Electrocatalytic oxidation (ECO) has attracted attention because of its high efficiency and environmental friendliness in water treatment. The preparation of anodes with high catalytic activity and long service lifetimes is a core part of electrocatalytic oxidation technology. Here, porous Ti/RuO2-IrO2@Pt, Ti/RuO2-TiO2@Pt, and Ti/Y2O3-RuO2-TiO2@Pt anodes were fabricated by means of modified micro-emulsion and vacuum impregnation methods with high porosity titanium plates as substrates. The scanning electron microscopy (SEM) images showed that RuO2-IrO2@Pt, RuO2-TiO2@Pt, and Y2O3-RuO2-TiO2@Pt nanoparticles were coated on the inner surface of the as-prepared anodes to form the active layer. Electrochemical analysis revealed that the high porosity substrate could result in a large electrochemically active area, and a long service life (60 h at 2 A cm−2current density, 1 mol L−1H2SO4as the electrolyte, and 40 °C). The degradation experiments conducted on tetracycline hydrochloride (TC) showed that the porous Ti/Y2O3-RuO2-TiO2@Pt had the highest degradation efficiency for tetracycline, reaching 100% removal in 10 min with the lowest energy consumption of 167 kWh kg−1TOC. The reaction was consistent with the pseudo-primary kinetics results with a k value of 0.5480 mol L−1s−1, which was 16 times higher than that of the commercial Ti/RuO2-IrO2electrode. The fluorospectrophotometry studies verified that the degradation and mineralization of tetracycline were mainly ascribed to the •OH generated in the electrocatalytic oxidation process. This study thus presents a series of alternative anodes for future industrial wastewater treatment.
In this study, the performance of a zero-gap flow-through reactor with three-dimensional (3D) porous Ti/RuO2-TiO2@Pt anodes was systematically investigated for the electrocatalytic oxidation of phenolic wastewater, considering phenol and 4-nitrophenol (4-NP) as the target pollutants. The optimum parameters for the electrochemical oxidation of phenol and 4-NP were examined. For phenol degradation, at an initial concentration of 50 mg/L, initial pH of 7, NaCl concentration of 10.0 g/L, current density of 10 mA/cm2, and retention time of 30 min, the degradation efficiency achieved was 95.05%, with an energy consumption of 15.39 kWh/kg; meanwhile, for 4-NP, the degradation efficiency was 98.42% and energy consumption was 19.21 kWh/kg (at an initial concentration of 40 mg/L, initial pH of 3, NaCl concentration of 10.0 g/L, current density of 10 mA/cm2, and retention time of 30 min). The electrocatalytic oxidation of phenol and 4-NP conformed to the pseudo-first-order kinetics model, and thekvalues were 0.2562 min−1and 0.1736 min−1, respectively, which are 1.7 and 3.6-times higher than those of a conventional electrolyzer. Liquid chromatography–mass spectrometry (LC–MS) was used to verify the intermediates formed during the degradation of phenol or 4-NP and a possible degradation pathway was provided. The extremely narrow electrode distance and the flow-through configuration of the zero-gap flow-through reactor were thought to be essential for its lower energy consumption and higher mass transfer efficiency. The zero-gap flow-through reactor with a novel 3D porous Ti/RuO2-TiO2@Pt electrode is a superior alternative for the treatment of industrial wastewater.
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