriculture for future generations.
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    62. 62
      Mikkonen, A. T.; Martin, J.; Upton, R. N.; Moenning, J.-L.; Numata, J.; Taylor, M. P.; Roberts, M. S.; Mackenzie, L. Dynamic Exposure and Body Burden Models for Per- and Polyfluoroalkyl Substances (PFAS) Enable Management of Food Safety Risks in Cattle. Environ. Int. 2023, 180, 108218  DOI: 10.1016/j.envint.2023.108218
      There is no corresponding record for this reference.
    63. 63
      Salierno, G. On the Chemical Pathways Influencing the Effective Global Warming Potential of Commercial Hydrofluoroolefin Gases. ChemSusChem 2024, 1– 20,  DOI: 10.1002/cssc.202400280
      There is no corresponding record for this reference.
    64. 64
      Russell, M. H.; Hoogeweg, G.; Webster, E. M.; Ellis, D. A.; Waterland, R. L.; Hoke, R. A. TFA from HFO-1234yf: Accumulation and Aquatic Risk in Terminal Water Bodies. Environ. Toxicol. Chem. 2012, 31 (9), 1957– 1965,  DOI: 10.1002/etc.1925
      64
      TFA from HFO-1234yf: accumulation and aquatic risk in terminal water bodies
      Russell, Mark H.; Hoogeweg, Gerco; Webster, Eva M.; Ellis, David A.; Waterland, Robert L.; Hoke, Robert A.
      Environmental Toxicology and Chemistry (2012), 31 (9), 1957-1965CODEN: ETOCDK; ISSN:0730-7268. (Wiley-Blackwell)
      A next-generation mobile automobile air conditioning (MAC) refrigerant, HFO-1234yf (CF3CF=CH2), is being developed with improved environmental characteristics. In the atm., it ultimately forms trifluoroacetic acid (TFA(A); CF3COOH), which is subsequently scavenged by atm. pptn. and deposited on land and water as trifluoroacetate (TFA; CF3COO-). Trifluoroacetate is environmentally stable and has the potential to accumulate in terminal water bodies, i.e., aquatic systems receiving inflow but with little or no outflow and with high evapn. rates. Previous studies estd. HFO-1234yf emission rates and modeled its deposition concns. and TFA rates throughout North America. This work used multi-media and geog. information system-based modeling to assess potential TFA concns. in terminal water bodies over extended periods. After 10 years of emissions, predicted TFA concns. in North American terminal water bodies were estd. to be from current background concns. (0.01-0.22 μg/L) to 1-6 μg/L. After 50 years of continuous emissions, aquatic concns. of 1-15 μg/L are predicted, with extreme concns. of 50-200 μg/L in settings such as the Sonoran Desert along the California/Arizona border. Based on the relative insensitivity of aquatic organisms to TFA, predicted TFA concns. in terminal water bodies are not expected to impair aquatic systems, even considering potential emissions over extended periods.
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    65. 65
      Arp, H. P. H.; Hale, S. E.; Borchers, U.; Valkov, V.; Wiegand, L.; Zahn, D.; Neuwald, I.; Nödler, K.; Scheurer, M. A Prioritization Framework for PMT/VPvM Substances under REACH for Registrants, Regulators, Researchers and the Water Sector, UBA TEXTE 22/2023. Neumann, M., Schliebner, I. Eds.; German Environment Agency (UBA): Dessau-Roßlau, Germany, pp 1– 238. https://www.umweltbundesamt.de/publikationen/a-prioritization-framework-for-pmtvpvm-substances (accessed 2024–06–03).
      There is no corresponding record for this reference.
    66. 66
      Hale, S. E.; Neumann, M.; Schliebner, I.; Schulze, J.; Averbeck, F. S.; Castell-Exner, C.; Collard, M.; Drmač, D.; Hartmann, J.; Hofman-Caris, R.; Hollender, J.; de Jonge, M.; Kullick, T.; Lennquist, A.; Letzel, T.; Nödler, K.; Pawlowski, S.; Reineke, N.; Rorije, E.; Scheurer, M.; Sigmund, G.; Timmer, H.; Trier, X.; Verbruggen, E.; Arp, H. P. H. Getting in Control of Persistent, Mobile and Toxic (PMT) and Very Persistent and Very Mobile (VPvM) Substances to Protect Water Resources: Strategies from Diverse Perspectives. Environ. Sci. Eur. 2022, 34 (1), 22,  DOI: 10.1186/s12302-022-00604-4
      66
      Getting in control of persistent, mobile and toxic (PMT) and very persistent and very mobile (vPvM) substances to protect water resources: strategies from diverse perspectives
      Hale, Sarah E.; Neumann, Michael; Schliebner, Ivo; Schulze, Jona; Averbeck, Frauke S.; Castell-Exner, Claudia; Collard, Marie; Drmac, Dunja; Hartmann, Julia; Hofman-Caris, Roberta; Hollender, Juliane; de Jonge, Martin; Kullick, Thomas; Lennquist, Anna; Letzel, Thomas; Nodler, Karsten; Pawlowski, Sascha; Reineke, Ninja; Rorije, Emiel; Scheurer, Marco; Sigmund, Gabriel; Timmer, Harrie; Trier, Xenia; Verbruggen, Eric; Arp, Hans Peter H.
      Environmental Sciences Europe (2022), 34 (1), 22CODEN: ESENCT; ISSN:2190-4715. (Springer)
      Safe and clean drinking water is essential for human life. Persistent, mobile and toxic (PMT) substances and/or very persistent and very mobile (vPvM) substances are an important group of substances for which addnl. measures to protect water resources may be needed to avoid neg. environmental and human health effects. PMT/vPvM substances do not sufficiently biodegrade in the environment, they can travel long distances with water and are toxic (those that are PMT substances) to the environment and/or human health. PMT/vPvM substance research and regulation is arguably in its infancy and in order to get in control of these substances the following (non-exhaustive list of) knowledge gaps should to be addressed: environmental occurrence; the suitability of currently available anal. methods; the effectiveness and availability of treatment technologies; the ability of regional governance and industrial stewardship to contribute to safe drinking water while supporting innovation; the ways in which policies and regulations can be used most effectively to govern these substances; and, the identification of safe and sustainable alternatives. The work is the outcome of the third PMT workshop, held in March 2021, that brought together diverse scientists, regulators, NGOs, and representatives from the water sector and the chem. sector, all concerned with protecting the quality of our water resources. The online workshop was attended by over 700 people. The knowledge gaps above were discussed in the presentations given and the attendees were invited to provide their opinions about knowledge gaps related to PMT/vPvM substance research and regulation. Strategies to closing the knowledge, tech. and practical gaps to get in control of PMT/vPvM substances can be rooted in the Chems. Strategy for Sustainability Towards a Toxic Free Environment from the European Commission, as well as recent advances in the research and industrial stewardship. Key to closing these gaps are: (i) advancing remediation and removal strategies for PMT/vPvM substances that are already in the environment, however this is not an effective long-term strategy; (ii) clear and harmonized definitions of PMT/vPvM substances across diverse European and international legislations; (iii) ensuring wider availability of anal. methods and ref. stds.; (iv) addressing data gaps related to persistence, mobility and toxicity of chem. substances, particularly transformation products and those within complex substance mixts.; and (v) advancing monitoring and risk assessment tools for stewardship and regulatory compliance. The two most effective ways to get in control were identified to be source control through risk governance efforts, and enhancing market incentives for alternatives to PMT/vPvM substances by using safe and sustainable by design strategies.
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    67. 67
      Zhou, J.; Saeidi, N.; Wick, L. Y.; Xie, Y.; Kopinke, F. D.; Georgi, A. Efficient Removal of Trifluoroacetic Acid from Water Using Surface-Modified Activated Carbon and Electro-Assisted Desorption. J. Hazard Mater. 2022, 436, 129051  DOI: 10.1016/j.jhazmat.2022.129051
      There is no corresponding record for this reference.
