Discriminative Behavior of Cyclodextrin Polymers against Dissolved Organic Matter: Role of Cavity Size and Sorbate Properties DOI
David Glöckler,

Mourad Harir,

Philippe Schmitt‐Kopplin

и другие.

Analytical Chemistry, Год журнала: 2023, Номер 95(39), С. 14582 - 14591

Опубликована: Сен. 18, 2023

Cyclodextrin polymers (CDPs) are promising next-generation adsorbents in water purification technologies. The selectivity of the polymer derivate cross-linked with tetrafluoroterephthalonitrile (TFN-CDP) for nonionic and cationic micropollutants (MPs) over dissolved organic matter (DOM) renders adsorbent also attractive many analytical applications. molecular drivers observed are, nonetheless, not yet fully understood. To provide new insights into sorption mechanism, we (i) synthesized TFN-CDPs different cavity sizes (α-, β-, γ-CDP); (ii) assessed their extraction efficiencies selected MPs competition DOM size fractions (<1, 1-3, 3-10, >10 kDa) to test size-selectivity; (iii) performed nontargeted, ultrahigh resolution Fourier transform ion cyclotron resonance mass spectrometry analysis on CDP-extracted compounds (<1 probe sorbate properties governing selective sorption. First, no evidence size-selectivity was obtained through either CD or two independent approaches (iii). Second, found a dominant impact oxygenation polarity MPs, respectively, relatively oxygen-poor/nonpolar molecules favorably retained all α-, γ-CDP. Third, our data indicates exclusion an anionic matrix, such as carboxylic acids, but preferential nitrogen-bearing DOM, pointing at repulsive forces negatively charged cross-linker likely reason. Therefore, ascribe TFN-CDP's nonpolar electrostatic interactions between MPs/DOM building blocks. These can further aid optimization efficient sorbent design environmental

Язык: Английский

Perspectives of compound-specific isotope analysis of organic contaminants for assessing environmental fate and managing chemical pollution DOI
Thomas B. Hofstetter, Rani Bakkour, Daniel Büchner

и другие.

Nature Water, Год журнала: 2024, Номер 2(1), С. 14 - 30

Опубликована: Янв. 17, 2024

Язык: Английский

Процитировано

30

Tripodal receptor cross-linked polymer as a promising adsorbent for iodine vapor capture and adsorption from water DOI
Arivazhagan Roja,

Sankar Srividhya,

M. Arunachalam

и другие.

Polymer, Год журнала: 2024, Номер 294, С. 126688 - 126688

Опубликована: Янв. 17, 2024

Язык: Английский

Процитировано

6

Cyclodextrin polymers containing ionizable and ionic groups: A comprehensive review from classifications and synthesis methods to applications DOI
Elmira Kashani, Saeid Maghsoudi,

Hamid Rezania

и другие.

Materials Today Chemistry, Год журнала: 2024, Номер 39, С. 102186 - 102186

Опубликована: Июль 1, 2024

Язык: Английский

Процитировано

4

Role of membrane porosity in passive sampling of aquatic contaminants for stable isotope analysis: enhancement of analyte accumulation rates and selectivity DOI Creative Commons

Armela Tafa,

Anat Bernstein, Martin Elsner

и другие.

Analytical and Bioanalytical Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Янв. 31, 2025

Abstract Compound-specific isotope analysis (CSIA) is a potent method for illustrating the in situ degradation of aquatic contaminants. However, its application to surface and groundwater hindered by low contaminant concentrations, typically nanogram-per-litre range, requiring processing large water volumes. Polar organic chemical integrative samplers (POCIS) have shown promising results when combined with CSIA, yet their extended deployment time accumulate sufficient analyte mass remains major limitation. In our study, we addressed this issue increasing pore size polyethersulfone membrane (PES) from 0.1 8 $$\upmu $$ μ m. This resulted significant increases accumulation rates atrazine (3.5-fold), S-metolachlor (3.4-fold), boscalid (3.0-fold). Importantly, larger sizes did not compromise isotopic integrity, $$\Delta \delta ^{13}$$ Δ δ 13 C $$\le +0.4\pm 0.1$$ + 0.4 ± 0.1 ‰ ^{15}$$ 15 N -0.6\pm 0.4$$ - 0.6 ‰, both within accepted uncertainties. Additionally, observed an enhanced selectivity pores towards target analytes over humic acids, whereas no increase (bio)fouling potential was detected m membrane, as demonstrated gravimetric analysis, SEM measurements, rates, ratios fouled unfouled POCIS. Our findings show that reduces expedites required gas chromatography ratio spectrometry, offering expand CSIA low-concentration pesticide field. Graphical abstract

