Carbon felt modified with N-doped rGO for an efficient electro-peroxone process in diuron degradation and biodegradability improvement of wastewater from a pesticide manufacture: Optimization of process parameters, electrical energy consumption and degradation pathway

摘要

In this study, diuron abatement in aqueous medium and the remediation of wastewater from a pesticide manufacture were studied by the E-peroxone process, using carbon felt modified with N-doped rGO (N-rGO/CF) as cathode and Ti/PbO2 anode. Compared with the unmodified CF, the N-rGO/CF displayed a higher response current, improved oxygen reduction activity, and larger BET specific surface area. Also, the modified CF provided a higher H2O2 production rate. The influence of several effective parameters on the diuron degradation rate in aqueous medium by the E-peroxone process was systematically explored by central composite design-response surface methodology; the approach suggested the optimal operating condition at pH of 9, applied current of 500 mA, Na2SO4 of 0.05 M, ozone flow of 1 L min(-1), and operating time of 15 min to attain the maximum removal of diuron. At the optimal condition, N-rGO/CF cathode increased diuron degradation rate and decreased electrical energy consumption rather than CF cathode, in the E-peroxone system. Radical quenching experiment and degradation pathway of diuron revealed that hydroxyl radicals were the dominant reactive oxidants. A possible degradation mechanism was proposed based on hydroxylated and demethylated products identified during diuron degradation. No significant difference of the electro-generated H2O2 after 10 successive recycles confirms the admirable reusability of N-rGO/CF. The application of the process for pesticide wastewater increased BOD5/COD ratio significantly from 0.041 (for non-treated wastewater) to 0.4 during 90 min treatment, showing a substantial improvement of the biodegradability of the wastewater. Accordingly, the E-peroxone system can be utilized as a promising pretreatment step before a biological process to facilitate and shorten the length of the biological treatment. The findings of this study could offer valuable information for practical applications of the E-peroxone system in the treatment of pesticide-manufacturing wastewater.