pH-Dependent Ozonation of Diclofenac: Molecular Insights and Implications for Water Quality and Nature-Based Water Reuse Systems

Diclofenac (DCF), a widely consumed non-steroidal anti-inflammatory drug, presents significant environmental challenges due to its persistence and toxicity in aquatic ecosystems. This study investigates the pH-dependent ozonation of DCF in aqueous media, focusing on degradation kinetics, transformat...

Full description

Saved in:
Bibliographic Details
Main Authors: Natalia Villota, Unai Duoandicoechea, Enzo Valentin Tosi-Zarate
Format: Article
Language:English
Published: MDPI AG 2025-06-01
Series:Clean Technologies
Subjects:
Online Access:https://www.mdpi.com/2571-8797/7/2/47
Tags: Add Tag
No Tags, Be the first to tag this record!
_version_ 1849435223229464576
author Natalia Villota
Unai Duoandicoechea
Enzo Valentin Tosi-Zarate
author_facet Natalia Villota
Unai Duoandicoechea
Enzo Valentin Tosi-Zarate
author_sort Natalia Villota
collection DOAJ
description Diclofenac (DCF), a widely consumed non-steroidal anti-inflammatory drug, presents significant environmental challenges due to its persistence and toxicity in aquatic ecosystems. This study investigates the pH-dependent ozonation of DCF in aqueous media, focusing on degradation kinetics, transformation pathways, and effects on key water quality indicators. Ozonation experiments were conducted across a broad pH range (2.0–13.0), using a multi-scale analytical approach combining UV/Vis spectroscopy, colorimetry, turbidity, and aromaticity measurements. The results show that pH strongly influences DCF degradation efficiency: acidic conditions favor selective reactions with molecular ozone, while an alkaline pH enhances non-selective oxidation via hydroxyl radicals. Spectroscopic analyses revealed the progressive breakdown of aromatic structures, the transient formation of quinonoid and phenolic intermediates, and eventual mineralization to inorganic by-products such as nitrate. Low-pH conditions also induced turbidity due to precipitation of neutral DCF species. These findings underline the importance of pH control in optimizing ozonation performance and minimizing toxic by-products. Furthermore, this study proposes ozonation as a viable pre-treatment step within Nature-Based Solutions (NBSs), potentially improving the performance of downstream biological systems such as constructed wetlands. The results contribute to the development of integrated and sustainable water treatment strategies for pharmaceutical contaminant removal and water reuse.
format Article
id doaj-art-e9f882ad38c9485c943200032cb6d83a
institution Kabale University
issn 2571-8797
language English
publishDate 2025-06-01
publisher MDPI AG
record_format Article
series Clean Technologies
spelling doaj-art-e9f882ad38c9485c943200032cb6d83a2025-08-20T03:26:21ZengMDPI AGClean Technologies2571-87972025-06-01724710.3390/cleantechnol7020047pH-Dependent Ozonation of Diclofenac: Molecular Insights and Implications for Water Quality and Nature-Based Water Reuse SystemsNatalia Villota0Unai Duoandicoechea1Enzo Valentin Tosi-Zarate2Department of Environmental and Chemical Engineering, Faculty of Engineering Vitoria-Gasteiz, University of the Basque Country UPV/EHU, Nieves Cano 12, 01006 Vitoria-Gasteiz, SpainDepartment of Environmental and Chemical Engineering, Faculty of Engineering Vitoria-Gasteiz, University of the Basque Country UPV/EHU, Nieves Cano 12, 01006 Vitoria-Gasteiz, SpainDepartment of Environmental and Chemical Engineering, Faculty of Engineering Vitoria-Gasteiz, University of the Basque Country UPV/EHU, Nieves Cano 12, 01006 Vitoria-Gasteiz, SpainDiclofenac (DCF), a widely consumed non-steroidal anti-inflammatory drug, presents significant environmental challenges due to its persistence and toxicity in aquatic ecosystems. This study investigates the pH-dependent ozonation of DCF in aqueous media, focusing on degradation kinetics, transformation pathways, and effects on key water quality indicators. Ozonation experiments were conducted across a broad pH range (2.0–13.0), using a multi-scale analytical approach combining UV/Vis spectroscopy, colorimetry, turbidity, and aromaticity measurements. The results show that pH strongly influences DCF degradation efficiency: acidic conditions favor selective reactions with molecular ozone, while an alkaline pH enhances non-selective oxidation via hydroxyl radicals. Spectroscopic analyses revealed the progressive breakdown of aromatic structures, the transient formation of quinonoid and phenolic intermediates, and eventual mineralization to inorganic by-products such as nitrate. Low-pH conditions also induced turbidity due to precipitation of neutral DCF species. These findings underline the importance of pH control in optimizing ozonation performance and minimizing toxic by-products. Furthermore, this study proposes ozonation as a viable pre-treatment step within Nature-Based Solutions (NBSs), potentially improving the performance of downstream biological systems such as constructed wetlands. The results contribute to the development of integrated and sustainable water treatment strategies for pharmaceutical contaminant removal and water reuse.https://www.mdpi.com/2571-8797/7/2/47ozonationdiclofenac degradationadvanced oxidation processespH-dependent transformationpharmaceutical pollutantswater quality
spellingShingle Natalia Villota
Unai Duoandicoechea
Enzo Valentin Tosi-Zarate
pH-Dependent Ozonation of Diclofenac: Molecular Insights and Implications for Water Quality and Nature-Based Water Reuse Systems
Clean Technologies
ozonation
diclofenac degradation
advanced oxidation processes
pH-dependent transformation
pharmaceutical pollutants
water quality
title pH-Dependent Ozonation of Diclofenac: Molecular Insights and Implications for Water Quality and Nature-Based Water Reuse Systems
title_full pH-Dependent Ozonation of Diclofenac: Molecular Insights and Implications for Water Quality and Nature-Based Water Reuse Systems
title_fullStr pH-Dependent Ozonation of Diclofenac: Molecular Insights and Implications for Water Quality and Nature-Based Water Reuse Systems
title_full_unstemmed pH-Dependent Ozonation of Diclofenac: Molecular Insights and Implications for Water Quality and Nature-Based Water Reuse Systems
title_short pH-Dependent Ozonation of Diclofenac: Molecular Insights and Implications for Water Quality and Nature-Based Water Reuse Systems
title_sort ph dependent ozonation of diclofenac molecular insights and implications for water quality and nature based water reuse systems
topic ozonation
diclofenac degradation
advanced oxidation processes
pH-dependent transformation
pharmaceutical pollutants
water quality
url https://www.mdpi.com/2571-8797/7/2/47
work_keys_str_mv AT nataliavillota phdependentozonationofdiclofenacmolecularinsightsandimplicationsforwaterqualityandnaturebasedwaterreusesystems
AT unaiduoandicoechea phdependentozonationofdiclofenacmolecularinsightsandimplicationsforwaterqualityandnaturebasedwaterreusesystems
AT enzovalentintosizarate phdependentozonationofdiclofenacmolecularinsightsandimplicationsforwaterqualityandnaturebasedwaterreusesystems