Identification of Novel Iodinated Polyfluoroalkyl Ether Acids and Other Emerging PFAS in Soils Using a Nontargeted Molecular Network Approach DOI

Yuyan Ji,

Yitao Pan,

Xiaoting Miao

et al.

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 31, 2024

Despite advancements in high-resolution screening techniques, the identification of novel perfluoroalkyl and polyfluoroalkyl substances (PFAS) remains challenging without prior structural information. In view this, we proposed implemented a new data-driven algorithm to calculate spectral similarity among PFAS, facilitating generation molecular networks screen for unknown compounds. Using this approach, 81 PFAS across 12 distinct classes were identified soil samples collected near an industrial park Shandong Province, China, including first reported occurrence iodine-substituted PFAS. Among them, standards four polyfluorinated ether sulfonates (I-PFESA) successfully synthesized, enabling confirmation subsequent quantitative analysis. Although median concentration ∑I-PFESA (0.74 ng/g dw) was lower than that ∑H-PFESA (hydrogen-substituted, 61.96 ∑Cl-PFESA (chlorine-substituted, 2.98 dw), embryotoxicity assays zebrafish revealed 6:2 I-PFESA exhibited greater toxicity compared Cl-PFESA same chain length. This highlights need closer examination toxic effects I-PFESA. Notably, algorithm, based on similarity, provides perspectives environmental behavior transformation I-PFESA, although further investigation is required elucidate underlying mechanisms their toxicity.

Language: Английский

Nontarget Analysis and Characterization of a Group of Abundant Polyfluoroalkyl Substances─Fluorinated Benzoylurea Pesticides and Their Analogues and Transformation Products in Fish by LC-HRMS and Chemical Species-Specific Algorithms DOI
Caiming Tang,

Yizhe Zhu,

Yiyang Liang

et al.

Journal of Agricultural and Food Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 13, 2025

Poly- and perfluoroalkyl substances (PFASs) are a large class of fluorinated chemicals used in various industrial agrochemical products such as benzoylurea (FBU) pesticides. Initiated from an incidental preliminary finding three high-abundance FBUs fish, this study implemented nontarget analysis characterization for together with their analogues transformation (TPs) fish using liquid chromatography, high-resolution mass spectrometry, chemical species-specific algorithms. A total 23 FBU-relevant compounds were found tentatively/accurately elucidated structures, including 18 PFASs 5 non-PFAS compounds, which 4 original FBUs, 8 FBU analogues, 11 FBU-TPs. The concentrations 0.8–1919.3 ng/g the samples. strategy data-processing algorithms can be extended to other fluorine-containing pesticides, results provide new understanding PFAS pollution unveil important source pollutants, utilization FBUs.

Language: Английский

Citations

0
Mass Spectrometry-Based Spatial Multiomics Revealed Bioaccumulation Preference and Region-Specific Responses of PFOS in Mice Cardiac Tissue DOI Creative Commons
Rui Shi, Yanyan Chen, Wenlong Wu

et al.

Environmental Science & Technology, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 22, 2025

The distribution and bioaccumulation of environmental pollutants are essential to understanding their toxicological mechanism. However, achieving spatial resolution at the subtissue level is still challenging. Perfluorooctanesulfonate (PFOS) a persistent pollutant with widespread occurrence. behavior PFOS complicated by its dual affinity for phospholipids protein albumin. It intriguing visualize preference investigate differential microenvironment responses level. Herein, we developed mass-spectrometry (MS)-based multiomics workflow, integrating matrix-assisted laser desorption/ionization MS imaging, microdissection, liquid chromatography analysis. This integrated workflow elucidates in mouse cardiac tissue, highlighting preferential accumulation pericardium over myocardium. pattern results greater toxicity pericardium, significantly altering cardiolipin levels disrupting energy metabolism lipid transport pathways. Our approach provides novel insights into demonstrates significant potential revealing complex molecular mechanisms underlying health impacts pollutants.