    68. 68
      Zhang, Z.; Wu, Y.; Luo, L.; Li, G.; Li, Y.; Hu, H. Application of Disk Tube Reverse Osmosis in Wastewater Treatment: A Review. Science of The Total Environment 2021, 792, 148291  DOI: 10.1016/j.scitotenv.2021.148291
      There is no corresponding record for this reference.
    69. 69
      Bartholomew, T. V.; Siefert, N. S.; Mauter, M. S. Cost Optimization of Osmotically Assisted Reverse Osmosis. Environ. Sci. Technol. 2018, 52 (20), 11813– 11821,  DOI: 10.1021/acs.est.8b02771
      69
      Cost Optimization of Osmotically Assisted Reverse Osmosis
      Bartholomew, Timothy V.; Siefert, Nicholas S.; Mauter, Meagan S.
      Environmental Science & Technology (2018), 52 (20), 11813-11821CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      We develop a nonlinear optimization model to identify min. cost designs for osmotically assisted reverse osmosis (OARO), a multistaged membrane-based process for desalinating high-salinity brines. The optimization model enables comprehensive evaluation of a complex process configuration and operational decision space that includes nonlinear process performance and implicit relationships among membrane stages, saline sweep cycles, and makeup, purge, and recycle streams. The objective function minimizes cost, rather than energy or capital expenditures, to accurately account for the trade-offs in capital and operational expenses inherent in multistaged membrane processes. Generally, we find that cost-optimal OARO processes minimize the no. of stages, eliminate the use of saline makeup streams, purge from the first sweep cycle, and successively decrease stage membrane area and sweep flow rates. The optimal OARO configuration for treating feed salinities of 50-125 g/L total dissolved solids with water recoveries between 30-70% results in costs less than or equal to $6 per m3 of product water. Sensitivity anal. suggests that future research to minimize OARO costs should focus on minimizing the membrane structural parameter while maximizing the membrane burst pressure and reducing the membrane unit cost.
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    70. 70
      Kim, J.; Park, K.; Yang, D. R.; Hong, S. A Comprehensive Review of Energy Consumption of Seawater Reverse Osmosis Desalination Plants. Appl. Energy 2019, 254, 113652  DOI: 10.1016/j.apenergy.2019.113652
      70
      A comprehensive review of energy consumption of seawater reverse osmosis desalination plants
      Kim, Jungbin; Park, Kiho; Yang, Dae Ryook; Hong, Seungkwan
      Applied Energy (2019), 254 (), 113652CODEN: APENDX; ISSN:0306-2619. (Elsevier Ltd.)
      A review. High specific energy consumption (SEC) is the main barrier for the expansion of seawater reverse osmosis (SWRO). Therefore, the main objective of current SWRO research is to lower the SEC of SWRO plants. However, SEC of SWRO plants has not been systemically explored or analyzed, despite the need for information to develop appropriate strategies to reduce SEC. Therefore, this study aims to review and analyze SWRO plants for a comprehensive understanding of their SEC. First, trends in SWRO application are investigated using more than 70 datasets on large-scale SWRO. The anal. explains the increasing no. of large-size SWRO plants, the SEC redn. by isobaric energy recovery devices (ERDs), and the use of different SWRO configurations to meet the energy and quality requirements. Factors assocd. with SEC (i.e., feed conditions, target conditions, and equipment efficiency) are also analyzed. High salinity increases energy demand, whereas the temp. effect on energy consumption is not entirely clear. High-efficiency ERDs and pumps can reduce SEC, but overall SEC cannot be explained by these factors alone. SEC is also affected by target water quality and quantity. Moreover, specific SWRO designs can improve the system to efficiently achieve the established goals. Furthermore, future directions to develop low-energy SWRO plants are discussed.
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    71. 71
      Elimelech, M.; Phillip, W. A. The Future of Seawater Desalination: Energy, Technology, and the Environment. Science (1979) 2011, 333 (6043), 712– 717,  DOI: 10.1126/science.1200488
      71
      The Future of Seawater Desalination: Energy, Technology, and the Environment
      Elimelech, Menachem; Phillip, William A.
      Science (Washington, DC, United States) (2011), 333 (6043), 712-717CODEN: SCIEAS; ISSN:0036-8075. (American Association for the Advancement of Science)
      A review. In recent years, numerous large-scale seawater desalination plants were built in water-stressed countries to augment available water resources, and construction of new desalination plants is expected to increase in the near future. Despite major advancements in desalination technologies, seawater desalination is still more energy intensive compared to conventional technologies for the treatment of fresh water. There are also concerns about the potential environmental impacts of large-scale seawater desalination plants. Here, the authors review the possible redns. in energy demand by state-of-the-art seawater desalination technologies, the potential role of advanced materials and innovative technologies in improving performance, and the sustainability of desalination as a technol. soln. to global water shortages.
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    72. 72
      European Parliament and the Council. Directive 2000/60/EC of the European Parliament and of the Council of 23 October 2000 Establishing a Framework for Community Action in the Field of Water Policy ; 2000; pp 1– 73. https://eur-lex.europa.eu/eli/dir/2000/60/oj (accessed 2024–08–20).
      There is no corresponding record for this reference.
    73. 73
      Austin, C.; Purohit, A. L.; Thomsen, C.; Pinkard, B. R.; Strathmann, T. J.; Novosselov, I. V. Hydrothermal Destruction and Defluorination of Trifluoroacetic Acid (TFA). Environ. Sci. Technol. 2024, 58 (18), 8076– 8085,  DOI: 10.1021/acs.est.3c09404
      There is no corresponding record for this reference.
    74. 74
      ATMOsphere. The Rising Threat of HFOs and TFA to Health and the Environment.; 2022. https://issuu.com/shecco/docs/2022_atmo_hfo_tfa_report (accessed 2023–12–06).
      There is no corresponding record for this reference.
    75. 75
      Molina, M. J.; Rowland, F. S. Stratospheric Sink for Chlorofluoromethanes: Chlorine Atom-Catalysed Destruction of Ozone. Nature 1974, 249 (5460), 810– 812,  DOI: 10.1038/249810a0
      75
      Stratospheric sink for chlorofluoromethanes. Chlorine atom-catalyzed destruction of ozone
      Molina, Mario J.; Rowland, F. S.
      Nature (London, United Kingdom) (1974), 249 (5460), 810-12CODEN: NATUAS; ISSN:0028-0836.
      Photolytic dissocn. of atm. CFCl3 and CF2Cl2 gives Cl which destroys the O3 layer. The halomethanes may remain at altitudes of 20-40 km for 40-150 yr and will reach satn. values of 10-30 times the present levels.
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    76. 76
      Farman, J. C.; Gardiner, B. G.; Shanklin, J. D. Large Losses of Total Ozone in Antarctica Reveal Seasonal ClOx/NOx Interaction. Nature 1985, 315 (6016), 207– 210,  DOI: 10.1038/315207a0
      76
      Large losses of total ozone in Antarctica reveal seasonal ClOx/NOx interaction
      Farman, J. C.; Gardiner, B. G.; Shanklin, J. D.
      Nature (London, United Kingdom) (1985), 315 (6016), 207-10CODEN: NATUAS; ISSN:0028-0836.
      Measurements of total O3 concns. in the Antarctic stratosphere (Oct. 1980 - Mar. 1984) indicate that the spring values have fallen considerably although the circulation in the lower stratosphere is apparently unchanged. The very low temps., which prevail from midwinter until several weeks after the spring equinox, may make the Antarctic stratosphere sensitive to the growth of inorg. Cl, primarily by the effect of this growth on the NO2/NO ratio. This, together with the height distribution of UV irradn. peculiar to the polar stratosphere, could account for the O3 losses.
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    77. 77
      Allen, M. Planetary Boundaries: Tangible Targets Are Critical. Nat. Clim Chang 2009, 1 (910), 114– 115,  DOI: 10.1038/climate.2009.95
      There is no corresponding record for this reference.