Язык: Английский

Процитировано

0

Quartz Crystal Microbalance as a Holistic Detector for Quantifying Complex Organic Matrices during Liquid Chromatography: 2. Compound-Specific Isotope Analysis DOI Creative Commons
Christopher Wabnitz, Wei Chen, Martin Elsner

и другие.

Analytical Chemistry, Год журнала: 2024, Номер 96(19), С. 7436 - 7443

Опубликована: Май 3, 2024

In carbon-compound-specific isotope analysis (carbon CSIA) of environmental micropollutants, purification samples is often required to guarantee accurate measurements a target compound. A companion paper has brought forward an innovative approach couple quartz crystal microbalance (QCM) with high-performance liquid chromatography (HPLC) for the online quantification matrices during gradient HPLC purification. This work investigates benefit polar micropollutants typically present in samples. Here, we studied impact natural organic matter (NOM) on isotopic integrity model analytes and suitability NOM-to-analyte ratio as proxy sample purity. We further investigated limitations enhancement using QCM C18 C8 phases single multiple targets. Strong shifts up 3.3% toward signature NOM were observed ≥10. Thanks QCM, optimization matrix removal 99.8% was possible late-eluting compounds. The efficiency deteriorated when aiming simultaneous two or three compounds, leading 2.5% less removal. Our results suggest that one optimized can be achieved through systematic screening 3 5 different gradients, thereby shift boundaries carbon CSIA by 2 orders magnitude lower micropollutant concentrations.

Язык: Английский

Процитировано

3

Lack of selectivity in sample preparation ‒ An achilles heel of compound-specific isotope analysis for environmental micropollutants DOI Creative Commons
Rani Bakkour, Christopher Wabnitz, David Glöckler

и другие.

TrAC Trends in Analytical Chemistry, Год журнала: 2024, Номер 180, С. 117908 - 117908

Опубликована: Авг. 12, 2024

The role of compound-specific isotope analysis (CSIA) in environmental research has been proven over the last few decades. Despite advances analytical methods and instrumentation, applying CSIA to low-concentration contaminants, especially at field scale, remains limited. In this perspective paper, we argue that limitation stems from underdeveloped sample preparation techniques, particularly lack required selectivity. Drawing an extensive review nearly 600 studies on (i) analyze methodologies' distribution dedication studies, discussing their connection with maturity suitable techniques. Additionally, (ii) examine general trends sorbent phase technologies, assessing adequacy meet CSIA's targeted nature applicability micropollutants. advocating for a paradigm shift, (iii) emphasize need adapt future development strategies light past current innovations.

Язык: Английский

Процитировано

3

Extending the potential of Fourier transform ion cyclotron resonance mass spectrometry for the analysis of disinfection by-products DOI Creative Commons
Anna Andersson,

Mourad Harir,

David Bastviken

и другие.

TrAC Trends in Analytical Chemistry, Год журнала: 2023, Номер 167, С. 117264 - 117264

Опубликована: Сен. 7, 2023

Potentially harmful disinfection by-products (DBPs) are formed upon drinking water treatment when disinfectants react with organic matter in the water. Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) provides information on compositions of individual DBPs unknown, toxicologically relevant fraction, comprising non-volatile, high-molecular weight DBPs. This review evaluates current applications FT-ICR-MS for DBP analysis to assist improved this technique. Four methodological aspects focus, 1) The use quenching agents, 2) choice extraction method 3) ionization techniques/modes, and 4) Data processing including formula verification interpretation. Quenching can lead decomposition or adduct formation needs be further evaluated avoided. There is a large potential expand by applying different SPE sorbents techniques, systematic procedures important ensure reliable non-target analysis.

