Occurrence of per- and polyfluoroalkyl substances in water: a review

Wang, Yifei; Kim, Juhee; Huang, Ching-Hua; Hawkins, Gary L.; Li, Ké; Chen, Yongsheng; Huang, Qingguo

doi:10.1039/d1ew00851j

Cited by 6 publications

(6 citation statements)

References 126 publications

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“…2 and 3 , S1–S7). Our results are also in agreement with the earlier reports (Jensen and Warming 2015 ; Kar et al 2017 ; Li et al 2020 ; Mortensen et al 2020 ; Wang et al 2022 ), demonstrating that longer carbon chains of PFASs favor stronger interactions with TTR than their shorter-chained counterparts through hydrophobic interactions and thereby enhance binding affinity with TTR and eventually more toxic than the short-chain analogs. According to OECD 2020 report, long-chain PFASs are being progressively replaced with short-chain PFASs’ alternatives in US and Europe (Brendel et al 2018 ; OECD 2020 ; Ren et al 2016 ).…”

Section: Discussionsupporting

confidence: 93%

In silico analysis decodes transthyretin (TTR) binding and thyroid disrupting effects of per- and polyfluoroalkyl substances (PFAS)

2022

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Transthyretin (TTR) is a homo-tetramer protein involved in the transport of thyroid hormone (thyroxine; T4) in the plasma and cerebrospinal fluid. Many pollutants have been shown to bind to TTR, which could be alarming as disruption in the thyroid hormone system can lead to several physiological problems. It is also indicated that the monomerization of tetramer and destabilization of monomer can lead to amyloidogenesis. Many compounds are identified that can bind to tetramer and stabilize the tetramer leading to the inhibition of amyloid fibril formation. Other compounds are known to bind tetramer and induce amyloid fibril formation. Among the pollutants, per- and polyfluoroalkyl substances (PFAS) are known to disrupt the thyroid hormone system. The molecular mechanisms of thyroid hormone disruption could be diverse, as some are known to bind with thyroid hormone receptors, and others can bind to membrane transporters. Binding to TTR could also be one of the important pathways to alter thyroid signaling. However, the molecular interactions that drive thyroid-disrupting effects of long-chain and short-chain PFASs are not comprehensively understood at the molecular level. In this study, using a computational approach, we show that carbon chain length and functional group in PFASs are structural determinants, in which longer carbon chains of PFASs and sulfur-containing PFASs favor stronger interactions with TTR than their shorter-chained counterparts. Interestingly, short-chain PFAS also showed strong binding capacity, and the interaction energy for some was as close to the longer-chain PFAS. This suggests that short-chain PFASs are not completely safe, and their use and build-up in the environment should be carefully regulated. Of note, TTR homologs analysis suggests that thyroid-disrupting effects of PFASs could be most likely translated to TTR-like proteins and other species.

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Section: Discussionsupporting

confidence: 93%

In silico analysis decodes transthyretin (TTR) binding and thyroid disrupting effects of per- and polyfluoroalkyl substances (PFAS)

2022

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“…We found that the degradation products were restricted to one hydrodefluorination product (C 4 F 8 HSO 3 − ) based on e aq − , whereas daughter species (C 4 F 7 H 2 SO 3 − ) appeared in the products under the CO 2 −• system, suggesting that CO 2 −• achieved defluorination from more locations on PFBS compared to e aq − . 19 F NMR characterization identified the defluorination location of PFBS in the above two systems, enriching the structure comprehension of the defluorinated products. As shown in Figure 4c, the initial hydrodefluorination location is on the β carbon of PFBS in the e aq − system, which affirmed the previous theoretical calculations involving C−F bond dissociation energy (BDE).…”

Section: ■ Materials and Methodsmentioning

confidence: 87%

“…Further, we both observed the formation of the hydrodefluorination product (C 4 F 8 HSO . 19 F NMR characterization identified the defluorination location of PFBS in the above two systems, enriching the structure comprehension of the defluorinated products. As shown in Figure 4c, the initial hydrodefluorination location is on the β carbon of PFBS in the e aq − system, which affirmed the previous theoretical calculations involving C−F bond dissociation energy (BDE).…”

Section: ■ Materials and Methodsmentioning

confidence: 87%

“…For decades, per- and polyfluoroalkyl substances (PFAS) chemicals have been widely used in various consumer, medical, and industrial products. − Owing to environmental persistence and being notoriously hazardous, the long-chain PFAS chemicalsperfluorooctanoate (PFOA) and perfluorooctanesulfonate (PFOS)have been prohibited under international regulations. , However, many short-chain fluorinated alternatives remain in use, and they could also be accumulated via physicochemical degradation pathways of longer-chain PFAS. − Even though the use of hydrated electron (e aq – )-based advanced reductive technology (e aq – -ART) has recently shown to be effective to destruct both perfluoroalkyl carboxylates (PFxA, x = number of carbons comprising the hydrophobic tail) and perfluoroalkyl sulfonates (PFxS), − PFxS with short fluoroalkyl chains such as PFBS (C 4 F 9 SO 3 – ) remains an exceptional case and displays very sluggish reactivity . To date, the abundance of short-chain PFAS from numerous sources has already been detected in most locations on the planet. − Recent toxicological studies revealed that the potential threats to human health posed by analogs had been underestimated due to increased solubility, mobility, and inertness. − Thus, their complete removal and decomposition from the aquatic environment has become an urgent concern.…”

