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1.
Sci Total Environ ; 914: 169832, 2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38190919

RESUMO

Antibiotics, recognized as Emerging Contaminants (ECs), have raised concerns due to their pervasive presence in wastewater treatment plants (WWTPs) and subsequent release into aquatic environments, posing potential ecological risks and contributing to the development of antibiotic-resistant genes. The COVID-19 pandemic prompted an unprecedented surge in antibiotic consumption, necessitating a comprehensive assessment of its impact on antibiotic levels in wastewater. In this light, a four-year monitoring study (2020-2023) was conducted in a WWTP located in the Northern Greece (Thessaloniki), employing High-Resolution Mass Spectrometry (HRMS) technology to monitor twenty antibiotics, during distinct phases pre-, during, and post-COVID-19. Our findings revealed that macrolides and fluoroquinolones were among the most often detected categories during the sampling period. Among the compounds detected, azithromycin and clarithromycin showed the most significant increases during the pandemic, doubling their average concentrations. This establishes a clear correlation between the rise in their concentrations and the incidence of COVID-19 cases. A general downward trend after 2021 was attributed to the new restrictions posed in Greece during this year, regarding the liberal prescription of antibiotics. Seasonal variation revealed a minute augmentation of antibiotics' use during the months that infections are increased. Additionally, the study highlights the ecological risks associated with elevated antibiotic presence and emphasizes the need for continued monitoring and regulatory measures to mitigate potential ecological repercussions. These findings contribute to our understanding of the complex interplay between antibiotic consumption, environmental presence, and the COVID-19 pandemic's impact on antibiotic pollution in WWTPs.


Assuntos
COVID-19 , Poluentes Químicos da Água , Humanos , Águas Residuárias , Antibacterianos/análise , Pandemias , Eliminação de Resíduos Líquidos , Grécia/epidemiologia , Monitoramento Ambiental , Poluentes Químicos da Água/análise , COVID-19/epidemiologia
2.
Environ Sci Technol ; 57(40): 14827-14838, 2023 Oct 10.
Artigo em Inglês | MEDLINE | ID: mdl-37746919

RESUMO

Non-targeted analysis (NTA) has made critical contributions in the fields of environmental chemistry and environmental health. One critical bottleneck is the lack of available analytical standards for most chemicals in the environment. Our study aims to explore a novel approach that integrates measurements of equilibrium partition ratios between organic solvents and water (KSW) to predictions of molecular structures. These properties can be used as a fingerprint, which with the help of a machine learning algorithm can be converted into a series of functional groups (RDKit fragments), which can be used to search chemical databases. We conducted partitioning experiments using a chemical mixture containing 185 chemicals in 10 different organic solvents and water. Both a liquid chromatography quadrupole time-of-flight mass spectrometer (LC-QTOF MS) and a LC-Orbitrap MS were used to assess the feasibility of the experimental method and the accuracy of the algorithm at predicting the correct functional groups. The two methods showed differences in log KSW with the QTOF method showing a mean absolute error (MAE) of 0.22 and the Orbitrap method 0.33. The differences also culminated into errors in the predictions of RDKit fragments with the MAE for the QTOF method being 0.23 and for the Orbitrap method being 0.31. Our approach presents a new angle in structure elucidation for NTA and showed promise in assisting with compound identification.


Assuntos
Água , Espectrometria de Massas/métodos , Cromatografia Líquida/métodos , Solventes
3.
Sci Total Environ ; 904: 166599, 2023 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-37640083

RESUMO

In recent years, transformation products-(TPs) of pharmaceuticals in the environment have received considerable attention. In this context, here, a customized overview of transformation of Furosemide-(FRS) in aqueous matrices treated by photo-oxidation is provided as a proof of concept. Hence, the primary goal of the study was to display an integrated strategy by combining the target (parent-molecule) and suspect screening-(SS) approaches (TPs) in order to build an in-house High-Resolution mass spectrometry (HRMS) database able to provide reference information (chromatographic/spectral) for environmental investigations in complex matrices (wastewaters/landfill leachates). Data analysis was performed by optimizing a SS workflow. Additional confirmation for the proposed structural elucidation was provided by correlating retention time to the proposed structure employing three prediction models. This approach was applied for the tentative identification of 35 TPs of FRS, 28 of which are reported herein for the first time. Finally, SS and non-target analysis (NTA) have been successfully applied for retrospective screening of FRS and its TPs in real samples. The findings demonstrated that SS allows the proper identification of TPs of FRS in complex matrices proving its outstanding importance compared to NTA. In total, six TPs were identified by SS with potential ecotoxicological implications for two of them according to in silico risk assessment.


