Catalytic hydrodehalogenation of iodinated contrast agents in drinking water: A kinetic study

The occurrence of iodinated contrast media (ICM) in water bodies represents a significant threat for public health due to their strong biochemical stability and recalcitrance to conventional water treatment systems. In this work, the feasibility of catalytic hydrodehalogenation (HDH) for the degrada...

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Detalles Bibliográficos
Autores: Benito del Olmo, Raúl, Martín Martín, María, Nieto-Sandoval Rodríguez, Julia, Muñoz García, Macarena, Martínez de Pedro, Zahara, Casas de Pedro, José Antonio
Tipo de recurso: artículo
Fecha de publicación:2024
País:España
Institución:Universidad Autónoma de Madrid
Repositorio:Biblos-e Archivo. Repositorio Institucional de la UAM
Idioma:inglés
OAI Identifier:oai:repositorio.uam.es:10486/715774
Acceso en línea:http://hdl.handle.net/10486/715774
https://dx.doi.org/10.1016/j.jece.2024.114390
Access Level:acceso abierto
Palabra clave:Catalytic Hydrodehalogenation
Iodinated Contrast Media
Drinking Water
Pd/Al2O
Rh/Al2O3
Pt/Al2O3
Química
Descripción
Sumario:The occurrence of iodinated contrast media (ICM) in water bodies represents a significant threat for public health due to their strong biochemical stability and recalcitrance to conventional water treatment systems. In this work, the feasibility of catalytic hydrodehalogenation (HDH) for the degradation of a representative group of ICMs (iohexol (IHX), iopromide (IPR), iopamidol (IPM) and diatrizoic acid (DIA)) is investigated. Complete degradation and deiodination of the isolated ICMs (1.6⋅10 2 mmol L 1) was achieved in less than 30 min in the presence of 0.25 g L 1 of different precious metal catalysts (Pd/Al2O3, Rh/Al2O3 and Pt/Al2O3) under ambient conditions, closing iodine balance by >95 %. Based on the identified reaction intermediates and final products, reaction mechanisms were accordingly proposed. A sequential reaction pathway was proposed for DIA removal, while reaction mechanisms encompassing both sequential and concerted reaction steps were proposed for the non-ionic ICMs (IHX, IPR, and IPM). Subsequent kinetic models, which successfully described experimental data, were developed from the elucidated reaction mechanisms, considering all species involved in the reaction. The versatility of the process was finally demonstrated in the treatment of real aqueous matrices (surface water and tap water) spiked with the ICMs mixture, except in the case of Pt/Al2O3 which suffered deactivation due to surface poisoning by halides. For this catalyst, kinetic constants ranged from 0.31 to 0.22 min 1 in deionized water, and from 0.04 to 0.08 min 1 in surface water as the reaction matrix. Among the tested catalysts, Pd/Al2O3 showed the highest activity and stability for the removal of ICMs