1. Nanjing Institute of Environmental Science, Ministry of Ecology and Environment of the People's Republic of China, Nanjing 210042, China; 2. College of Environmental and Safety Engineering, Changzhou University, Changzhou 213164, China
Abstract：Three-dimensional electrode and electric Fenton system were combined to degrade methyl orange wastewater with the method of electrocatalytic oxidation degradation. Fe3O4 loaded graphene oxide particle electrode GO@Fe3O4 (GF) and spherical gel structure SA/GO@Fe3O4 (SGF) particle electrode were made by our research group. Then, the two kinds of particle electrodes were characterized, the influence factors of electrocatalytic oxidation performance by three-dimensional electrode-electro Fenton (3D-EF) system were discussed and the reaction kinetic analysis was carried out. Based on the design of Box-Benhnken central composite response surface, the response surface quadratic multiple regression equation model was established. The degradation process of methyl orange was studied by UV-vis and GC-MS. There was three-dimensional network fold structure on the surface of SGF particle electrode. Under the reaction conditions, namely initial pH=5, particle electrode dosage 3.0g/L, reaction time 90min, current density 30mA/cm2and applied voltage 7V, the removal efficiencies of methyl orange chromaticity and COD of SGF particle electrode system were 98.8% and 87.5% respectively, which were higher than that of GF particle electrode system, which were 87.2% and 71.2% respectively. Based on the present study, the reaction conditions and the removal efficiency of methyl orange chromaticity predicted by the response surface model were consistent with the experimental results. The speculated degradation process of methyl orange can be divided into three stages:bond breaking oxidation process, ring opening process and complete oxidation process.
Zou H, Wang Y. Azo dyes wastewater treatment and simultaneous electricity generation in a novel process of electrolysis cell combined with microbial fuel cell[J]. Bioresource Technology, 2017,235:167-175.
[2]
Wang Y, Pan Y, Zhu T, et al. Enhanced performance and microbial community analysis of bio-electrochemical system integrated with bio-contact oxidation reactor for treatment of wastewater containing azo dye[J]. Science of the Total Environment, 2018,634:616-627.
[3]
Xu L, Liang G, Yin M. A promising electrode material modified by Nb-doped TiO2 nanotubes for electrochemical degradation of AR 73[J]. Chemosphere, 2017,173:425-434.
[4]
Verma A K, Bhunia P, Dash R R, et al. Sonolytic decolorization of textile wastewater containing a mixture of reactive, acid and disperse dyes[J]. Clean-Soil, Air, Water, 2015,43(5):767-774.
[5]
Carlos A. Martínez-Huitle, Brillas E. Decontamination of wastewaters containing synthetic organic dyes by electrochemical methods:A general review[J]. Applied Catalysis B Environmental, 2009,87(3/4):105-145.
[6]
Tao H, Liu L F, Zhou L L, et al. Electrokinetic removal of chromium from chromite ore-processing residue using graphite particle-supported nanoscale zero-valent iron as the three-dimensional electrode[J]. Chemical Engineering Journal, 2018,350:1022-1034.
[7]
郑帅,范云双,文晨,等.F-SnO2/GAC粒子电极的制备及其电催化性能[J]. 中国环境科学, 2020,40(2):661-669. Zheng S, Fan Y S, Wen C, et al. Preparation of F-SnO2/GAC particle electrode and its electrocatalytic performance[J]. China Environmental Science, 2020,40(2):661-669.
[8]
Mao R, Zhao X, Lan H, et al. Graphene-modified Pd/C cathode and Pd/GAC particles for enhanced electrocatalytic removal of bromate in a continuous three-dimensional electrochemical reactor[J]. Water Research, 2015,77:1-12.
[9]
Shen B, Wen X H, Huang X. Enhanced removal performance of estriol by a three-dimensional electrode reactor[J]. Chemical Engineering Journal, 2017,327:597-607.
[10]
Chu H, Wang Z, Liu Y. Application of modified bentonite granulated electrodes for advanced treatment of pulp and paper mill wastewater in three-dimensional electrode system[J]. Journal of Environmental Chemical Engineering, 2016,4(2):1810-1817.
[11]
刘伟军,段平洲,胡翔,等.活性炭纤维三维电极电催化降解水中间甲酚-效能及影响因素研究[J]. 中国环境科学, 2019,39(1):166-171. Liu W J, Duan P Z, Hu X, et al. Efficacy and influencing factors of electrocatalytic degradation of m-cresol in wastewater by activated carbon fiber as three-dimensional electrodes[J]. China Environmental Science, 2019,39(1):166-171.
