Photo-electro-Fenton process applied to the degradation of valsartan: Effect of parameters, identification of degradation routes and mineralization in combination with a biological system

Abstract

In this work, the oxidation of the antihypertensive drug valsartan by the Electro-Fenton (EF) and photo-electro-Fenton (PEF) processes was studied using a Ti/IrO2 doped with SnO2 as anode, and a carbon felt air diffusion electrode as cathode. Initially, the influence of variables such as supporting electrolyte type, current density, and pH on EF and/or PEF processes was evaluated. The processes were carried out in batch mode, in an open and undivided cell of 200 cm3. The efficiency of the systems was evaluated in terms of the removal of the initial contaminant and rate of mineralization. When NaCl was used as a supporting electrolyte at pH 3.0 and current density 3.46 mA/cm2 adding 3.6 × 10−5 mol/L of Fe2+, total valsartan (20 mg/L) degradation was observed after 45 min. After 120 min, even if total removal of valsartan was reached, only 25% of mineralization was obtained. Thus, valsartan degradation tests at near neutral pH in presence of oxalic acid (4.6 × 10−5 mol/L) lead to comparable results with those obtained at pH 3.0. Primary aromatic intermediates were identified by high resolution mass spectrometry (HRMS) using hybrid quadrupole- time-of-flight (QTOF) MS, from which an initial degradation pathway was proposed. At the end of the PEF system, several aliphatic acids were accumulated and observed, which were effectively removed in a subsequent aerobic biological system. The results demonstrate the feasibility of PEF and biological coupling process to completely mineralize emerging pharmaceutical pollutants, such as valsartan, at natural pH.