    78. 78
      Ozone Secretariat. Handbook for the Montreal Protocol on Substances That Deplete the Ozone Layer, 14th ed.; 2020; pp 1– 960. https://ozone.unep.org/sites/default/files/Handbooks/MP-Handbook-2020-English.pdf (accessed 2024–10–13).
      There is no corresponding record for this reference.
    79. 79
      Falkner, R. The Business of Ozone Layer Protection: Corporate Power in Regime Evolution. In The Business of Global Environmental Governance. Global environmental accord: strategies for sustainability and institutional innovation; Levy, D. L., Newell, P. J., Eds.; MIT Press: Cambridge, MA, 2005; pp 105– 134.
      There is no corresponding record for this reference.
    80. 80
      Regulation (EU) No 517/2014 of the European Parliament and of the Council of 16 April 2014 on Fluorinated Greenhouse Gases and Repealing Regulation (EC) No 842/2006; European Parliament, Council of the European Union, 2014; pp 195– 230. https://eur-lex.europa.eu/legal-content/en/ALL/?uri=CELEX:32014R0517 (accessed 2023–12–06).
      There is no corresponding record for this reference.
    81. 81
      Behringer, D.; Heydel, F.; Gschrey, B.; Osterheld, S.; Schwarz, W.; Warncke, K.; Freeling, F.; Nödler, K.; Wasser, T.; Henne, S.; Reimann Empa, S.; Blepp, M.; Jörß, W.; Liu, R.; Ludig, S.; Rüdenauer, I.; Gartiser, S. Persistent Degradation Products of Halogenated Refrigerants and Blowing Agents in the Environment: Type, Environmental Concentrations, and Fate with Particular Regard to New Halogenated Substitutes with Low Global Warming Potential ; UBA TEXTE 73/2021, 2021; pp 1– 259. https://www.umweltbundesamt.de/sites/default/files/medien/5750/publikationen/2021-05-06_texte_73-2021_persistent_degradation_products.pdf (accessed 2023–12–06).
      There is no corresponding record for this reference.
    82. 82
      Holland, R.; Khan, M. A. H.; Driscoll, I.; Chhantyal-Pun, R.; Derwent, R. G.; Taatjes, C. A.; Orr-Ewing, A. J.; Percival, C. J.; Shallcross, D. E. Investigation of the Production of Trifluoroacetic Acid from Two Halocarbons, HFC-134a and HFO-1234yf and Its Fates Using a Global Three-Dimensional Chemical Transport Model. ACS Earth Space Chem. 2021, 5 (4), 849– 857,  DOI: 10.1021/acsearthspacechem.0c00355
      82
      Investigation of the production of trifluoroacetic acid from two halocarbons, HFC-134a and HFO-1234yf and its fates using a global three-dimensional chemical transport model
      Holland, Rayne; Khan, M. Anwar H.; Driscoll, Isabel; Chhantyal-Pun, Rabi; Derwent, Richard G.; Taatjes, Craig A.; Orr-Ewing, Andrew J.; Percival, Carl J.; Shallcross, Dudley E.
      ACS Earth and Space Chemistry (2021), 5 (4), 849-857CODEN: AESCCQ; ISSN:2472-3452. (American Chemical Society)
      Trifluoroacetic acid (TFA), a highly sol. and stable org. acid, is photochem. produced by certain anthropogenically emitted halocarbons such as HFC-134a and HFO-1234yf. Both these halocarbons are used as refrigerants in the automobile industry, and the high global warming potential of HFC-134a has promoted regulation of its use. Industries are transitioning to the use of HFO-1234yf as a more environmentally friendly alternative. We investigated the environmental effects of this change and found a 33-fold increase in the global burden of TFA from an annual value of 65 tonnes formed from the 2015 emissions of HFC-134a to a value of 2220 tonnes formed from an equiv. emission of HFO-1234yf. The percentage increase in surface TFA concns. resulting from the switch from HFC-134a to HFO-1234yf remains substantial with an increase of up to 250-fold across Europe. The increase in emissions greater than the current emission scenario of HFO-1234yf is likely to result in significant TFA burden as the atm. is not able to disperse and deposit relevant oxidn. products. The Criegee intermediate initiated loss process of TFA reduces the surface level atm. lifetime of TFA by up to 5 days (from 7 days to 2 days) in tropical forested regions.
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    83. 83
      Xie, G.; Cui, J.; Zhai, Z.; Zhang, J. Distribution Characteristics of Trifluoroacetic Acid in the Environments Surrounding Fluorochemical Production Plants in Jinan, China. Environmental Science and Pollution Research 2020, 27 (1), 983– 991,  DOI: 10.1007/s11356-019-06689-4
      83
      Distribution characteristics of trifluoroacetic acid in the environments surrounding fluorochemical production plants in Jinan, China
      Xie, Guiying; Cui, Jia'nan; Zhai, Zihan; Zhang, Jianbo
      Environmental Science and Pollution Research (2020), 27 (1), 983-991CODEN: ESPLEC; ISSN:0944-1344. (Springer)
      Trifluoroacetic acid (TFA) is a ubiquitous and extremely stable contaminant in the ambient environment and may be discharged during fluorochem. prodn. processes. However, the impacts of fluorochem. prodn. on surrounding areas have seldom been evaluated. We focused on Jinan, the capital of Shandong Province, China, and measured TFA levels in water, soil, and air samples. Our results showed that the av. TFA concns. in flowing water bodies were lower than those in landscape water bodies. The av. TFA concns. in soils were significantly higher than the background concn. As for atm. TFA levels, the mean concns. in the gas phase were higher than those in the particle phase, and av. daytime levels were slightly higher than nighttime levels. In addn., the quotient method was used to assess the ecol. risk of TFA in water in Jinan. The ratio of pollutant environmental concn. to predicted no-effect concn. (PEC/PNEC) for TFA was greater than 1, indicating that TFA does potentially damage the aquatic ecosystem of Jinan. Our findings suggest that TFA pollution around fluoride prodn. plants is a serious problem and that actions are required to avoid exacerbating the local ecol. and environmental risks of TFA.
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    84. 84
      Horel, S.. Record Levels of “forever Chemicals” Found in One French Village’s Water. Le Monde . Paris February 7, 2024. https://www.lemonde.fr/en/les-decodeurs/article/2024/02/07/record-levels-of-forever-chemicals-found-in-one-french-village-s-water-supply_6502237_8.html (accessed 2024–05–31).
      There is no corresponding record for this reference.
    85. 85
      Générations Futures. PFAS Contamination Des Eaux Par Des “Polluants Éternels” à Salindres , 2024. https://www.generations-futures.fr/wp-content/uploads/2024/02/rapport-salindres-pfas.pdf (accessed 2024–08–27).
      There is no corresponding record for this reference.
    86. 86
      Ellis, D. A.; Mabury, S. A. The Aqueous Photolysis of TFM and Related Trifluoromethylphenols. An Alternate Source of Trifluoroacetic Acid in the Environment. Environ. Sci. Technol. 2000, 34 (4), 632– 637,  DOI: 10.1021/es990422c
      86
      The Aqueous Photolysis of TFM and Related Trifluoromethylphenols. An Alternate Source of Trifluoroacetic Acid in the Environment
      Ellis, David A.; Mabury, Scott A.
