Active-chlorine-mediated oxidation of 5-fluorouracil on a hierarchically ordered macroporous RuO₂ electrode

A hierarchically ordered macroporous RuO₂ electrode (HOM-RuO₂) was fabricated to enhance in situ active chlorine production in an electrochemical system intended for treatment of pharmaceutical active compounds (PhACs). The unique structure of HOM-RuO₂ resulted in a decrease of the chlorine evolution potential, a large electro-active area available for in situ conversion of Cl^- to active chlorine, and hence improved the active chlorine production by 40%. 5-Fluorouracil (5-FU) was used as a target pollutant to explore the performance of the HOM-RuO₂ for PhACs degradation based on the in situ generated active chlorine. The results showed that the reaction rate of active-chlorine-mediated oxidation of 5-FU produced using the HOM-RuO₂ was 18.4 times higher than that in the case of hydroxyl radicals (OH)-initiated oxidation using a PbO₂ electrode at 30 mA cm^-2. The effects of current density and initial solution pH on the 5-FU removal were investigated. The mechanism of 5-FU degradation was proposed taking into accounts both active chlorine production, and change of the speciation of 5-FU caused by pH variations. The dominant degradation products observed for the degradation of 5-FU using the HOM-RuO₂ were lactic acid, propanol, acetic acid, urea and other small molecules, but no chlorinated products were detected. These study demonstrates the promise of the HOM-RuO₂-based electrochemical systems for the active-chlorine-mediated treatment of recalcitrant pharmaceuticals found in wastewater.