Mechanistic modelling of Fe3+-EDDS mediated photo-fenton revisited: lumped radicals and sensitivity analysis
This study proposes a new kinetic model of the Fe3+-EDDS mediated photo-Fenton process at circumneutral pH when applied to microcontaminants (MCs) removal. The model is also able to work in the absence of H2O2, when EDDS•3- radicals generated from the lysis of the Fe3+-EDDS complex are responsible f...
| Autores: | , , , , |
|---|---|
| Tipo de recurso: | artículo |
| Fecha de publicación: | 2023 |
| País: | España |
| Institución: | Universitat Politècnica de Catalunya (UPC) |
| Repositorio: | UPCommons. Portal del coneixement obert de la UPC |
| Idioma: | inglés |
| OAI Identifier: | oai:upcommons.upc.edu:2117/422117 |
| Acceso en línea: | https://hdl.handle.net/2117/422117 https://dx.doi.org/10.1016/j.cej.2023.142559 |
| Access Level: | acceso abierto |
| Palabra clave: | Photo-Fenton Photo-catalytic reaction Kinetic model Microcontaminants Fe3+-EDDS Lumped radicals |
| Sumario: | This study proposes a new kinetic model of the Fe3+-EDDS mediated photo-Fenton process at circumneutral pH when applied to microcontaminants (MCs) removal. The model is also able to work in the absence of H2O2, when EDDS•3- radicals generated from the lysis of the Fe3+-EDDS complex are responsible for MCs degradation, representing a new advance in this research field. A novel semi-empirical approach based on lumping radical species is adopted. This is done by including a factor in the model to describe the lower oxidation capacity of EDDS•3- radicals in front of hydroxyl radicals. Model calibration demonstrated the effectiveness of the semi-empirical strategy to successfully predict the system behaviour in terms of sulfamethoxazole (SMX, model MC), Fe3+-EDDS and H2O2 (when needed) concentration evolution during the process. Then, a global sensitivity analysis (GSA) was carried out to reduce the computation cost of the model, indicating that once the initial Fe3+-EDDS complex is oxidized to Fe3+-EDDSox, its photo-activation to (Fe3+-EDDSox)* is not actually reversible despite possible. Finally, the model was validated, showing that experimental data could be predicted properly, with NRMSE (Normalized Root Mean Square Errors) < 0.08 for SMX and < 0.15 for Fe3+-EDDS (normalized data). The oxidation capacity of the EDDS•3- radicals was estimated to be approximately 11% that of the hydroxyl radicals. |
|---|