      Environmental Science and Technology (2000), 34 (4), 632-637CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      The lampricide 3-trifluoromethyl-4-nitrophenol (TFM) is added annually to the Great Lakes (∼50,000 Kg/yr), with treatment concns. 1-14 mg/L at source. TFM was shown to undergo photohydrolytic degrdn., at 365 nm and under actinic radiation, to produce trifluoroacetic acid (TFA). A mechanistic study for the prodn. of TFA from TFM was conducted, and the structural parameters assocd. with the prodn. of TFA from trifluoromethylated phenols were studied. It was found that the yield of TFA depended on the nature of the trifluoromethylated phenol. The nature of the substituents, the substitution pattern, and the pH strongly effected the photolytic half-life of the parent compd. and the yield of TFA. The half-life of TFM at 365 nm was 22 h (pH 9) and yielded 5.1% TFA, and 91.7 h at pH 7, yielding 17.8% TFA. Converting the nitro substituent of TFM to an amino group caused a decrease in the half-life to 2.3 min and yielded 11% TFA. The mechanism for the prodn. of TFA from TFM was deduced from the pH dependence and the effect of altering substituents on the trifluoromethylphenol. Ultimately, the formation of trifluoromethylquinone led to the quant. prodn. of TFA.
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    87. 87
      EFSA Peer Review of the Pesticide Risk Assessment of the Active Substance Flurtamone. EFSA Journal 2016, 14 (6), e04498,  DOI: 10.2903/j.efsa.2016.4498
      There is no corresponding record for this reference.
    88. 88
      EFSA Reasoned Opinion on the Setting of MRLs for Saflufenacil in Various Crops, Considering the Risk Related to the Metabolite Trifluoroacetic Acid (TFA). EFSA Journal 2014, 12 (2), 3585,  DOI: 10.2903/j.efsa.2014.3585
      There is no corresponding record for this reference.
    89. 89
      Joudan, S.; Gauthier, J.; Mabury, S. A.; Young, C. J. Aqueous Leaching of Ultrashort-Chain PFAS from (Fluoro)Polymers: Targeted and Nontargeted Analysis. Environ. Sci. Technol. Lett. 2024, 11 (3), 237– 242,  DOI: 10.1021/acs.estlett.3c00797
      There is no corresponding record for this reference.
    90. 90
      Cui, J.; Guo, J.; Zhai, Z.; Zhang, J. The Contribution of Fluoropolymer Thermolysis to Trifluoroacetic Acid (TFA) in Environmental Media. Chemosphere 2019, 222, 637– 644,  DOI: 10.1016/j.chemosphere.2019.01.174
      90
      The contribution of fluoropolymer thermolysis to trifluoroacetic acid (TFA) in environmental media
      Cui, Jia-nan; Guo, Junyu; Zhai, Zihan; Zhang, Jianbo
      Chemosphere (2019), 222 (), 637-644CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
      The source of trifluoroacetic acid (TFA) has long been a controversial issue. Fluoropolymer thermolysis is expected to be a potential anthropogenic source except for CFC alternatives. However, its TFA yield and contributions have rarely been reported more recently. In this study, we investigated the thermal properties of three kinds of fluoropolymers, including poly (vinylidene fluoride-co-hexafluropropylene) (PVDF-HFP), poly (vinylidene fluoride-co-chlorotrifluoroethylene) (PVDF-CTFE) and poly (tetrafluoroethylene) (PTFE). A lab. simulation expt. was then performed to analyze the TFA levels in the thermolysis products and hence to examine the TFA yields of these fluoropolymers. Thermolysis of these fluoropolymers occurred in the temp. ranges from ∼400°C to ∼650°C, with the peak wt. loss rate at around 550-600°C. TFA could be produced through fluoropolymer thermolysis when being heated to 500°C and above. Av. TFA yields of PTFE, PVDF-HFP and PVDF-CTFE were 1.2%, 0.9% and 0.3%, resp. Furthermore, the contribution of fluoropolymer thermolysis and CFC alternatives to rainwater TFA in Beijing, China was evaluated by using a Two-Box model. The degrdn. of fluoropolymers and HCFCs/HFCs could explain 37.9-43.4 ng L-1 rainwater TFA in Beijing in 2014. The thermolysis of fluoropolymers contributed 0.6-6.1 ng L-1 of rainwater TFA, accounting for 1.6-14.0% of the TFA burden from all the precursors which were considered here.
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    91. 91
      Martin, J. W.; Franklin, J.; Hanson, M. L.; Solomon, K. R.; Mabury, S. A.; Ellis, D. A.; Scott, B. F.; Muir, D. C. G. Detection of Chlorodifluoroacetic Acid in Precipitation: A Possible Product of Fluorocarbon Degradation. Environ. Sci. Technol. 2000, 34 (2), 274– 281,  DOI: 10.1021/es990935j
      91
      Detection of Chlorodifluoroacetic Acid in Precipitation: A Possible Product of Fluorocarbon Degradation
      Martin, Jonathan W.; Franklin, James; Hanson, Mark L.; Solomon, Keith R.; Mabury, Scott A.; Ellis, David A.; Scott, Brian F.; Muir, Derek C. G.
      Environmental Science and Technology (2000), 34 (2), 274-281CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      Chlorodifluoroacetic acid (CDFA) was detected in rain and snow samples from various regions of Canada. Routine quant. anal. was performed using an in-situ derivatization technique that allowed CDFA detn. by gas chromatog.-mass spectrometry of its anilide deriv. Validation of environmental CDFA was provided by strong anionic exchange chromatog. and detection by 19F NMR. CDFA concns. were <7.1-170 ng/L among all samples analyzed. Monthly vol.-weighted CDFA concns. in rain samples showed a seasonal trend between June and Nov. 1998, peaking in late summer and decreasing in fall for Guelph and Toronto sites. Preliminary toxicity tests with the aquatic macrophytes, Myriophyllum sibiricum and Myriophyllum spicatum, suggested CDFA does not represent a risk of acute toxicity to these aquatic macrophytes at current environmental concns. A degrdn. study suggested CDFA is recalcitrant to biotic and abiotic degrdn. relative to dichloroacetic acid (DCA) and may accumulate in the aquatic environment. Based on existing exptl. data, it is postulated that CDFA is a degrdn. product of CFC-113, and, to a lesser extent, HCFC-142b. If CFC-113 is a source, its O3 depletion potential may be lower than previously assumed.
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    92. 92
      Sun, M.; Cui, J.; Guo, J.; Zhai, Z.; Zuo, P.; Zhang, J. Fluorochemicals Biodegradation as a Potential Source of Trifluoroacetic Acid (TFA) to the Environment. Chemosphere 2020, 254, 126894  DOI: 10.1016/j.chemosphere.2020.126894
      92
      Fluorochemicals biodegradation as a potential source of trifluoroacetic acid (TFA) to the environment
      Sun, Mei; Cui, Jia'nan; Guo, Junyu; Zhai, Zihan; Zuo, Peng; Zhang, Jianbo
      Chemosphere (2020), 254 (), 126894CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
      The anthropogenic release of trifluoroacetic acid (TFA) into the environmental media is not limited to photochem. oxidn. of CFC alternatives and industrial emissions. Biol. degrdn. of some fluorochems. is expected to be a potential TFA source. For the first time, we assess if the potential precursors [6:2 fluorotelomer alc. (6:2 FTOH), 4:2 fluorotelomer alc. (4:2 FTOH), acrinathrin, trifluralin, and 2-(trifluoromethyl)acrylic acid (TFMAA)] can be biol. degraded to TFA. Results show that 6:2 FTOH was terminally transformed to 5:3 polyfluorinated acid (5:3 FTCA; 12.5 mol%), perfluorohexanoic acid (PFHxA; 2.0 mol%), perfluoropentanoic acid (PFPeA; 1.6 mol%), perfluorobutyric acid (PFBA; 1.7 mol%), and TFA (2.3 mol%) by day 32 in the landfill soil microbial culture system. 4:2 FTOH could remove multiple -CF2 groups by microorganisms and produce PFPeA (2.6 mol%), PFBA (17.4 mol%), TFA (7.8 mol%). Furthermore, we basically analyzed the biodegrdn. contribution of short-chain FTOH as raw material residuals in com. products to the TFA burden in the environmental media. We est. global emission of 3.9-47.3 tonnes of TFA in the period from 1961 to 2019, and project 3.8-46.4 tonnes to be emitted from 2020 to 2040 via the pathway of 4:2 and 6:2 FTOH biodegrdn. (0.6-7.1 and 0.6-7.0 tonnes in China, resp.). Direct evidence of the expts. indicates that biodegrdn. of fluorochems. is an overlooked source of TFA and there are still some unspecified mech. of TFA prodn. pathways.
