Machine learning assisted single-molecule sensing of per- and polyfluoroalkyl carboxylic acids: Quantification without standards DOI
Kaipei Qiu, Jiaqi Zuo,

H B Li

и другие.

Research Square (Research Square), Год журнала: 2024, Номер unknown

Опубликована: Июль 15, 2024

Abstract Per- and polyfluoroalkyl carboxylic acids (PFCA) are of great concern due to their ubiquitous presence in the environment. Despite a severe shortage authentic standards, compared rapid increase possible structures identified, it remains difficult quantify mixture PFCA without references. Herein, standard-free single-molecule electrochemical sensing method was developed for first time by establishing linear correlation between current blockades volumes simulated molecular dynamics. A nearly 100% accuracy realized simultaneous determination 13 pristine or H- / Cl-substituted PFCA, using frequency-modulated multi-feature classification. Shortlisting 21 high-priority features reduced required number training data 7.6 folds, almost 80% quantification reliability maintained even with interference 100 times concentration. Moreover, detection limit trifluoroacetic acid (an ultrashort-chain PFCA) went down 57 ng·L-1, comparable state-of-the-art performance.

Язык: Английский

Trifluoroacetic Acid: Toxicity, Sources, Sinks and Future Prospects DOI Open Access
María de los A. Garavagno, Rayne Holland, M. Anwar H. Khan

и другие.

Sustainability, Год журнала: 2024, Номер 16(6), С. 2382 - 2382

Опубликована: Март 13, 2024

Trifluoroacetic acid (TFA) is a known and persistent pollutant in the environment. Although several direct anthropogenic sources exist, production from atmospheric degradation of fluorocarbons such as some hydrofluorocarbons (HFCs) has been source for time. The current transition HFCs to HFOs (hydrofluoroolefins) beneficial global warming viewpoint because are much shorter-lived pose smaller threat terms warming, but fraction converted into TFA higher than seen corresponding region which produced close source. Therefore, it timely review role Earth’s This considers its toxicity, removal processes, measurement variety environments, future prospects. New model integrations used quantify impacts uncertainties on levels using Henry’s Law constant range gas-phase kinetic parameters chosen reaction OH radicals with representative HFO (HFO-1234yf). Model runs suggest that surface concentrations vary by up 10% based data could be 25% previously modelled values depending analysis adopted. estimates require updating warrants further investigation. toxicity appears low, studies wider animal plant types required.

Язык: Английский

Процитировано

21

Stability and Biotransformation of 6:2 Fluorotelomer Sulfonic Acid, Sulfonamide Amine Oxide, and Sulfonamide Alkylbetaine in Aerobic Sludge DOI
Bo Fang, Yaozhi Zhang, Hao Chen

и другие.

Environmental Science & Technology, Год журнала: 2024, Номер 58(5), С. 2446 - 2457

Опубликована: Янв. 5, 2024

The 6:2 fluorotelomer sulfonamide (6:2 FTSAm)-based compounds signify a prominent group of per- and polyfluoroalkyl substances (PFAS) widely used in contemporary aqueous film-forming foam (AFFF) formulations. Despite their widespread presence, the biotransformation behavior these wastewater treatment plants remains uncertain. This study investigated FTSAm-based amine oxide FTNO), alkylbetaine FTAB), sulfonic acid FTSA) aerobic sludge over 100-day incubation period. alkylamine FTAA), primary intermediate product FTNO, was indirectly assessed. Their stability ranked based on estimated half-lives (t1/2): FTAB (no obvious products were detected) ≫ FTSA (t1/2 ≈28.8 days) > FTAA ≈11.5 FTNO ≈1.2 days). Seven transformation 15 identified through nontarget suspect screening using high-resolution mass spectrometry. pathways proposed. Interestingly, FTSAm hardly hydrolyzed to further biotransformed perfluoroalkyl carboxylic acids (PFCAs). Furthermore, novel for generation perfluoroheptanoic (PFHpA) from revealed.

Язык: Английский

Процитировано

16

Forever Chemicals, Per-and Polyfluoroalkyl Substances (PFAS), in Lubrication DOI Creative Commons
Darrius Dias,

Jake Bons,

Abhishek Kumar

и другие.

Lubricants, Год журнала: 2024, Номер 12(4), С. 114 - 114

Опубликована: Март 29, 2024

Per- and polyfluoroalkyl substances (PFAS), also known as forever chemicals, exhibit exceptional chemical stability resistance to environmental degradation thanks their strong C-F bonds nonpolar nature. However, widespread use persistence have a devastating impact on the environment. This review examines roles of PFAS in tribological applications, specifically lubricants lubricating systems. article focuses conventional advanced lubricants, including ionic liquids (ILs) modern automotive vehicles. The objective this paper is provide comprehensive overview adverse impacts whilst acknowledging outstanding performance surface coatings, composite materials, additives oils greases. pathways through which are introduced into environment via systems such seals O-rings identified, alongside subsequent dispersion routes interfaces across they interact. Furthermore, we examine toxicological implications exposure terrestrial aquatic life forms, plants, animals, humans, along with ecological consequences bioaccumulation biomagnification trophic levels ecosystems. ends potential remediation strategies for use, treatment technologies, biodegradation, recovery recycling methods, search more environmentally benign alternatives.