Section: Introductionmentioning

confidence: 99%

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Transient Kinetics of Short-Chain Perfluoroalkyl Sulfonate with Radiolytic Reducing Species

Jiang

Adjei

Denisov

et al. 2022

Environ. Sci. Technol. Lett.

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The role of the short-lived hydrated electron (e aq − ) has recently begun to be appreciated in per-and polyfluoroalkyl substances (PFAS) remediations; nevertheless, few studies to date focused on short-chain PFAS, and their effective defluorination has been limited by an insufficient mechanistic understanding, which starts with the elusive initial step of e aq − reduction. Herein, this study uses pulse radiolysis to clarify the rate constant of the e aq − reaction with a highly recalcitrant short-chain PFAS, perfluorobutanesulfonate (PFBS, C 4 F 9 SO 3 − ), and verify chain length dependence. The measured values contradict earlier results from laser photolysis but reconcile with the apparent degradation profiles and theoretical predictions. Besides, we first disclose radiolytic carbon dioxide radicals (CO 2 −• ) to defluorinate PFBS with an initial reaction constant of 4.8 × 10 7 M −1 s −1 , and it achieves selective cleavage on the more obstinate C−F bond than e aq − even under a neutral condition. Quantitative 60 Co γ-ray irradiation experiments further show that initial reduction occurs through a defluorination pathway rather than a desulfurization pathway, and the redox potential of PFBS exceeds −2.0 eV. This radiolytic study addressed the long-standing mechanistic contradictions regarding short-chain PFAS degradation and suggested ionizing radiation as a versatile and direct treatment technique.

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“…Different classes of emerging contaminants, their source of origin, and their adverse health effects are listed in Table 1 . Emerging contaminants can be primarily classified as organic, inorganic, microbial, perfluoroalkylated, and radioactive substances [ 3 , 6 , 7 , 8 , 9 , 10 ]. They do not degrade or hydrolyze easily and are persistent in the environment, resulting in bioaccumulation [ 6 ].…”

Section: Introductionmentioning

confidence: 99%

Advanced Polymeric Nanocomposite Membranes for Water and Wastewater Treatment: A Comprehensive Review

Sahu¹,

Dosi

Kwiatkowski

et al. 2023

Polymers

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Nanomaterials have been extensively used in polymer nanocomposite membranes due to the inclusion of unique features that enhance water and wastewater treatment performance. Compared to the pristine membranes, the incorporation of nanomodifiers not only improves membrane performance (water permeability, salt rejection, contaminant removal, selectivity), but also the intrinsic properties (hydrophilicity, porosity, antifouling properties, antimicrobial properties, mechanical, thermal, and chemical stability) of these membranes. This review focuses on applications of different types of nanomaterials: zero-dimensional (metal/metal oxide nanoparticles), one-dimensional (carbon nanotubes), two-dimensional (graphene and associated structures), and three-dimensional (zeolites and associated frameworks) nanomaterials combined with polymers towards novel polymeric nanocomposites for water and wastewater treatment applications. This review will show that combinations of nanomaterials and polymers impart enhanced features into the pristine membrane; however, the underlying issues associated with the modification processes and environmental impact of these membranes are less obvious. This review also highlights the utility of computational methods toward understanding the structural and functional properties of the membranes. Here, we highlight the fabrication methods, advantages, challenges, environmental impact, and future scope of these advanced polymeric nanocomposite membrane based systems for water and wastewater treatment applications.

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Occurrence of per- and polyfluoroalkyl substances in water: a review

Abstract: Per- and polyfluoroalkyl substances (PFASs) have drawn increasing concern due to their widespread presence and persistence in the environment. In contrast, standard methods and manuals have been developed only recently...

Cited by 6 publications

References 126 publications

In silico analysis decodes transthyretin (TTR) binding and thyroid disrupting effects of per- and polyfluoroalkyl substances (PFAS)

In silico analysis decodes transthyretin (TTR) binding and thyroid disrupting effects of per- and polyfluoroalkyl substances (PFAS)

Transient Kinetics of Short-Chain Perfluoroalkyl Sulfonate with Radiolytic Reducing Species

Advanced Polymeric Nanocomposite Membranes for Water and Wastewater Treatment: A Comprehensive Review

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