Feasibility of micropollutants removal by solar-activated persulfate: Reactive oxygen species formation and influence...

As a natural source of visible light and a type of renewable energy, solar energy is extensively used in the field of photochemistry. In this study, solar was employed to activate persulfate (PS) to degrade typical micropollutants. The removal kinetics of aspirin (ASA) and flunixin meglumine (FMME) in the solar/PS system were well fitted by pseudo-first-order models (R² > 0.99). In the system containing 1.0 mM PS activated by solar irradiation at a fluence of 1.14 × 10^-4 E·m^-2·s^-1, 72.6% and 97.5% of ASA and FMME were degraded, and the corresponding kinetic constants were 6.8-9.8 × 10^-2 and 1.6-9.8 × 10^-1 min^-1, respectively. Qualitative and quantitative analyses of the reactive oxygen species (ROS) indicated that sulfate radical (SO₄^·-) played a major role in degradation, with the maximum contributions of 77.7% and 88.8% for the degradation of ASA and FMME, whereas the maximum contributions of hydroxyl radical (·OH) were only 11.6% and 6.5%, respectively. The contributions of singlet oxygen (¹O₂) were less than 15% at pH 5.5, but increased to 25.6% and 45.5% at pH 8.5, respectively. Solar/PS pre-oxidation increased disinfection byproducts (DBPs) (95.8% for trihalomethanes (THMs) and 47.9% for haloacetic acids (HAAs) at pH 7.0) after chlorination in deionized water, and an opposite trend was found in systems coexisting with natural organic matter (NOM). Residual PS after oxidation resulted in a high aquatic toxicity, with an inhibition rate of 18.70% to algae growth. Economic analysis showed that the electrical energy per order values of the system ranged from 23.5 to 86.5 kWh·m^-3·order^-1, indicating that the solar/PS system shows promise for practical applications.