Язык: Английский

Процитировано

13

Nontarget Identification of Novel Organophosphorus Flame Retardants and Plasticizers in Indoor Air and Dust from Multiple Microenvironments in China DOI

Yang Ji,

Yiming Yao, Xiaoxiao Li

и другие.

Environmental Science & Technology, Год журнала: 2024, Номер 58(18), С. 7986 - 7997

Опубликована: Апрель 24, 2024

The indoor environment is a typical source for organophosphorus flame retardants and plasticizers (OPFRs), yet the characteristics of OPFRs in different microenvironments remain less clear. This study collected 109 air samples 34 paired dust from 4 within university Tianjin, China, including dormitory, office, library, information center. 29 target were analyzed, novel compounds (NOPs) identified by fragment-based nontarget analysis. Target exhibited highest concentrations 46.2–234 ng/m3 20.4–76.0 μg/g, respectively, center, where chlorinated dominant. Triphenyl phosphate (TPHP) was primary OPFR office air, while tris(2-chloroethyl) dominated dust. TPHP predominant library. Triethyl (TEP) ubiquitous tris(2-butoxyethyl) particularly high 9 25 NOPs first time, mainly center such as bis(chloropropyl) 2,3-dichloropropyl phosphate. Diphenyl phosphinic acid, two hydroxylated methylated metabolites tris(2,4-ditert-butylphenyl) phosphite (AO168), dimer newly reported environment. widely associated with OPFRs, their human exposure risk environmental behaviors warrant further study.

Язык: Английский

Процитировано

11

Nontarget Analysis of Legacy and Emerging PFAS in a Lithium-Ion Power Battery Recycling Park and Their Possible Toxicity Measured Using High-Throughput Phenotype Screening DOI
Zenghua Qi,

Yutian Cao,

Dan Li

и другие.

Environmental Science & Technology, Год журнала: 2024, Номер 58(32), С. 14530 - 14540

Опубликована: Июль 17, 2024

Driven by the global popularity of electric vehicles and shortage critical raw materials for batteries, spent lithium-ion power battery (LIPB) recycling industry has exhibited explosive growth in both quantity scale. However, relatively little information is known about environmental risks posed LIPB recycling, particular with regards to perfluoroalkyl polyfluoroalkyl substances (PFAS). In this work, suspect screening nontarget analysis were carried out characterize PFAS soil, dust, water sediment from a area. Twenty-five nine classes identified at confidence level 3 or above, including 13 legacy 12 emerging PFAS, as well two ultrashort-chain PFAS. Based on target 16 least detected each sample, indicating their widespread presence Perfluorodecanoic acid, perfluorooctanesulfonic acid trifluoromethanesulfonamide showed significant differences four phenotypic parameters (growth, movement, survival fecundity)

Язык: Английский

Процитировано

9

Identification of Emerging Per- and Polyfluoroalkyl Substances (PFAS) in E-waste Recycling Practices and New Precursors for Trifluoroacetic Acid DOI
Mujtaba Baqar, Maosen Zhao,

Rimsha Saleem

и другие.

Environmental Science & Technology, Год журнала: 2024, Номер 58(36), С. 16153 - 16163

Опубликована: Авг. 23, 2024

Electronic waste is an emerging source of per- and polyfluoroalkyl substance (PFAS) emissions to the environment, yet contribution from hazardous recycling practices in South Asian region remains unclear. This study detected 41 PFAS soil samples e-waste sites Pakistan total concentrations were 7.43–367 ng/g dry weight (dw) (median: 37.7 dw). Trifluoroacetic acid (TFA) 6:2 fluorotelomer sulfonic emerged as dominant PFAS, constituting 49% 13% concentrations, respectively. Notably, nine CF3-containing identified by high-resolution mass spectrometry (HRMS)-based screening. Specifically, hexafluoroisopropanol bistriflimide (NTf2) consistently across all samples, with quantified reaching up 854 90 dw, suggests their potential association electronic manufacturing processes. Furthermore, except for NTf2, confirmed precursors TFA molar yields 8.87–40.0% TOP assay validation Milli-Q water. Overall, this reveals significant emission emphasizes identification sources precursor transformation, which are essential risk assessment.

Язык: Английский

Процитировано

5

Nontarget Discovery of Per- and Polyfluoroalkyl Sulfonyl Halides in Soils by Integration of Derivatization and Specific Fragment-Based Liquid Chromatography-High Resolution Mass Spectrometry Screening DOI
Kun Wang, Xin Xiao, Zhengzheng Liu

и другие.