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    93. 93
      Björnsdotter, M. K.; Yeung, L. W. Y.; Kärrman, A.; Jogsten, I. E. Ultra-Short-Chain Perfluoroalkyl Acids Including Trifluoromethane Sulfonic Acid in Water Connected to Known and Suspected Point Sources in Sweden. Environ. Sci. Technol. 2019, 53 (19), 11093– 11101,  DOI: 10.1021/acs.est.9b02211
      93
      Ultra-Short-Chain Perfluoroalkyl Acids Including Trifluoromethane Sulfonic Acid in Water Connected to Known and Suspected Point Sources in Sweden
      Bjornsdotter Maria K; Yeung Leo W Y; Karrman Anna; Jogsten Ingrid Ericson
      Environmental science & technology (2019), 53 (19), 11093-11101 ISSN:.
      Data presenting the environmental occurrence of ultra-short-chain perfluoroalkyl acids (PFAAs) are scarce and little is known about the potential sources. In this study, ultra-short-chain PFAAs were analyzed in water connected to potential point sources using supercritical fluid chromatography coupled with tandem mass spectrometry. Samples (n = 34) were collected in connection with firefighting training sites, landfills, and a hazardous waste management facility. Ultra-short-chain PFAAs were detected in all samples at concentrations up to 84 000 ng/L (.sum.C1-C3), representing up to 69% of the concentration of 29 per- and polyfluoroalkyl substances (PFASs). Trifluoroacetic acid (TFA), perfluoropropanoic acid (PFPrA), trifluoromethane sulfonic acid (TFMS), perfluoroethane sulfonic acid (PFEtS), and perfluoropropane sulfonic acid (PFPrS) were detected at concentrations up to 14 000, 53 000, 940, 1700, and 15 000 ng/L, respectively. Principal component analysis suggests that TFA is associated with landfills. PFPrS was associated with samples collected close to the source at all types of sites included in this study. These findings reveal the presence of high concentrations of ultra-short-chain PFAAs released into the environment from various sources and emphasize the large fraction of ultra-short-chain PFAAs to the total concentration of PFASs in water.
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    94. 94
      Wang, B.; Yao, Y.; Chen, H.; Chang, S.; Tian, Y.; Sun, H. Per- and Polyfluoroalkyl Substances and the Contribution of Unknown Precursors and Short-Chain (C2–C3) Perfluoroalkyl Carboxylic Acids at Solid Waste Disposal Facilities. Sci. Total Environ. 2020, 705, 135832  DOI: 10.1016/j.scitotenv.2019.135832
      94
      Per- and polyfluoroalkyl substances and contribution of unknown precursors and short-chain (C2-C3) perfluoroalkyl carboxylic acids at solid waste disposal facilities
      Wang, Bin; Yao, Yiming; Chen, Hao; Chang, Shuai; Tian, Ying; Sun, Hongwen
      Science of the Total Environment (2020), 705 (), 135832CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)
      The emission of per- and polyfluoroalkyl substances (PFASs) from municipal solid wastes (MSW) disposal raises concerns for their potential of long-term release and risks. In this study, the occurrence of PFASs was investigated in ambient air and leachate from seven MSW disposal facilities including three landfills, two incineration plants, and two MSW transfer stations in Tianjin, China. Mass loads of PFASs (≥C4) released to the atm. were estd. at 0.007-0.97 kg/y/site, which were much lower than those to leachate (0.04-1.3 kg/y/site), while emission to the atm. at landfills was more considerable. With total oxidizable precursor (TOP) assay, unknown C4-C12 perfluoroalkyl acids (PFAAs)-precursors were found contributing 10-97 mol% in leachate and accounting for addnl. 15%-43% mass loads. Using IC-Ba/Ag/H cartridges, trifluoroacetic acid (C2) and perfluoropropionic acid (C3) were recovered in leachate for TOP assay (62%-78%) and detd. at dominant levels of 19-81μg/L, which accounted for mass loads of 0.08-2.6 kg/y/site. Unknown C2-C3 PFAA-precursors contributed 12-93 mol% with mass loads of 0.10-3.0 kg/y/site. Overall, unknown C2-C12 PFAA-precursors remained contributing 0.35-68 mol% in biochem. treated leachate. This study emphasizes that the profiles of unknown PFAA-precursors released during MSW disposal are to be identified, which is essential for their environmental risk assessment.
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    95. 95
      Tsou, K.; Antell, E.; Duan, Y.; Olivares, C. I.; Yi, S.; Alvarez-Cohen, L.; Sedlak, D. L. Improved Total Oxidizable Precursor Assay for Quantifying Polyfluorinated Compounds Amenable to Oxidative Conversion to Perfluoroalkyl Carboxylic Acids. ACS ES&T Water 2023, 3 (9), 2996– 3003,  DOI: 10.1021/acsestwater.3c00224
      There is no corresponding record for this reference.
    96. 96
      Adlunger, K.; Anke, J. M.; Bachem, G.; Banning, H.; Biegel-Engler, A.; Blondzik, K.; Braun, U.; Eckhardt, A.; Gildemeister, D.; Hilliges, F.; Hoffmann, G.; Jentzsch, F.; Klitzke, S.; Kuckelkorn, J.; Martens, K.; Müller, A.; Pickl, C.; Pirntke, U.; Rechenberg, J.; Sättler, D.; Schmidt, U.; Speichert, G.; Warnke, I.; Wehner, J.; Wischer, R. Reducing the Input of Chemicals into Waters: Trifluoroacetate (TFA) as a Persistent and Mobile Substance with Many Sources; Dessau-Roßlau, Germany, 2022; pp 1– 52. https://www.umweltbundesamt.de/en/publikationen/reducing-the-input-of-chemicals-into-waters (accessed 2024–06–03).
      There is no corresponding record for this reference.
    97. 97
      Joudan, S.; De Silva, A. O.; Young, C. J. Insufficient Evidence for the Existence of Natural Trifluoroacetic Acid. Environ. Sci. Process Impacts 2021, 23 (11), 1641– 1649,  DOI: 10.1039/D1EM00306B
      97
      Insufficient evidence for the existence of natural trifluoroacetic acid
      Joudan, Shira; De Silva, Amila O.; Young, Cora J.
      Environmental Science: Processes & Impacts (2021), 23 (11), 1641-1649CODEN: ESPICZ; ISSN:2050-7895. (Royal Society of Chemistry)
      Trifluoroacetic acid (TFA) is a persistent and mobile pollutant that is present ubiquitously in the environment. As a result of a few studies reporting its presence in pre-industrial samples and a purported unaccounted source, TFA is often claimed to exist naturally. Here, we examine the evidence for natural TFA by: (i) critically evaluating measurements of TFA in pre-industrial samples; (ii) examg. the likelihood of TFA formation by hypothesized mechanisms; (iii) exploring other potential TFA sources to the deep ocean; and (iv) examg. global budgets of TFA. We conclude that the presence of TFA in the deep ocean and lack of closed TFA budget is not sufficient evidence that TFA occurs naturally, esp. without a reasonable mechanism of formation. We argue the paradigm of natural TFA should no longer be carried forward.
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    98. 98
      Ellis, D. A.; Mabury, S. A.; Martin, J. W.; Muir, D. C. G. Thermolysis of Fluoropolymers as a Potential Source of Halogenated Organic Acids in the Environment. Nature 2001, 412 (6844), 321– 324,  DOI: 10.1038/35085548
      98
      Thermolysis of fluoropolymers as a potential source of halogenated organic acids in the environment
      Ellis, David A.; Mabury, Scott A.; Martin, Jonathan W.; Muir, Derek C. G.
