Bypassing the Identification: MS2Quant for Concentration Estimations of Chemicals Detected with Nontarget LC-HRMS from MS² Data

Analytical Chemistry, Journal Year: 2023, Volume and Issue: 95(33), P. 12329 - 12338

Published: Aug. 7, 2023

Nontarget analysis by liquid chromatography-high-resolution mass spectrometry (LC-HRMS) is now widely used to detect pollutants in the environment. Shifting away from targeted methods has led detection of previously unseen chemicals, and assessing risk posed these newly detected chemicals an important challenge. Assessing exposure toxicity with nontarget HRMS highly dependent on knowledge structure chemical. However, majority features screening remain unidentified therefore assessment conventional tools hampered. Here, we developed MS2Quant, a machine learning model that enables prediction concentration fragmentation (MS2) spectra detected, but chemicals. MS2Quant xgbTree algorithm-based regression using ionization efficiency data for 1191 unique spans 8 orders magnitude. The values are predicted structural fingerprints can be computed SMILES notation identified or MS2 SIRIUS+CSI:FingerID software. root mean square errors training test sets were 0.55 (3.5×) 0.80 (6.3×) log-units, respectively. In comparison, approaches depend assigning unequivocal typically yield 2× 6×. quantification was validated set 39 environmental resulted error 7.4×, geometric 4.5×, median 4.0×. For based PaDEL descriptors depends assignment same dataset. latter approach yielded comparable 9.5×, 5.6×, 5.2× validation when top as input. This confirms extract information which, although have thus far been disregarded due lack accurate quantification. available R-package GitHub improving discovery monitoring potentially hazardous screening.

Language: Английский

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Architectural design of 2D covalent organic frameworks (COFs) for pharmaceutical pollutant removal

npj Clean Water, Journal Year: 2024, Volume and Issue: 7(1)

Published: April 15, 2024

Abstract Macrolide antibiotics, including erythromycin, clarithromycin, and azithromycin, are frequently misused for human treatment globally. Therefore, they were considered high-risk substances on the Union-wide monitoring Watch list under Regulation 2018/840/EU. The present work investigates adsorption behavior of pharmaceutical pollutants 1,3,5-tris (4-aminophenyl) benzene/2,5 dimethoxyterephthalaldehyde (TAPB-DMTP) covalent organic frameworks (COFs). In this study, we employ molecular dynamics simulations well-tempered metadynamics to evaluate affinity pristine their functionalized form (F-COFs) removal four distinct pollutant molecules (PPMs): erythromycin (EMC), dexamethasone (DEG), azithromycin (AZM), clarithromycin (CMC). We utilized MD examine impact two different temperatures (298 310 K) enhancing contaminants from wastewater by COFs/F-COFs. To process, several descriptors calculated simulation trajectories, interaction energies, root-mean-square deviation, radial distribution function, solvent-accessible surface area, mean square displacement, number hydrogen bonds (HB). It is determined that HB X–H⋯π (X = C, N, O; π aromatic system) interactions most critical factors contributing system stability. addition, it shown COFs with a pore-based structure have higher capacity removing pollutants. free energy landscapes confirm global minimum typically associated formation bonds. At 298 K, minima DEG/F-COFs −665.81, AZM/F-COFs −638.53, EMC/F-COFs −566.31, CMC/F-COFs −326.75 KJ mol −1 .

Language: Английский

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Non-target screening in water analysis: recent trends of data evaluation, quality assurance, and their future perspectives

Analytical and Bioanalytical Chemistry, Journal Year: 2024, Volume and Issue: 416(9), P. 2125 - 2136

Published: Feb. 1, 2024

Abstract This trend article provides an overview of recent advancements in Non-Target Screening (NTS) for water quality assessment, focusing on new methods data evaluation, qualification, quantification, and assurance (QA/QC). It highlights the evolution NTS processing, where open-source platforms address challenges result comparability complexity. Advanced chemometrics machine learning (ML) are pivotal identification correlation analysis, with a growing emphasis automated workflows robust classification models. The also discusses rigorous QA/QC measures essential NTS, such as internal standards, batch effect monitoring, matrix assessment. examines progress quantitative (qNTS), noting ionization efficiency-based quantification predictive modeling despite sample variability analytical standards. Selected studies illustrate NTS’s role combining high-resolution mass spectrometry chromatographic techniques enhanced chemical exposure addresses prioritization challenges, highlighting integration database searches computational tools efficiency. Finally, outlines future research needs including establishing comprehensive guidelines, improving measures, reporting results. underscores potential to integrate multivariate chemometrics, AI/ML tools, multi-way into combine various sources understand ecosystem health protection comprehensively.

