| The three-dimensional electrochemical oxidation method is a new advanced oxidation technology developed by adding particle electrodes in the traditional two-dimensional electrolysis system.The existence of particle electrodes in the three-dimensional electrolysis system has attracted widespread attention for several potential advantages,such as improving the low current efficiency and poor mass transfer effect of the traditional two-dimensional electrolysis system.To overcome the limitation of the pure carbonaceous materials,potassium ferrate(K2FeO4)was used as an iron-containing catalyst,which is loaded on the surface of activated carbon materials by means of ball mill grinding.It can endow carbon materials with a special graphitized structure and excellent electron transport capabilities after high-temperature calcination.In this paper,the K2FeO4/AC particle electrode was constructed to investigated the effect of Cu-EDTA treatment,and the reaction mechanism was also revealed.Through the selection of activated carbon types,acid treatment and K2FeO4loading methods,the best preparation method of K2FeO4/AC particle electrode was determined.The experimental results showed that the best preparation process of load K2FeO4 on the nutshell activated carbon which has been modified by hydrochloric acid by means of ball milling.The prepared K2FeO4/AC particle electrode had a higher removal rate of Cu(II)and COD than the original nutshell carbon particle electrode which was 12.3%and 14.0%.Compared with the original nutshell activated carbon particle electrode,the graphitization degree of the K2FeO4/AC particle electrode was significantly improved,and a large number of graphene nanosheets were produced on the surface.The operating conditions of the three-dimensional electrolysis system for treating Cu-EDTA containing wastewater were optimized.The experimental results showed that the optimal operating conditions for the three-dimensional electrode system to treat the Cu-EDTA concentration of 50 mg L-1 were:current intensity of 30m A cm-2,solution p H of 5,and Na2SO4 electrolyte concentration of 0.05 mmol L-1.After 180 min treatment,the removal rate of Cu(II)and COD can reach 96.8%and92.5%,respectively.The K2FeO4/AC particle electrode had good stability,and the treatment effect was only reduced by 10%after 5 consecutive operations.The removal rate of Cu(II)and COD of K2FeO4/AC particle electrode could be recovered to 95.3%and 93.7%of the first use after hydrochloric acid regeneration treatment.The reaction process of the three-dimensional electrode system with K2FeO4/AC particle electrode in the treatment of Cu-EDTA containing wastewater,and the effect of the particle electrode were analyzed.The results showed that,the Cu(II)and COD removal of the three-dinemsional electrolysis system was better when compare with the two-dimensional electrode system or a solo adsorption system,and showed a significant synergistic effect on the removal of Cu(II).Under the action of electric current,the K2FeO4/AC particle electrode had both indirect oxidation and direct oxidation,in which promote the production of hydroxyl radicals.The existence of K2FeO4/AC particle electrode also helped to accelerate the electron transfer rate and strengthen the direct oxidation ability. |