[12]
Chen Z, Zhang Y M, Zhou L C, et al. Performance of nitrogen-doped graphene aerogel particle electrodes for electro-catalytic oxidation of simulated Bisphenol A wastewaters[J]. Journal of Hazardous Materials, 332:70-78.
[13]
Zhang Y, Zhang D, Zhou L, et al. Polypyrrole/reduced graphene oxide aerogel particle electrodes for high efficiency electro-catalytic synergistic removal of Cr(VI) and bisphenol A[J]. Chemical Engineering Journal, 2018,336:690-700.
[14]
Pignatello J J, Oliveros E, Mackay A. Advanced oxidation processes for organic contaminant destruction based on the fenton reaction and related chemistry[J]. Critical Reviews in Environmental Science and Technology, 2006,36(1):1-84.
[15]
Li X, Pi Y, Wu L, et al. Facilitation of the visible light-induced Fenton-like excitation of H2O2via heterojunction of g-C3N4/NH2-Iron terephthalate metal-organic framework for MB degradation[J]. Applied Catalysis B Environmental, 2017,202:653-663.
[16]
Zheng G W, Wei J D, Wei Z, et al. Novel magnetic polysaccharide/graphene oxide@Fe3O4gel beads for adsorbing heavy metal ions[J]. Carbohydrate Polymers, 2019,216:119-128.
[17]
吴彦晨,戚后娟,黄占华.海藻酸钠/丙烯酰胺/氧化石墨烯复合凝胶球的制备与吸附性能研究[J]. 功能材料, 2017,48(8):117-122. Wu Y C, Qi H J, Huang Z H. Preparation and study of adsorption properties of sodium alginate/acrylamide/graphene oxide composite gel balls[J]. Journal of Functional Materials, 2017,48(8):117-122.
[18]
Chen K, Ling Y, Cao C, et al. Chitosan derivatives/reduced graphene oxide/alginate beads for small-molecule drug delivery[J]. Materials Science and Engineering:C, 2016,69:1222-1228.
[19]
Fadillah G, Tawfik A, Sayekti W, et al. Electrochemical removal of methylene blue using alginate-modified graphene adsorbents[J]. Chemical Engineering Journal, 2019,378:122-140.
[20]
Wang S B. A comparative study of Fenton and Fenton-like reaction kinetics in decolourisation of wastewater[J]. Dyes and Pigments, 2008,76(3):714-720.
[21]
Youssef N A, Shaban S A, Ibrahim F A, et al. Degradation of methyl orange using Fenton catalytic reaction[J]. Egyptian Journal of Petroleum, 2016,25(3):317-321.
[22]
He W, Ma Q, Wang J, et al. Preparation of novel kaolin-based particle electrodes for treating methyl orange wastewater[J]. Applied Clay Science, 2014,99:178-186.
[23]
Chen Y Z, Li N, Zhang Y, et al. Novel low-cost Fenton-like layered Fe-titanate catalyst:Preparation, characterization and application for degradation of organic colorants[J]. Journal of Colloid and Interface Science, 2014,422:9-15.
[24]
Sun H, Chen T, Kong L, et al. Potential of sludge carbon as new granular electrodes for degradation of acid orange 7[J]. Industrial & Engineering Chemistry Research, 2015,54(20):5468-5474.
[25]
汤哲人,陈泉源,邓东升,等.以黄铜矿作为颗粒三维电极的电Fenton氧化处理维尼纶废水中的COD研究[J]. 中国环境科学, 2017, 37(1):95-101. Tang Z R, Chen Q Y, Deng D S, et al. COD of vinylon waste-water oxidizing treatment by three-dimensional-electrode electricity-fenton using brass copper grains[J]. China Environmental Science, 2017, 37(1):95-101.
[26]
Zhang Y, Dou X, Liu J, et al. Decolorization of reactive brilliant red X-3B by heterogeneous photo-Fenton reaction using an Fe-Ce bimetal catalyst[J]. Catalysis Today, 2007,126(3/4):387-393.
[27]
冯俊生,姚海祥,蔡晨,等.微生物燃料电池电活化过硫酸盐降解甲基橙偶氮染料[J]. 环境科学研究, 2019,32(5):195-202. Feng J S, Yao H Y, Cai C, et al. Microbial fuel cell electro-activated persulfate to degrade methyl orange azo dye[J]. Research of Environmental Sciences, 2019,32(5):195-202.
[28]
Huang F, Chen L, Wang H, et al. Degradation of methyl orange by atmospheric DBD plasma:Analysis of the degradation effects and degradation path[J]. Journal of Electrostatics, 2012,70(1):43-47.
