Two-layer homolog network approach for PFAS nontarget screening and retrospective data mining

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Jan. 15, 2025

Abstract The rapid increase of novel per- and polyfluoroalkyl substances (PFAS) raises concerns, while their identification remains challenging. Here, we develop a two-layer homolog network approach for PFAS nontarget screening using mass spectrometry. first layer constructs networks between homologs, with evaluation showing that it filters 94% false candidates. second builds classes to expedite the PFAS. We detected 94 in twelve waterproof products two related industrial sludges, including 36 not previously reported any sample. A local dataset is constructed retrospective analysis by re-analyzing our previous samples, revealing fifteen samples collected 2005. retrieval public database MassIVE uncovers from seven countries. reveal historic global presence PFAS, providing guidance management policy-making concerning persistent chemicals.

Language: Английский

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Emerging perfluoroalkyl substances in environmental waters revealed by non-targeted screening

Current Opinion in Environmental Science & Health, Journal Year: 2024, Volume and Issue: 37, P. 100531 - 100531

Published: Jan. 4, 2024

Language: Английский

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PFΔScreen — an open-source tool for automated PFAS feature prioritization in non-target HRMS data

Analytical and Bioanalytical Chemistry, Journal Year: 2023, Volume and Issue: 416(2), P. 349 - 362

Published: Nov. 30, 2023

Abstract Per- and polyfluoroalkyl substances (PFAS) are a huge group of anthropogenic chemicals with unique properties that used in countless products applications. Due to the high stability their C-F bonds, PFAS or transformation (TPs) persistent environment, leading ubiquitous detection various samples worldwide. Since industrial chemicals, availability authentic reference standards is limited, making non-target screening (NTS) approaches based on high-resolution mass spectrometry (HRMS) necessary for more comprehensive characterization. NTS usually time-consuming process, since only small fraction detected can be identified. Therefore, efficient prioritization relevant HRMS signals one most crucial steps. We developed PFΔ Screen , Python-based open-source tool simple graphical user interface (GUI) perform feature using several PFAS-specific techniques such as highly promising MD/C-m/C approach, Kendrick defect analysis, diagnostic fragments (MS 2 ), fragment differences suspect screening. Feature from vendor-independent MS raw data (mzML, data-dependent acquisition) performed via pyOpenMS (or custom lists) subsequent calculations identification both HPLC- GC-HRMS data. The workflow presented four PFAS-contaminated agricultural soil south-western Germany. Over 15 classes (more than 80 single compounds isomers) could identified, including novel classes, potentially TPs precursors fluorotelomer mercapto alkyl phosphates (FTMAPs). within Python environment easily automatically installable executable Windows. Its source code freely available GitHub ( https://github.com/JonZwe/PFAScreen ). Graphical abstract

Language: Английский

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Can Qualitative Nontarget Data Be Indicative of PFAS Contamination? First Evidence by Correlation with EOF in Environmental Samples

Environmental Science & Technology Letters, Journal Year: 2024, Volume and Issue: 11(9), P. 996 - 1001

Published: July 17, 2024

Language: Английский

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Non-target screening reveals 124 PFAS at an AFFF-impacted field site in Germany specified by novel systematic terminology

Analytical and Bioanalytical Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 28, 2024

Language: Английский

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Transforming PFAS management: A critical review of machine learning applications for enhanced monitoring and treatment

Journal of Water Process Engineering, Journal Year: 2025, Volume and Issue: 70, P. 106941 - 106941

Published: Jan. 15, 2025

Language: Английский

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Prioritization Strategies in Non-Target Screening of Environmental Samples by Chromatography – High-Resolution Mass Spectrometry: A Tutorial

Published: Jan. 1, 2025

Language: Английский

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Assessment of PFAS contamination in agricultural soils: non-target identification of precursors, fluorine mass balance and microcosm studies

Journal of Hazardous Materials, Journal Year: 2025, Volume and Issue: unknown, P. 137798 - 137798

Published: Feb. 1, 2025

Language: Английский

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Development of a Nontargeted Algorithm for Per- and Polyfluoroalkyl Substances in the FT-ICR Mass Spectra of Complex Organic Mixtures

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

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Multidimensional Separations for Characterization of Isomeric PFAS Using SLIM High-Resolution Ion Mobility and Tandem Mass Spectrometry

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

Published: March 17, 2025

Per- and polyfluoroalkyl substances (PFAS) are synthetic organofluorine compounds that accumulate in the environment due to significant industrial use resistance degradation. PFAS of global interest because their environmental health concerns. They exist a variety linear nonlinear forms containing isomers, as well differing functional headgroups for each class. That structural complexity requires advanced analytical techniques, beyond current high-resolution mass spectrometry (HRMS) methods, accurate identification quantification wide range samples. Herein, we demonstrate power Structures Lossless Ion Manipulations (SLIM)-based ion mobility (HRIM) separation complex branched isomers. SLIM is integrated into multidimensional LC-SLIM IM-MS/MS workflow, developed extensive characterization compounds. As surveyed sulfonate carboxylic acid classes PFAS, observed unique arrival time vs m/z trend lines were representative class; these important allowing emerging species based on placement two-dimensional space. Next, used complementary tandem (MS/MS) approaches with all fragmentation (AIF), energy-resolved MS/MS, further investigate structure mobility-separated species. This allowed both investigation mechanism fragment ions could allow differentiation isomers when was insufficient. Overall, combination chromatography, SLIM, MS/MS provided comprehensive workflow capable identifying unknown

Language: Английский

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