Language: Английский

Citations

0
Exploring the Chemical Complexity and Sources of Airborne Fine Particulate Matter in East Asia by Nontarget Analysis and Multivariate Modeling DOI Creative Commons
Jean Froment, Jong‐Uk Park, Sang‐Woo Kim

et al.

Environmental Science & Technology, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 27, 2025

The complex and dynamic nature of airborne fine particulate matter (PM2.5) has hindered understanding its chemical composition, sources, toxic effects. In the first steps a larger study, here, we aimed to elucidate relationships between source regions, ambient conditions, composition in water extracts PM2.5 samples (n = 85) collected over 16 months at an observatory Yellow Sea. each extract, quantified elements major ions profiled mixtures organic compounds by nontarget mass spectrometry. More than 50,000 features were detected, consensus silico tools, assigned molecular formula 13,907 features. Oxygenated most prominent, followed mixed nitrogenated/oxygenated compounds, sulfates, sulfonates. Spectral matching enabled identification or structural annotation 43 substances, workflow involving SIRIUS MS-DIAL software 74 unknown per- polyfluoroalkyl substances with primary regions China Korean Peninsula. Multivariate modeling revealed seasonal variations chemistry, attributable combination warmer temperatures maritime summer cooler winter.

Language: Английский

Citations

0
Perfluoroalkyl and Polyfluoroalkyl Substances Interact with Platelet Glycoprotein Ibα and Exacerbate Thrombosis DOI
Ming Liu, Weiqing Zhao, Chao Ma

et al.

Published: Jan. 1, 2025

Language: Английский

Citations

0
Entropy Similarity-Driven Transformation Reaction Molecular Networking Reveals Transformation Pathways and Potential Risks of Emerging Contaminants in Wastewater: The Example of Sartans DOI

Yuli Qian,

Yunhao Ke,

Liye Wang

et al.

Environmental Science & Technology, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 19, 2025

The transformation pathways and risks of emerging contaminants (ECs) in wastewater remain unclear due to the limited throughput nontarget screening. In this study, an improved method called entropy similarity-driven reaction molecular networking (ESTRMN) was developed identify products (TPs) wastewater. detail, similarity most effective algorithm for identifying parent-product spectrum pairs a threshold 0.5 it determined with guarantee high specificity. Additionally, TP structure database predicted according known structures reactions established assist identification. Sartan is one commonly used angiotensin II receptor blocker antihypertensive drugs. Take sartans as example, 69 TPs confidence levels above 3 were identified by ESTRMN, 43 which newly discovered. common included hydroxylation, hydrolysis, oxidation, resulting majority sartan exhibiting higher persistence, mobility, toxicity (PMT) than their parents. concentration 75% increased after treatment WWTP, overall risk has not been effectively mitigated. This study emphasizes role ESTRMN incorporating ECs into environmental monitoring protocols assessment frameworks management.

Language: Английский

Citations

0
Development of a Nontargeted Algorithm for Per- and Polyfluoroalkyl Substances in the FT-ICR Mass Spectra of Complex Organic Mixtures DOI
Qing‐Long Fu, Y.S. Cheng, Jibao Liu

et al.

Analytical Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: March 6, 2025

The unrivaled mass resolving power and subppm error enable the application of Fourier transform ion cyclotron resonance spectrometry (FT-ICR MS) for nontargeted screening per- polyfluoroalkyl substances (PFAS). Few automated FT-ICR MS methods exist analysis PFAS in solutions containing other dissolved organic matter. In this study, isotopic pattern dynamic homologous series inspection were complementarily employed FTMSDeu algorithm to simultaneously assign chemical formulas molecules, with an overall assignment accuracy 91.2% 1,802 unique their 11,634 formulas. negative effects fluorine-related isobaric isotopes sub-mDa differences on formula natural matter addressed by empirical F/(H + X) rule adoption a threshold number plus number. There 203 one novel formula, C9H6O4S1I1F11, identified fluoropolymer industry-impacted river water sample using our analyzing spectra. Overall, results study highlighted great potential updated high-throughput spectra complex mixtures from real environmental samples.