Environmental Science & Technology, Год журнала: 2024, Номер 58(23), С. 10287 - 10297

Опубликована: Май 28, 2024

Though long recognized as synthetic precursors to other poly- and perfluoroalkyl substances (PFASs), most sulfonyl halides (PASXs) cannot be directly measured have generally received minimal attention. Inspired by the redox reaction between halide groups p-toluenethiol in organic chemistry, we developed a novel nontarget analysis strategy for PASXs intergrating derivatization specific fragment-based liquid chromatography-high resolution mass spectrometry screening m/z 82.961 [SO2F–] 95.934 [S2O2–]. By using this strategy, discovered 11 PASXs, namely, fluorides (5), polyfluoroalkyl (2), unsaturated fluoride (1), chlorides (3) soil samples collected from an abandoned fluorochemical manufacturing park. These average ∑PASXs concentrations were 1120 μg kg–1 (range: 9.7–9860 kg–1), which very likely key intermediates undesired byproducts of electrochemical fluorination processes. Spatial variation ratio ∑PFSAs 0.7–795%) also indicates their different transportation pathways. More importantly, decline increase sulfonates (when compared prior study at site) suggest continued hydrolysis relatively fast environmental transformation rates park soils. Overall, these findings demonstrated utility may change inferred further could adapted structures, distribution, studies PFASXs matrices.

Язык: Английский

Процитировано

4

Non-Targeted PFAS Suspect Screening and Quantification of Drinking Water Samples Collected through Community Engaged Research in North Carolina’s Cape Fear River Basin DOI Creative Commons
Rebecca A. Weed,

Grace Campbell,

Lacey Brown

и другие.

Toxics, Год журнала: 2024, Номер 12(6), С. 403 - 403

Опубликована: Май 31, 2024

A community engaged research (CER) approach was used to provide an exposure assessment of poly- and perfluorinated (PFAS) compounds in North Carolina residential drinking water. Working concert with partners, who acted as liaisons local residents, samples were collected by residents from three different locations along the Cape Fear River basin: upper, middle, lower areas river. Residents either water their homes or recreational near residence that then submitted partners for PFAS analysis. All processed using weak anion exchange (WAX) solid phase extraction analyzed a non-targeted suspect screening well quantitative included panel 45 analytes, several which are specific chemical industries collection site locations. The approach, utilized list (obtained EPA CompTox database) identified at level two confidence rating (Schymanski scale); fluorinated insecticide, herbicide, polymer chemistry, another is battery production. Notably, locations, PFOA (39.8 ng/L) PFOS (205.3 levels exceeded mandatory maximum contaminant (MCL) 4 ng/L. Additionally, sites had detectable unique manufacturer. These findings communicated back disseminated this information help empower aid making decisions reducing exposure.

Язык: Английский

Процитировано

4

Thermal Destruction Pathways and Kinetics for NTf2 and Longer-Chain Bis(perfluoroalkanesulfonyl)imides (Bis-FASIs) DOI Creative Commons
Jens Blotevogel, Wenchao Lu, Anthony K. Rappé

и другие.

Environmental Science & Technology Letters, Год журнала: 2024, Номер 11(11), С. 1254 - 1259

Опубликована: Окт. 18, 2024

A growing number of recent studies have reported the global environmental occurrence bis(perfluoroalkanesulfonyl)imides (bis-FASIs). While shorter-chain bis-FASIs such as NTf2 (aka bis(trifluoromethanesulfonyl)imide or bistriflimide) are often tied to battery and energy sectors, aqueous film-forming foams may be potential sources longer-chain bis-FASIs. As remediation technologies for destruction these persistent per- polyfluoroalkyl substances (PFAS) urgently needed but not yet been identified, we investigated effectiveness incineration using quantum chemical calculations. At temperatures around 600 °C, parent readily decompose through carbon–sulfur bond cleavage a minor extent nitrogen–sulfur cleavage. However, mineralization released perfluoroalkyl substituent HF CO2 only proceeds at >900 °C. Temperature requirements slightly increase with chain length due time required break additional C–C bonds. Under conditions ≥1000 °C typical secondary combustion units in hazardous waste incinerators, complete thermal is viable given all other process variables optimized. The same true treatment operating lower gas-phase unless catalytic effects activation barriers.

Язык: Английский

Процитировано

4

Overcoming challenges in the analysis of short-chain per- and polyfluoroalkyl substances in raw landfill leachates: Clean-up method optimization and interference identification DOI
Liping Chen, Jiaxi Wang, Xia Yu

и другие.

Journal of Hazardous Materials, Год журнала: 2025, Номер 489, С. 137518 - 137518

Опубликована: Фев. 5, 2025

Язык: Английский

Процитировано

0