Assuntos
Poluentes Químicos da Água , Cromatografia Líquida , Poluentes Químicos da Água/análise , Águas Residuárias , Furosemida , Estudos Retrospectivos , Fluxo de Trabalho
5.
J Hazard Mater ; 454: 131478, 2023 07 15.
Artigo em Inglês | MEDLINE | ID: mdl-37116332

RESUMO

Bisphenols are widely recognised as toxic compounds that potentially threaten the environment and public health. Here we report the use of cold atmospheric pressure plasma (CAP) to remove bisphenol A (BPA) and bisphenol S (BPS) from aqueous systems. Additionally, methanol was added as a radical scavenger to simulate environmental conditions. After 480 s of plasma treatment, 15-25 % of BPA remained, compared to > 80 % of BPS, with BPA being removed faster (-kt = 3.4 ms-1, half-life = 210 s) than BPS (-kt = 0.15 ms-1, half-life 4700 s). The characterisation of plasma species showed that adding a radical scavenger affects the formation of reactive oxygen and nitrogen species, resulting in a lower amount of ˙OH, H2O2, and NO2- but a similar amount of NO3-. In addition, a non-target approach enabled the elucidation of 11 BPA and five BPS transformation products. From this data, transformation pathways were proposed for both compounds, indicating nitrification with further cleavage, demethylation, and carboxylation, and the coupling of smaller bisphenol intermediates. The toxicological characterisation of the in vitro HepG2 cell model has shown that the mixture of transformation products formed during CAP is less toxic than BPA and BPS, indicating that CAP is effective in safely degrading bisphenols.


Assuntos
Compostos Benzidrílicos , Peróxido de Hidrogênio , Compostos Benzidrílicos/toxicidade , Compostos Benzidrílicos/metabolismo , Fenóis/toxicidade , Fenóis/metabolismo
6.
Environ Res ; 227: 115790, 2023 06 15.
Artigo em Inglês | MEDLINE | ID: mdl-37003551

RESUMO

This study investigated the bio-degradation kinetics of tetramethyl bisphenol F (TMBPF), a non-estrogenic alternative to bisphenol A (BPA). Batch biotransformation experiments were performed whereby samples were inoculated with activated sludge and analysed using liquid chromatography-Orbitrap-tandem mass spectrometry (LC-Orbitrap-MS) utilising two non-targeted workflows (commercial and freely available online) for biotransformation products (BTP) identification. The degradation of TMBPF followed single first-order reaction kinetics and depended on the initial concentration (ci) with faster degradation -kt = 0.16, (half-life = 4.4 days) at lower concentrations ci = 0.1 mg L-1, compared with -kt = 0.02 (half-live = 36.4 days) at ci = 10.0 mg L-1. After 18 days, only 8% of the original TMBPF remained at the lowest tested concentration (0.1 mg L-1). Twelve BTPs were identified, three of which were workflow and one condition-specific. The highest relative quantities of BTPs were observed in nutrient-mineral and mineral media after ten days, while after 14 days, 36 and 31% of TMBPF (ci = 1 mg L-1) remained in the nutrient-mineral and mineral media, respectively. Also, the kinetics of TMBPF and its BTPs were the same with and without an additional carbon source. A newly proposed biodegradation pathway for TMBPF involves cleavage of the methylene bridge, hydroxylation with further oxidation, sulphation, nitrification, nitro reduction with further oxidation, acetylation, and glycine conjugation, providing a deeper insight into the fate of TMBPF during biological wastewater treatment.


Assuntos
Esgotos , Águas Residuárias , Biotransformação , Biodegradação Ambiental , Cinética
7.
Molecules ; 28(4)2023 Feb 16.
Artigo em Inglês | MEDLINE | ID: mdl-36838865

RESUMO

This study explores the photocatalytic transformation of the antiviral drug abacavir employing different advanced oxidation processes (AOPs) such as UV/TiO2, UV/MOF/H2O2, UV/MOF/S2O82-, UV/Fe2+/H2O2, and UV/Fe2+/S2O82-. All processes appear to be effective in eliminating abacavir within a few minutes, while the evolution profile of the basic transformation product, descyclopropyl-abacavir (TP-247) was also monitored. Moreover, the implementation of the most efficient technologies towards the removal of abacavir in different matrices such as wastewater effluent and leachate was also assessed, revealing that the organic matter present or the inorganic constituents can retard the whole process. Four major transformation products were detected, and their time-evolution profiles were recorded in all studied matrices, revealing that different transformation pathways dominate in each matrix. Finally, the prediction of the toxicity of the major TPs employing ECOSAR software was conducted and showed that only hydroxylation can play a detoxification role in the treated solution.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Peróxido de Hidrogênio , Oxirredução , Águas Residuárias , Raios Ultravioleta
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