      Nature (London, United Kingdom) (2001), 412 (6844), 321-324CODEN: NATUAS; ISSN:0028-0836. (Nature Publishing Group)
      Following the introduction of hydrochlorofluorocarbon (HCFCs) and hydrofluorocarbon (HFCs) gases as replacements for the ozone-destroying chlorofluorocarbons (CFCs), it has been discovered that HCFCs/HFCs can degrade in the atm. to produce trifluoroacetic acid, a compd. with no known loss mechanisms in the environment, and higher concns. in natural waters have been shown to be mildly phytotoxic. Present environmental levels of trifluooracetic acid are not accounted by HCFC/HFC degrdn. alone. Here we report that thermolysis of fluorinated polymers, such as the com. polymers Teflon and Kel-F, can also produce trifluoroacetate and the similar compd. chlorodifluoroacetate. This can occur either directly, or indirectly via products that are known to degrade to these haloacetates in the atm. The environmental significance of these findings is confirmed by modeling, which indicates that the thermolysis of fluoropolymers in industrial and consumer high-temp. applications (ovens, non-stick cooking utensils and combustion engines) is likely to be a significant source of trifluoroacetate in urban rainwater (∼25 ngL-1, as estd. for Toronto). Thermolysis also leads to longer chain polyfluoro- and/or polychlorofluoro-(C3-C14) carboxylic acids which may be equally persistent. Some of these products have recently been linked with possible adverse health and environmental impacts and are being phased out of the US market. Furthermore, we detected CFCs and fluorocarbons-groups that can destroy ozone and act as greenhouse gases, resp.-among the other thermal degrdn. products, suggesting that continued use of fluoropolymers may also exacerbate stratospheric ozone-depletion and global warming.
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    99. 99
      Duchesne, A. L.; Brown, J. K.; Patch, D. J.; Major, D.; Weber, K. P.; Gerhard, J. I. Remediation of PFAS-Contaminated Soil and Granular Activated Carbon by Smoldering Combustion. Environ. Sci. Technol. 2020, 54 (19), 12631– 12640,  DOI: 10.1021/acs.est.0c03058
      99
      Remediation of PFAS-contaminated soil and granular activated carbon by smoldering combustion
      Duchesne, Alexandra L.; Brown, Joshua K.; Patch, David J.; Major, David; Weber, Kela P.; Gerhard, Jason I.
      Environmental Science & Technology (2020), 54 (19), 12631-12640CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      This study explored smoldering combustion for remediating polyfluoroalkyl substance (PFAS)-impacted granular activated carbon (GAC) and PFAS-contaminated soil. GAC, both fresh and PFAS-loaded, was employed as the supplemental fuel supporting smoldering in mixts. with sand (≈175 mg PFAS/kg GAC-sand), with PFAS-spiked, lab.-constructed soil (≈4 mg PFAS/kg soil), and with a PFAS-impacted field soil (≈0.2 mg PFAS/kg soil). The fate of PFAS and fluorine was quantified with soil and emission analyses, including targeted PFAS and suspect screening as well as hydrogen fluoride and total fluorine. Results demonstrated that exceeding 35 g GAC/kg soil resulted in self-sustained smoldering with temps. exceeding 900°C. Post-treatment PFAS concns. of the treated soil were near (2 expts.) or below (7 expts.) detection limits (0.0004 mg/kg). Further, 44% of the initial PFAS on GAC underwent full destruction, compared to 16% of the PFAS on soil. Less than 1% of the initial PFAS contamination on GAC or soil was emitted as PFAS in the quantifiable anal. suite. Results suggest that the rest were emitted as altered, shorter-chain PFAS and volatile fluorinated compds., which were scrubbed effectively with GAC. Total org. fluorine anal. proved useful for PFAS-loaded GAC in sand; however, analyzing soils suffered from interference from non-PFAS. Overall, this study demonstrated that smoldering has significant potential as an effective remediation technique for PFAS-impacted soils and PFAS-laden GAC.
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    100. 100
      Trang, B.; Li, Y.; Xue, X.-S.; Ateia, M.; Houk, K. N.; Dichtel, W. R. Low-Temperature Mineralization of Perfluorocarboxylic Acids. Science (1979) 2022, 377 (6608), 839– 845,  DOI: 10.1126/science.abm8868
      There is no corresponding record for this reference.
    101. 101
      Nödler, K.; Scheurer, M. Substances from Multiple Sources (SMS): The Presence of Multiple Primary and Secondary Sources of Persistent and Mobile Organic Contaminants Is an Upcoming Challenge for the Drinking Water Sector and Regulatory Frameworks. Environ. Sci. Technol. 2019, 53 (19), 11061– 11062,  DOI: 10.1021/acs.est.9b05168
      There is no corresponding record for this reference.
    102. 102
      ECHA. Registry of CLH intentions until outcome - Trifluoroacetic acid. https://echa.europa.eu/de/registry-of-clh-intentions-until-outcome/-/dislist/details/0b0236e188e6e587 (accessed 2024–05–15).
      There is no corresponding record for this reference.
    103. 103
      ECHA. Registry of CLH intentions until outcome - sodium trifluoroacetate and other inorganic salts of trifluoroacetic acid. https://echa.europa.eu/registry-of-clh-intentions-until-outcome/-/dislist/details/0b0236e188e8d4b8 (accessed 2024–08–12).
      There is no corresponding record for this reference.
    104. 104
      Umweltbundesamt (UBA). Ableitung Eines Gesundheitlichen Leitwertes Für Trifluoressigsäure (TFA) ; 2020; pp 1– 6. https://www.umweltbundesamt.de/sites/default/files/medien/421/dokumente/ableitung_eines_gesundheitlichen_leitwertes_fuer_trifluoressigsaeure_fuer_uba-homepage.pdf (accessed 2023–12–20).
      There is no corresponding record for this reference.
    105. 105
      RIVM. RIVM-VSP Advies 14434A02 – Drinkwaterrichtwaarde Voor Trifluorazijnzuur ; 2023; pp 1– 47. https://www.rivm.nl/documenten/bijlage-bij-rivm-brief-aan-ilt-indicatieve-drinkwaterrichtwaarde-trifluorazijnzuur-tfa (accessed 2024–08–30).
      There is no corresponding record for this reference.
    106. 106
      CLP. Harmonised classification - Annex VI of Regulation (EC) No 1272/2008 (CLP Regulation) - Trifluoroacetic acid. https://echa.europa.eu/de/information-on-chemicals/cl-inventory-database/-/discli/details/47316 (accessed 2023–12–19).
      There is no corresponding record for this reference.
    107. 107
      U.S. EPA. USEPA ECOTOX database. https://cfpub.epa.gov/ecotox/ (accessed 2023–12–15).
      There is no corresponding record for this reference.
    108. 108
      European Chemicals Bureau. Technical Guidance Document on Risk Assessment, Part II; Ispra, Italy, 2023; pp 1– 337. https://echa.europa.eu/documents/10162/987906/tgdpart2_2ed_en.pdf/138b7b71-a069-428e-9036-62f4300b752f (accessed 2024–05–14).
      There is no corresponding record for this reference.
    109. 109
      Hanson, M. L.; Madronich, S.; Solomon, K.; Sulbaek Andersen, M. P.; Wallington, T. J. Trifluoroacetic Acid in the Environment: Consensus, Gaps, and Next Steps. Environ. Toxicol. Chem. 2024, 43 (10), 2091– 2093,  DOI: 10.1002/etc.5963
      There is no corresponding record for this reference.
    110. 110
      Madronich, S.; Sulzberger, B.; Longstreth, J. D.; Schikowski, T.; Andersen, M. P. S.; Solomon, K. R.; Wilson, S. R. Changes in Tropospheric Air Quality Related to the Protection of Stratospheric Ozone in a Changing Climate. Photochemical & Photobiological Sciences 2023, 22 (5), 1129– 1176,  DOI: 10.1007/s43630-023-00369-6
      There is no corresponding record for this reference.