Язык: Английский

Процитировано

6

Nitrogen stable isotope analysis of sulfonamides by derivatization-gas chromatography-isotope ratio mass spectrometry DOI Creative Commons

Qingyuan Dou,

Aoife Canavan,

Yuhao Fu

и другие.

Analytical and Bioanalytical Chemistry, Год журнала: 2024, Номер 416(19), С. 4237 - 4247

Опубликована: Июнь 7, 2024

Abstract The continuous introduction of micropollutants into the environment through livestock farming, agricultural practices, and wastewater treatment is a major concern. Among these pollutants are synthetic sulfonamide antibiotics such as sulfamethoxazole, which not always fully degraded pose risk fostering antimicrobial resistance. It challenging to assess degradation sulfonamides with conventional concentration measurements. This study introduces compound-specific isotope analysis nitrogen ratios at natural abundances by derivatization-gas chromatography hyphenated ratio mass spectrometry (derivatization-GC-IRMS) new more precise method for tracing origin sulfonamides. Here, sulfamethoxazole was used model compound develop optimize derivatization conditions using (trimethylsilyl)diazomethane reagent. With optimized conditions, accurate reproducible δ 15 N derivatization-GC-IRMS achieved in two different laboratories limit 3 nmol on column, corresponding 0.253 µg non-derivatized SMX. Application four further sulfonamides, sulfadiazine, sulfadimethoxine, sulfadimidine, sulfathiazole, shows versatility developed method. Its benefit demonstrated first application, highlighting possibility distinguishing from suppliers pharmaceutical products. Graphical

Язык: Английский

Процитировано

1

Current trends and challenges in the analysis of marine environmental contaminants by isotope ratio mass spectrometry DOI
Olga V. Kuznetsova

Analytical and Bioanalytical Chemistry, Год журнала: 2023, Номер 416(1), С. 71 - 85

Опубликована: Ноя. 18, 2023

Язык: Английский

Процитировано

3

Selectivity of β-Cyclodextrin Polymer toward Aquatic Contaminants: Insights from Ultrahigh-Resolution Mass Spectrometry of Dissolved Organic Matter DOI
David Glöckler,

Mourad Harir,

Philippe Schmitt‐Kopplin

и другие.

Analytical Chemistry, Год журнала: 2023, Номер 95(42), С. 15505 - 15513

Опубликована: Окт. 13, 2023

Selectivity in solid-phase extraction (SPE) materials has become increasingly important for analyte enrichment sensitive analytical workflows to alleviate detrimental matrix effects. Molecular-level investigation of constituents, which are preferentially extracted or excluded, can provide the chemist with valuable information learn about their control on sorbent selectivity. In this work, we employ nontargeted Fourier transform ion cyclotron resonance mass spectrometry (FTICR MS) elucidate molecular chemodiversity freshwater-derived dissolved organic matter (DOM) by selective model β-cyclodextrin polymer (β-CDP) comparison conventional, universal SPE sorbents (i.e., Oasis HLB, Supel-Select and LiChrolut EN). Statistical analysis MS data corroborated highly nature β-CDP revealing DOM spectra that most dissimilar original compositions. We found its selectivity was characterized pronounced discrimination against oxygenated unsaturated compounds, were associated classes lignin-like, tannin-like, carboxylic-rich alicyclic molecules. contrast, conventional excluded less compounds showed a more behavior wide range compositional space. lay these findings larger context aids analyst obtaining an priori estimate toward any target interest serving thereby optimization sample preparation. This study highlights great value ultrahigh-resolution better understanding targeted analytics provides new insights into sorption novel sorbents.

Язык: Английский

Процитировано

2