A1 Vertaisarvioitu alkuperäisartikkeli tieteellisessä lehdessä
Catalytic ozonation of multi-component pharmaceutical mixtures: Kinetic evaluation, molecular interaction, including catalyst structure effects
Tekijät: Tolvanen Pasi; Núñez Núñez Ana Fernanda; Duverger Estéban; Saarinen Nikke; Shahid Abdul; Fale Shey Jude; Saeid Soudabeh; Kråkström Matilda; Kumar Narendra; Eränen Kari; Eklund Patrik C.; Mikkola Jyri-Pekka; Murzin Dmitry Yu.; Salmi Tapio
Kustantaja: Elsevier BV
Julkaisuvuosi: 2026
Lehti: Applied Catalysis B: Environmental
Artikkelin numero: 126274
Vuosikerta: 385
ISSN: 0926-3373
eISSN: 1873-3883
DOI: https://doi.org/10.1016/j.apcatb.2025.126274
Julkaisun avoimuus kirjaamishetkellä: Avoimesti saatavilla
Julkaisukanavan avoimuus : Osittain avoin julkaisukanava
Verkko-osoite: https://doi.org/10.1016/j.apcatb.2025.126274
Rinnakkaistallenteen osoite: https://research.utu.fi/converis/portal/detail/Publication/506328454
Rinnakkaistallenteen lisenssi: CC BY
Rinnakkaistallennetun julkaisun versio: Kustantajan versio
Removal of pharmaceuticals from wastewater remains a major environmental challenge, requiring efficient and selective Advanced Oxidation Processes (AOPs). Catalytic and non-catalytic ozonation was investigated in a laboratory-scale reactor under optimized flow conditions (500–750 mL min⁻¹, 98 % O₂ feed). Ozonation kinetics of active pharmaceutical ingredient mixtures (APIs) consisting of ibuprofen (IBU), diclofenac (DCF), carbamazepine (CBZ), sulfadiazine (SDZ), and sulfamethoxazole (SFX) (40 mg L⁻¹ each) — was investigated using iron-modified zeolite catalysts, Fe-H-Y and Fe-H-Beta, under semi-batch operations (0.5 g catalyst, 20 °C) in order to correlate degradation and mineralization efficiency with catalyst structure, acidity, and stability. Both catalysts significantly improved the ozone utilization compared to non-catalytic ozonation. Interestingly, Fe-H-Y accelerated initial degradation rate, while the use of Fe-H-Beta resulted in the highest level of mineralization. Adsorption–desorption analysis revealed that the molecular size and polarity controlled the interactions between the pharmaceutical and the catalyst: smaller polar compounds (SDZ, SFX) exhibited stronger adsorption on the catalyst, while bulkier molecules (DCF, IBU) were restricted to external surfaces. Post-reaction characterization confirmed that the Fe-H-Y retained more surface area and exhibited lower Fe leaching, while Fe-H-Beta showed significantly higher carbon deposition. Overall, Fe-H-Y combined rapid kinetics and structural stability, while Fe-H-Beta provided higher mineralization, at the expense of more extensive fouling. The study demonstrated that optimized ozonation conditions, coupled with tailored zeolite catalysts, markedly improve the oxidation efficiency and long-term performance in the oxidation of pharmaceuticals.
Ladattava julkaisu This is an electronic reprint of the original article. |  |
Julkaisussa olevat rahoitustiedot:
Pasi Tolvanen gratefully acknowledges financial support from Liedon Säästöpankkisäätiö (personal research grant, 2024–2025, ref. 20240388) and from Svenska litteratursällskapet i Finland (SLS) (personal research grant, 2025–2026; supported by Ingrid, Margit och Henrik Höijers donationsfond II), whose contributions made this research possible. Pasi Tolvanen also thank Maa- ja vesitekniikan tuki Foundation for providing a travel grant that enabled participation in the International Conference on Environmental Catalysis (ICEC 2025), where part of this work was presented. Collaboration with the Erasmus Mundus Joint Master Programme IMATEC (International Master in Technology and Management for Circular Economy) is appreciated for hosting the MSc thesis project of Ms Ana Fernanda Nuñez Nuñez and for providing financial support for analytical expenses through the student’s scholarship. The participation of Estéban Duverger was made possible through the Erasmus+ internship exchange programme, which supported his three-month research placement during the summer 2025 (also supported by the French government program France2030 – EUR INTREE, reference ANR-18-EURE-0010). In Sweden the Bio4Energy program is acknowledged. The authors also thank the SpinChem AB for providing the SpinChem® equipment.
