Application of a fluidized three-dimensional electrochemical reactor with Ti/SnO2–Sb/β-PbO2 anode and granular activated carbon particles for degradation and mineralization of 2,4-dichlorophenol: Process optimization and degradation pathway

Abstract

A three-dimensional electrochemical reactor with Ti/SnO2–Sb/β-PbO2 anode and granular activated carbon (3DER-GAC) particle electrodes were used for degradation of 2,4-dichlorophenol (2,4-DCP). Process modeling and optimization were performed using an orthogonal central composite design (OCCD) and genetic algorithm (GA), respectively. Ti/SnO2–Sb/β-PbO2 anode was prepared by electrochemical deposition method and then its properties were studied by FESEM, EDX, XRD, Linear sweep voltammetry and accelerated lifetime test techniques. The results showed that lead oxide was precipitated as highly compact pyramidal clusters in the form of β-PbO2 on the electrode surface. In addition, the prepared anode had high stability (170 h) and oxygen evolution potential (2.32 V). A robust quadratic model (p-value < 0.0001 and R2 > 0.99) was developed to predict the 2,4-DCP removal efficiency in the 3DER-GAC system. Under optimal conditions (pH = 4.98, Na2SO4 concentration = 0.07 M, current density = 35 mA cm−2, GAC amount = 25 g and reaction time = 50 min), the removal efficiency of 2,4-DCP in the 3DER-GAC system and the separate electrochemical degradation process (without GAC particle electrode) were 99.8 and 71%, respectively. At a reaction time of 80 min, the TOC removal efficiencies in the 3DER-GAC and the separate electrochemical degradation system were 100 and 57.5%, respectively. Accordingly, the energy consumed in these two systems was calculated to be 0.81 and 1.57 kWh g−1 TOC, respectively. Based on the results of LC-MS analysis, possible degradation pathways of 2,4-DCP were proposed. Trimerization and ring opening reactions were the two dominant mechanisms in 2,4-DCP degradation.