PMS coupled Mn(II) mediated electrochemistry processes (E-Mn(II)-PMS) on the efficient RB19 wastewater treatment: Focus on the regulation and reinforcement of Mn(III)/Mn(II)

Abstract

Dye wastewater, represented by reactive blue 19 (RB19), severely threatens the aquatic ecological environment and human health, such that an efficient RB19 wastewater treatment technology should be urgently developed. Based on manganese ion-mediated electrochemistry, PMS was introduced to develop a novel electrocatalytic system (E-Mn(II)-PMS) that can efficiently remove and degrade RB19. The synergistic effect between E, Mn(II), and PMS was verified in this study through comparative experiments of a wide variety of systems. The removal efficiency of RB19 reached 95.1% in 50 min under reasonable power consumption (3.29 kWh/m3). Moreover, the effects exerted by different operating conditions (e.g., initial pH, current density, RB19 concentration, Mn(II) concentration, as well as PMS concentration) and water matrix on the degradation efficiency of RB19 were explored through single factor experiments. The active oxidation species (ROS) and their contribution rate for the degrading and removing RB19 were studied through quenching experiments, EPR experiments, TMT-15 metal capture experiments, as well as PP complexation experiments. The role played by non-free radicals took on critical significance in the oxidation removal of RB19, which comprised direct electro oxidation, Mn(III) oxidation, and 1O2 oxidation. The enhancement effect of free radicals (SO4·− and HO∙) was not sufficiently significant, with a low degree of contribution. The oxidation effect of the anode facilitated the conversion of Mn (II) to Mn (III), which was employed in PMS for expediting the production of 1O2. The reduction effect of the cathode blocked the production of Mn (IV) as a side reaction, such that the continuous circulation of manganese ions between divalent and trivalent was promoted. Meanwhile, the cathode reacted with PMS to generate a small part of SO4·− and HO∙. In addition, the reaction active site of RB19 was predicted, and a possible degradation pathway was proposed in accordance with the mass spectrometry results and the DFT calculation. As revealed by the results of the QSAR analysis and the plant culture experiments, the biological toxicity of RB19 was markedly reduced after the sample was administrated with E-Mn(II)-PMS. E-Mn(II)-PMS-mediated electrochemical technology displays several advantages (e.g., high efficiency, low consumption, recyclability, wide pH window, and strong applicability) while showing promising market development and utilization for treating dye wastewater.