    111. 111
      Felizeter, S.; McLachlan, M. S.; De Voogt, P. Root Uptake and Translocation of Perfluorinated Alkyl Acids by Three Hydroponically Grown Crops. J. Agric. Food Chem. 2014, 62 (15), 3334– 3342,  DOI: 10.1021/jf500674j
      111
      Root uptake and translocation of perfluorinated alkyl acids by three hydroponically grown crops
      Felizeter, Sebastian; McLachlan, Michael S.; De Voogt, Pim
      Journal of Agricultural and Food Chemistry (2014), 62 (15), 3334-3342CODEN: JAFCAU; ISSN:0021-8561. (American Chemical Society)
      Tomato, cabbage, and zucchini plants were grown hydroponically in a greenhouse. They were exposed to 14 perfluorinated alkyl acids (PFAAs) at four different concns. via the nutrient soln. At maturity the plants were harvested, and the roots, stems, leaves, twigs (where applicable), and edible parts (tomatoes, cabbage head, zucchinis) were analyzed sep. Uptake and transfer factors were calcd. for all plant parts to assess PFAA translocation and distribution within the plants. Root concn. factors were highest for long-chain PFAAs (>C11) in all three plant species, but these chems. were not found in the edible parts. All other PFAAs were present in all above-ground plant parts, with transpiration stream concn. factors (TSCFs) of 0.05-0.25. These PFAAs are taken up with the transpiration stream and accumulate primarily in the leaves. Although some systematic differences were obsd., overall their uptake from nutrient soln. to roots and their further distribution within the plants were similar between plant species and among PFAAs.
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    112. 112
      Felizeter, S.; McLachlan, M. S.; De Voogt, P. Uptake of Perfluorinated Alkyl Acids by Hydroponically Grown Lettuce (Lactuca Sativa). Environ. Sci. Technol. 2012, 46 (21), 11735– 11743,  DOI: 10.1021/es302398u
      112
      Uptake of Perfluorinated Alkyl Acids by Hydroponically Grown Lettuce (Lactuca sativa)
      Felizeter, Sebastian; McLachlan, Michael. S.; de Voogt, Pim
      Environmental Science & Technology (2012), 46 (21), 11735-11743CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      An uptake study was carried out to assess the potential human exposure to perfluorinated alkyl acids (PFAAs) through the ingestion of vegetables. Lettuce (Lactuca sativa) was grown in PFAA-spiked nutrient solns. at four different concns., ranging from 10 ng/L to 10 μg/L. Eleven perfluorinated carboxylic acids (PFCAs) and three perfluorinated sulfonic acids (PFSAs) were analyzed by HPLC-MS/MS. At the end of the expt., the major part of the total mass of each of the PFAAs (except the short-chain, C4-C7, PFCAs) taken up by plants appeared to be retained in the nonedible part, viz. the roots. Root concn. factors (RCF), foliage/root concn. factors (FRCF), and transpiration stream concn. factors (TSCF) were calcd. For the long chained PFAAs, RCF values were highest, whereas FRCF were lowest. This indicates that uptake by roots is likely governed by sorption of PFAAs to lipid-rich root solids. Translocation from roots to shoots is restricted and highly depending on the hydrophobicity of the compds. Although the TSCF show that longer-chain PFCAs (e.g., perfluorododecanoic acid) get better transferred from the nutrient soln. to the foliage than shorter-chain PFCAs (e.g., perfluoroheptanoic acid), the major fraction of longer-chain PFCAs is found in roots due to addnl. adsorption from the spiked soln. Due to the strong electron-withdrawing effect of the fluorine atoms the role of the neg. charge of the dissocd. PFAAs is likely insignificant.
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    113. 113
      Gredelj, A.; Nicoletto, C.; Polesello, S.; Ferrario, C.; Valsecchi, S.; Lava, R.; Barausse, A.; Zanon, F.; Palmeri, L.; Guidolin, L.; Bonato, M. Uptake and Translocation of Perfluoroalkyl Acids (PFAAs) in Hydroponically Grown Red Chicory (Cichorium Intybus L.): Growth and Developmental Toxicity, Comparison with Growth in Soil and Bioavailability Implications. Science of The Total Environment 2020, 720, 137333  DOI: 10.1016/j.scitotenv.2020.137333
      There is no corresponding record for this reference.
    114. 114
      Hubert, M.; Arp, H. P. H.; Hansen, M. C.; Castro, G.; Meyn, T.; Asimakopoulos, A. G.; Hale, S. E. Influence of Grain Size, Organic Carbon and Organic Matter Residue Content on the Sorption of per- and Polyfluoroalkyl Substances in Aqueous Film Forming Foam Contaminated Soils - Implications for Remediation Using Soil Washing. Science of The Total Environment 2023, 875, 162668  DOI: 10.1016/j.scitotenv.2023.162668
      There is no corresponding record for this reference.
    115. 115
      Nguyen, T. M. H.; Bräunig, J.; Thompson, K.; Thompson, J.; Kabiri, S.; Navarro, D. A.; Kookana, R. S.; Grimison, C.; Barnes, C. M.; Higgins, C. P.; Mclaughlin, M. J.; Mueller, J. F. Influences of Chemical Properties, Soil Properties, and Solution PH on Soil-Water Partitioning Coefficients of Per- And Polyfluoroalkyl Substances (PFASs). Environ. Sci. Technol. 2020, 54 (24), 15883– 15892,  DOI: 10.1021/acs.est.0c05705
      115
      Influences of chemical properties, soil properties, and solution pH on soil-water partitioning coefficients of per- and polyfluoroalkyl substances (PFASs)
      Nguyen, Thi Minh Hong; Braunig, Jennifer; Thompson, Kristie; Thompson, Jack; Kabiri, Shervin; Navarro, Divina A.; Kookana, Rai S.; Grimison, Charles; Barnes, Craig M.; Higgins, Christopher P.; McLaughlin, Michael J.; Mueller, Jochen F.
      Environmental Science & Technology (2020), 54 (24), 15883-15892CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)
      The aim of this study was to assess the soil-water partitioning behavior of a wider range of per- and polyfluoroalkyl substances (PFASs) onto soils covering diverse soil properties. The PFASs studied include perfluoroalkyl carboxylates (PFCAs), perfluoroalkane sulfonates (PFSAs), fluorotelomer sulfonates (FTSs), nonionic perfluoroalkane sulfonamides (FASAs), cyclic PFAS (PFEtCHxS), per- and polyfluoroalkyl ether acids (GenX, ADONA, 9Cl-PF3ONS), and three aq. film-forming foam (AFFF)-related zwitterionic PFASs (AmPr-FHxSA, TAmPr-FHxSA, 6:2 FTSA-PrB). Soil-water partitioning coeffs. (log Kd values) of the PFASs ranged from less than zero to approx. three, were chain-length-dependent, and were significantly linearly related to mol. wt. (MW) for PFASs with MW > 350 g/mol (R2 = 0.94, p < 0.0001). Across all soils, the Kd values of all short-chain PFASs (≤5 -CF2- moieties) were similar and varied less (<0.5 log units) compared to long-chain PFASs (>0.5 to 1.5 log units) and zwitterions AmPr- and TAmPr-FHxSA (~ 1.5 to 2 log units). Multiple soil properties described sorption of PFASs better than any single property. The effects of soil properties on sorption were different for anionic, nonionic, and zwitterionic PFASs. Soln. pH could change both PFAS speciation and soil chem. affecting surface complexation and electrostatic processes. The Kd values of all PFASs increased when soln. pH decreased from approx. eight to three. Short-chain PFASs were less sensitive to soln. pH than long-chain PFASs. The results indicate the complex interactions of PFASs with soil surfaces and the need to consider both PFAS type and soil properties to describe mobility in the environment.
