Photo-Fenton oxidation of 3-amino-5-methylisoxazole: a by-product from biological breakdown of some pharmaceutical compounds

Abstract

The present study aims to assess the removal of 3-amino- 5-methylisoxazole (AMI), a recalcitrant by-product resulting from the biological breakdown of some pharmaceuticals, applying a solar photo-Fenton process assisted by ferrioxalate complexes (SPFF) (Fe3+/H2O2/oxalic acid/UVA-Vis) and classical solar photo-Fenton process (SPF) (Fe2+/ H2O2/UVA-Vis). The oxidation ability of SPFF was evaluated at different iron/oxalate molar ratios (1:3, 1:6, and 1:9, with [total iron]= 3.58x10(-2) mM and [oxalic acid]= 1.07x10(-1), 2.14x10(-1) and 3.22x10(-1) mM, respectively) and pH values (3.5-6.5), using low iron contents (2.0 mg Fe3+ L-1). Additionally, the use of other organic ligands such as citrate and ethylenediamine-N, N'-disuccinic acid (EDDS) was tested. The oxidation power of the classical SPF was assessed at different pH values (2.8-4.0) using 2.0 mg Fe2+ per liter. Furthermore, the effect of AMI concentration (220 mg L-1), presence of inorganic ions (Cl-, SO42-, NO3-, HCO3-, NH4+), and radical scavengers (sodium azide and D-mannitol) on the SPF method at pH 3.5 was also assessed. Experiments were done using a lab-scale photoreactor with a compound parabolic collector (CPC) under simulated solar radiation. A pilot-scale assay was conducted using the best operation conditions. While at near neutral pH, an iron/oxalate molar ratio of 1:9 led to the removal of 72 % of AMI after 90 min of SPFF, at pH 3.5, an iron/oxalate molar ratio of 1:3 was enough to achieve complete AMI degradation (below the detection limit) after 30 min of reaction. The SPF process at pH 3.5 underwent a slower AMI degradation, reaching total AMI degradation after 40 min of reaction. The scale up of SPF process showed a good reproducibility. Oxalic and oxamic acids were identified as the main low-molecular-weight carboxylic acids detected during the pilot-scale SPF reaction.