Language: Английский

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De facto Water Reuse: Investigating the Fate and Transport of Chemicals of Emerging Concern from Wastewater Discharge through Drinking Water Treatment Using Non-targeted Analysis and Suspect Screening

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(5), P. 2468 - 2478

Published: Jan. 22, 2024

Wastewater is a source for many contaminants of emerging concern (CECs), and surface waters receiving wastewater discharge often serve as water downstream drinking treatment plants. Nontargeted analysis suspect screening methods were used to characterize chemicals in residence-time-weighted grab samples companion polar organic chemical integrative samplers (POCIS) collected on three separate hydrologic sampling events along flow path representative de facto reuse. The goal this work was examine the fate CECs study transported from effluent through treatment. Grab POCIS provided comparison between single-point sample results. This unique rigorous design, coupled with advanced analytical chemistry tools, important insights into found their potential sources, which can be help prioritize further study. K-means clustering identify patterns occurrences across both sites events. Chemical features that occurred frequently or survived prioritized identification, resulting probable identification over 100 watershed 28 treated water.

Language: Английский

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Pyrolysis temperature dependent effects of biochar on shifting fluorescence spectrum characteristics of soil dissolved organic matter under warming

The Science of The Total Environment, Journal Year: 2023, Volume and Issue: 892, P. 164656 - 164656

Published: June 5, 2023

Language: Английский

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Increasing chemical coverage, accuracy, and reproducibility of the processing method for polar organic chemical integrative samplers

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

Published: Feb. 1, 2025

Despite their diffusion in research studies, passive samplers are rarely used regulatory applications. To expand the employment of environmental standardized procedures for processing each sampler type should be proposed and accepted, but currently, study develops its own protocol based on previous knowledge specific needs. In this work, six identical polar organic chemical integrative seawater were deployed to understand importance sorbent transfer method prior elution step. A common "wet transfer" with ultra-pure water was compared a less diffused "dry-transfer," assessing recoveries matrix effects 38 target compounds emerging concern, including pesticides, recreational food-related substances, pharmaceuticals, industrial additives, ultra-violet (UV) filters. The dry-transfer procedure generally allowed better recoveries, especially more compounds, without affecting (which remained range 40-130%). Along recovery assessment, analysis non-spiked extracts revealed traces many targeted contaminants, quantifying perfluorooctanoic acid, UV-filters, carbamazepine, diclofenac, triclosan. Furthermore, other found below limits quantitation. Ten analytes detected only dry-transferred samplers, highlighting applying protocol, when dealing compounds. This refined method, therefore, permits reproducible strategy, at same time enlarging set which could quantified.

Language: Английский

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Assessing the spatiotemporal variability of dissolved organic matter fluorescence composition in the Lake George, NY watershed

Biogeochemistry, Journal Year: 2024, Volume and Issue: 167(6), P. 849 - 870

Published: May 15, 2024

Abstract Lake George (LG) is a temperate, oligotrophic, medium-sized lake (114 km 2 ) located in northeastern New York State (U.S.). Lakes are highly understudied environments where extensive dissolved organic matter (DOM) processing occurs. With this study we establish the foundation for researching biogeochemistry of LG watershed, particular, numerous tributaries flowing into lake. Collected were 213 samples from 64 and 12 locations. Some had unique wastewater, agricultural, or wetland influences. We employed fluorescence spectroscopy, common biogeochemical technique, to characterize fluorescent DOM (FDOM) component. developed parallel factor analysis (PARAFAC) model deconvolution FDOM data allowing depict six underlying constituents, which varied source reactivity on spatiotemporal scales. Tributary DOM, comparison was much more aromatic, larger molecular weight, humic, contained less protein-like material. The distribution humic PARAFAC components impacted by land-use wastewater Supporting characterization chromophoric (CDOM) total (on carbon basis) allowed differentiating influence wetlands, could not be depicted spatiotemporally assessing variability components. Temporal assessment revealed minor variabilities tributary quantity quality except cases point sources such as treatment facilities. Overall, primer establishes baseline understanding baseflow levels constituents broadly, presents spectra temperate oligotrophic watersheds LG.

Language: Английский

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Pollution by Polar Pesticides and Pharmaceuticals and Risk Assessment in Surface Water Bodies Along the French Mediterranean Coast: Complementarity of Target and Non-Target Screenings

Published: Jan. 1, 2025

Language: Английский

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Pollution by polar pesticides and pharmaceuticals and risk assessment in surface water bodies along the French Mediterranean coast: Complementarity of target and non-target screenings

Environmental Chemistry and Ecotoxicology, Journal Year: 2025, Volume and Issue: unknown

Published: April 1, 2025

Language: Английский

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Scientometric review: Concentration and toxicity assessment in environmental non-targeted LC/HRMS analysis

Trends in Environmental Analytical Chemistry, Journal Year: 2023, Volume and Issue: 40, P. e00217 - e00217

Published: Oct. 13, 2023

Non-targeted screening with LC/HRMS is a go-to approach to discover relevant contaminants in environmental water samples that contain an abundance of chemicals. The rapidly increasing popularity non-targeted has initiated development diverse set methods for assessing the concentration and toxicity detected This review aims benchmark trends NTS literature particular focus on (1) used quantification tentatively identified chemicals lack analytical standards, (2) chemicals, (3) combining former into risk evaluation. Here we provide scientometric these strategies based Web Science referenced papers published between 2019 2022. General show assessments are widely employed NTS, reaching 66% 45% over four years, respectively. Simultaneously, only 13% covered here combine results factor or similar. With this aim highlight advantages gaps approaches assessment guidelines more homogeneous data interrogation extrapolation.

Language: Английский

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