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    116. 116
      McLachlan, M. S.; Felizeter, S.; Klein, M.; Kotthoff, M.; De Voogt, P. Fate of a Perfluoroalkyl Acid Mixture in an Agricultural Soil Studied in Lysimeters. Chemosphere 2019, 223, 180– 187,  DOI: 10.1016/j.chemosphere.2019.02.012
      116
      Fate of a perfluoroalkyl acid mixture in an agricultural soil studied in lysimeters
      McLachlan, Michael S.; Felizeter, Sebastian; Klein, Michael; Kotthoff, Matthias; De Voogt, Pim
      Chemosphere (2019), 223 (), 180-187CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)
      Perfluoroalkyl acids (PFAAs) are environmental contaminants of concern in both food and drinking water. PFAA fate in agricultural soil is an important determinant of PFAA contamination of groundwater and crops. The fate of C4-C14 perfluorinated carboxylic acids (PFCAs) and two perfluorinated sulfonic acids (PFSAs) in an agricultural soil was studied in a field lysimeter expt. Soil was spiked with PFAAs at four different levels and crops were planted. PFAA concns. in soil were measured at the beginning and end of the growing season. Lysimeter drainage water was collected and analyzed. The concns. of all PFAAs decreased in the surface soil during the growing season, with the decrease being neg. correlated with the no. of fluorinated carbons in the PFAA mol. PFAA transfer to the drainage water was also neg. correlated with the no. of fluorinated carbons. For the C11-C14 PFCAs most of the decrease in soil concn. was attributed to the formation of non-extractable residues. For the remaining PFAAs leaching was the dominant removal process. Leaching was concn. dependent, with more rapid removal from the soils spiked with higher PFAA levels. Model simulations based on measured Kd values under-predicted removal by leaching. This was attributed to mixt. effects that reduced PFAA sorption to soil.
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    117. 117
      Gredelj, A.; Nicoletto, C.; Valsecchi, S.; Ferrario, C.; Polesello, S.; Lava, R.; Zanon, F.; Barausse, A.; Palmeri, L.; Guidolin, L.; Bonato, M. Uptake and Translocation of Perfluoroalkyl Acids (PFAA) in Red Chicory (Cichorium Intybus L.) under Various Treatments with Pre-Contaminated Soil and Irrigation Water. Science of The Total Environment 2020, 708, 134766  DOI: 10.1016/j.scitotenv.2019.134766
      There is no corresponding record for this reference.
    118. 118
      Xu, B.; Alizray, R.; Lammel, D. R.; Riedel, S.; Rillig, M. C. Concentration-Dependent Response of Soil Parameters and Functions to Trifluoroacetic Acid. Eur. J. Soil Sci. 2022, 73 (4), e13266  DOI: 10.1111/ejss.13266
      There is no corresponding record for this reference.
    119. 119
      Bott, T. L.; Standley, L. J. Incorporation of Trifluoroacetate, a Hydrofluorocarbon Decomposition Byproduct, by Freshwater Benthic Microbial Communities. Water Res. 1999, 33 (6), 1538– 1544,  DOI: 10.1016/S0043-1354(98)00359-5
      There is no corresponding record for this reference.
    120. 120
      Lu, Y.; Liu, L.; Ning, A.; Yang, G.; Liu, Y.; Kurtén, T.; Vehkamäki, H.; Zhang, X.; Wang, L. Atmospheric Sulfuric Acid-Dimethylamine Nucleation Enhanced by Trifluoroacetic Acid. Geophys. Res. Lett. 2020, 47 (2), e2019GL085627  DOI: 10.1029/2019GL085627
      There is no corresponding record for this reference.
    121. 121
      Liu, L.; Yu, F.; Tu, K.; Yang, Z.; Zhang, X. Influence of Atmospheric Conditions on the Role of Trifluoroacetic Acid in Atmospheric Sulfuric Acid-Dimethylamine Nucleation. Atmos Chem. Phys. 2021, 21 (8), 6221– 6230,  DOI: 10.5194/acp-21-6221-2021
      There is no corresponding record for this reference.
    122. 122
      Rockström, J.; Steffen, W.; Noone, K.; Persson, Å.; Chapin, F. S.; Lambin, E. F.; Lenton, T. M.; Scheffer, M.; Folke, C.; Schellnhuber, H. J.; Nykvist, B.; de Wit, C. A.; Hughes, T.; van der Leeuw, S.; Rodhe, H.; Sörlin, S.; Snyder, P. K.; Costanza, R.; Svedin, U.; Falkenmark, M.; Karlberg, L.; Corell, R. W.; Fabry, V. J.; Hansen, J.; Walker, B.; Liverman, D.; Richardson, K.; Crutzen, P.; Foley, J. A. A Safe Operating Space for Humanity. Nature 2009, 461 (7263), 472– 475,  DOI: 10.1038/461472a
      122
      A safe operating space for humanity
      Rockstrom Johan; Steffen Will; Noone Kevin; Persson Asa; Chapin F Stuart 3rd; Lambin Eric F; Lenton Timothy M; Scheffer Marten; Folke Carl; Schellnhuber Hans Joachim; Nykvist Bjorn; de Wit Cynthia A; Hughes Terry; van der Leeuw Sander; Rodhe Henning; Sorlin Sverker; Snyder Peter K; Costanza Robert; Svedin Uno; Falkenmark Malin; Karlberg Louise; Corell Robert W; Fabry Victoria J; Hansen James; Walker Brian; Liverman Diana; Richardson Katherine; Crutzen Paul; Foley Jonathan A
      Nature (2009), 461 (7263), 472-5 ISSN:.
      There is no expanded citation for this reference.
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    123. 123
      Steffen, W.; Richardson, K.; Rockström, J.; Cornell, S. E.; Fetzer, I.; Bennett, E. M.; Biggs, R.; Carpenter, S. R.; De Vries, W.; De Wit, C. A.; Folke, C.; Gerten, D.; Heinke, J.; Mace, G. M.; Persson, L. M.; Ramanathan, V.; Reyers, B.; Sörlin, S. Planetary Boundaries: Guiding Human Development on a Changing Planet. Science (1979) 2015, 347 (6223), 1259855  DOI: 10.1126/science.1259855
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      Caldeira, C.; Farcal, R.; Garmendia Aguirre, I.; Mancini, L.; Tosches, D.; Amelio, A.; Rasmussen, K.; Rauscher, H.; Riego Sintes, J.; Sala, S. Safe and Sustainable by Design Chemicals and Materials - Framework for the Definition of Criteria and Evaluation Procedure for Chemicals and Materials; Publications Office of the European Union, 2022; pp 1– 124.  DOI: 10.2760/487955 .
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    125. 125
      Roy, M. A.; Cousins, I.; Harriman, E.; Scheringer, M.; Tickner, J. A.; Wang, Z. Combined Application of the Essential-Use and Functional Substitution Concepts: Accelerating Safer Alternatives. Environ. Sci. Technol. 2022, 56 (14), 9842– 9846,  DOI: 10.1021/acs.est.2c03819
      125
      Combined Application of the Essential-Use and Functional Substitution Concepts: Accelerating Safer Alternatives
      Roy, Monika A.; Cousins, Ian; Harriman, Elizabeth; Scheringer, Martin; Tickner, Joel A.; Wang, Zhanyun
      Environmental Science & Technology (2022), 56 (14), 9842-9846CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)
      There is no expanded citation for this reference.
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    126. 126
      Chirsir, P.; Palm, E. H.; Baskaran, S.; Schymanski, E. L.; Wang, Z.; Wolf, R.; Hale, S. E.; Arp, H. P. H. Grouping Strategies for Assessing and Managing Persistent and Mobile Substances. Environ. Sci. Eur. 2024, 36 (1), 102,  DOI: 10.1186/s12302-024-00919-4
      There is no corresponding record for this reference.

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