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Enhanced catalytic ozonation using MIL-53(Fe) MOF and CS@MIL-53(Fe) composite beads: A comparative evaluation for organic contaminant removal

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Autor(es):
Camparotto, Natalia Gabriele ; Malvestiti, Jacqueline A. ; de Sousa, Iure Bernardino ; Fokoue, Harold H. ; Dantas, Renato Falcao ; Vieira, Melissa Gurgel Adeodato ; Prediger, Patricia
Número total de Autores: 7
Tipo de documento: Artigo Científico
Fonte: JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING; v. 13, n. 6, p. 18-pg., 2025-12-25.
Resumo

The limited efficiency of single ozonation in the degradation of organic pollutants highlights the necessity for catalysts capable of enhancing this process. In this study, the metal-organic framework (MOF) MIL-53(Fe) was synthesized and immobilized in chitosan beads (CS@MIL-53(Fe)), to promote catalytic ozonation of water contaminants. The immobilization of MOF addresses the practical challenge of catalyst separation, enabling recovery and reuse. The MIL-53(Fe) was homogenously encapsulated into the beads, which exhibited a spherical morphology, a rough surface, and interconnected pores. These characteristics enhance stability, mass transport, and accessibility to active sites. Thermogravimetric analysis revealed that the presence of chitosan provides a protective barrier, enhancing thermal resistance of the CS@MIL-53(Fe). Ozonation tests demonstrated that MIL53(Fe) achieved high degradation efficiencies: 96 % for basic orange 2, 78 % for rhodamine B, 63 % for basic yellow 2, 88 % for naproxen, 47 % for ibuprofen, and 32 % for ketoprofen, substantially surpassing non-catalytic ozonation. Notably, Basic Orange 2 maintained 97 % removal after encapsulation, confirming that immobilization preserved catalytic activity. center dot OH and center dot O2- were identified as the potential main reactive oxygen species. A CCD model identified the optimal operating conditions: pH 8.3, catalyst concentration of 50 mg.L- 1, and ozone concentration of 5.7 mg.L- 1, maximizing degradation efficiency. A DFT study elucidated the molecular-level reactivity of the contaminants toward ozone, corroborating the experimental results. This is the first time that MIL-53(Fe) has been immobilized on a solid support for ozonation. The results suggest that CS@MIL-53(Fe) beads hold considerable promise as a viable and practical alternative for environmental applications in advanced oxidation processes. (AU)

Processo FAPESP: 22/14834-0 - Síntese de novos nanoadsorventes através de protocolos verdes e suas aplicações na remoção de poluentes em águas
Beneficiário:Patricia Prediger
Modalidade de apoio: Auxílio à Pesquisa - Regular
Processo FAPESP: 23/09491-9 - Desenvolvimento de adsorventes avançados à base de nanomateriais de carbono para aplicação na remediação de poluentes presentes em "água produzida" por adsorção e processos oxidativos avançados
Beneficiário:Melissa Gurgel Adeodato Vieira
Modalidade de apoio: Auxílio à Pesquisa - Regular
Processo FAPESP: 24/23386-6 - Avaliação da Eficiência de Nanobolhas de Ozônio no Tratamento de Efluentes
Beneficiário:Renato Falcão Dantas
Modalidade de apoio: Auxílio à Pesquisa - Regular
Processo FAPESP: 23/02041-8 - Preparação de membranas poliméricas a base de MOF contendo nióbio por rotofiação e sua aplicação na remoção de contaminantes em água
Beneficiário:Natália Gabriele Camparotto
Modalidade de apoio: Bolsas no Brasil - Doutorado