Language: Английский

Citations

0
Unraveling the Exposure Spectrum of PFAS in Fluorochemical Occupational Workers: Structural Diversity, Temporal Trends, and Risk Prioritization DOI
Yanna Liu, Yunhe Guo,

Meilin Lv

et al.

Environmental Science & Technology, Journal Year: 2025, Volume and Issue: unknown

Published: March 18, 2025

Despite extensive poly/perfluoroalkyl substance (PFAS) discovery studies in various samples, the exposure spectrum fluorochemical occupational workers remains largely unexplored. Here, serum samples from 28 at a facility were analyzed using nontarget techniques, identifying 64 PFAS classes, including 15 novel ones such as pentafluorosulfur ether-substituted perfluoroalkyl sulfonic acids, hydrogen-substituted perfluoroalkylamines, and perfluoroalkylsulfonyl protocatechualdehyde esters. Temporal trend analyses (2008–2018) revealed stable levels for most but an increase perfluorobutanoic acid (PFBA) perfluorohexanesulfonic (PFHxS), suggesting industrial shifts long-chain to short-chain homologues China since early 2010s. Commonly reported structurally modified (e.g., hydrogen/carbonyl/chlorine substitution, ether insertion, unsaturation) likely historical byproducts of legacy production rather than intentionally manufactured alternatives. A Toxicological Priority Index-based risk assessment, integrating mobility, persistence, bioaccumulation indices, identified di(perfluoroakyl sulfonyl)imides, acids/carboxylic perfluoroalkylsulfonamidoacetic acids high-risk chemicals. Overall, exhibited higher mobility lower persistence PFAS, except chlorinated variants, which showed increased potential. This study highlights critical gaps historically emitted emphasizes need large-scale monitoring assessments manage emerging PFAS.

Language: Английский

Citations

0
Accurate Detection and High Throughput Profiling of Unknown PFAS Transformation Products for Elucidating Degradation Pathways DOI
Bei Zhang, Jibao Liu, S M Qing

et al.

Water Research, Journal Year: 2025, Volume and Issue: 282, P. 123645 - 123645

Published: April 15, 2025

Language: Английский

Citations

0
Identification of Novel Iodinated Polyfluoroalkyl Ether Acids and Other Emerging PFAS in Soils Using a Nontargeted Molecular Network Approach DOI

Yuyan Ji,

Yitao Pan,

Xiaoting Miao

et al.

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 31, 2024

Despite advancements in high-resolution screening techniques, the identification of novel perfluoroalkyl and polyfluoroalkyl substances (PFAS) remains challenging without prior structural information. In view this, we proposed implemented a new data-driven algorithm to calculate spectral similarity among PFAS, facilitating generation molecular networks screen for unknown compounds. Using this approach, 81 PFAS across 12 distinct classes were identified soil samples collected near an industrial park Shandong Province, China, including first reported occurrence iodine-substituted PFAS. Among them, standards four polyfluorinated ether sulfonates (I-PFESA) successfully synthesized, enabling confirmation subsequent quantitative analysis. Although median concentration ∑I-PFESA (0.74 ng/g dw) was lower than that ∑H-PFESA (hydrogen-substituted, 61.96 ∑Cl-PFESA (chlorine-substituted, 2.98 dw), embryotoxicity assays zebrafish revealed 6:2 I-PFESA exhibited greater toxicity compared Cl-PFESA same chain length. This highlights need closer examination toxic effects I-PFESA. Notably, algorithm, based on similarity, provides perspectives environmental behavior transformation I-PFESA, although further investigation is required elucidate underlying mechanisms their toxicity.

Language: Английский

Citations

0