Abstract：Large quantities of refractory organic matters still leave in the coking wastewater after biological treatment, making wastewater not meet the requirements of discharge or recycling. In the present study, activated carbon was applied as carrier. Five kinds of particle electrodes that were loaded with single elements of Ni, Fe and Co and binary elements of Ni-Fe and Co-Fe, were prepared and used to degrade the simulated coking tail-wastewater. The results showed that the particle electrodes loaded with binary elements achieved better treatment effects than those loaded with single elements. Ni-Fe/PAC possessed the best degradation performance among the electrodes, with COD and TOC removal efficiency of 70.1% and 40.1%, respectively. Ni-Fe/PAC also possessed the highest oxygen evolution potential and the lowest Tafel slope, namely 2.25V and 86mV/dec, respectively. The crystal structure was consisted by metallic Ni and Fe and small amount of iron oxide. The addition of particle electrodes resulted in the effluent to be alkaline. The loading Co increased the alkalinity, while the Fe was beneficial to reduce the pH value of effluent. The degradation effects of the three category organics in simulated wastewater were in the order of polycyclic aromatic hydrocarbon < heterocyclic compound < benzene series during Ni-Fe/PAC processes. Ni-Fe/PAC can catalyze the generation of ·OH and new atomic hydrogen. The degradation of organic matters was mainly fulfilled through indirect oxidation.
Yuan X Y, Sun H F, Guo D S. The removal of COD from coking wastewater using extraction replacement-biodegradation coupling[J]. Desalination, 2012,289:45-50.
Wu K Y, Zhang F Z, Wu H Z, et al. The mineralization of oxalic acid and bio-treated coking wastewater by catalytic ozonation using nickel oxide[J]. Environmental Science and Pollution Research, 2018,25(3):2389-2400.
Shi J X, Han Y X, Xu C Y, et al. Enhanced anaerobic degradation of selected nitrogen heterocyclic compounds with the assistance of carboxymethyl cellulose[J]. Science of the Total Environment, 2019, 689:781-788.
Wang S J, Li E, Du Z P, et al. Preparation of a PASi-P (AM-ADB) hybrid flocculant and efficiently removal bio-refractory organics from coking wastewater[J]. Environmental Chemistry Letters, 2019,17(1):509-514.
Pan M, Li H Z, Wu J. Study on catalysed treatment of coking wastewater by TiO2[J]. Oxidation Communications, 2016,39(4):3457-3461.
Ouyang S G, Yao J Y, Zhu G H, et al. Hydrophilic modification of a poly (ether sulfone) flat-sheet ultrafiltration membrane applied to coking sewage[J]. Journal of Applied Polymer Science, 2017,134(31):45149.
熊道文,王合德,刘利军,等.电絮凝法用于重金属废水处理研究进展[J]. 环境工程, 2013,31(S1):61-65. Xiong D W, Wang H D, Liu L J, et al. Research progress of electrocoagulation for treatment of heavy metal wastewater[J]. Environmental Engineering, 2013,31(S1):61-65.
Mohammadi L, Rahdar A, Bazrafshan E, et al. Petroleum hydrocarbon removal from wastewaters:a review[J]. Processes, 2020,8(4):447.
Zhao K, Quan X, Chen S, et al. Preparation of fluorinated activated carbon for electro-Fenton treatment of organic pollutants in coking wastewater:the influences of oxygen-containing groups[J]. Separation and Purification Technology, 2019,224:534-542.
李新洋,李燕楠,祁丹阳,等.电-多相臭氧催化工艺深度处理焦化废水[J]. 中国环境科学, 2020,40(10):4354-4361. Li X Y, Li Y N, Qi D Y, et al. Advanced treatment of coking wastewater by electro-multiphase ozonation[J]. China Environmental Science, 2020,40(10):4354-4361.
Jia Y N, Jiang W F, Hao S J, et al. Feasibility study on coking waste water treatment by three-dimensional electrode[J]. Advanced Materials Research, 2013,750:1437-1440.
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.
Zhen Y, Wu Y, Liu S Y, et al. A novel integrated system of three-dimensional electrochemical reactors (3DERs) and three-dimensional biofilm electrode reactors (3DBERs) for coking wastewater treatment[J]. Bioresource technology, 2019,284:222-230.
Cao G P, Xu F, Xia S G. Preparation of a composite particle electrode by electroless plating and its electrocatalytic performance in the decolorization of methyl orange dye solution[J]. Journal of the Brazilian Chemical Society, 2013,24(12):2050-2058.
Zhang W W, He Y C, Li C, et al. Persulfate activation using Co/AC particle electrodes and synergistic effects on humic acid degradation[J]. Applied Catalysis B:Environmental, 2021,285:119848.
Li S S, Gao Y Q, Li N, et al. Transition metal-based bimetallic MOFs and MOF-derived catalysts for electrochemical oxygen evolution reaction[J]. Energy & Environmental Science, 2021,14(4):1897-1927.
Nawaz M A, Saif M, Li M Z, et al. Tailoring the synergistic dual-decoration of (Cu-Co) transition metal auxiliaries in Fe-oxide/zeolite composite catalyst for the direct conversion of syngas to aromatics[J]. Catalysis Science & Technology, 2021,11(24):7992-8006.
Safizadeh F, Ghali E, Houlachi G. Electrocatalysis developments for hydrogen evolution reaction in alkaline solutions-a review[J]. International Journal of Hydrogen Energy, 2015,40(1):256-274.
Jiang H L, Xu Q. Recent progress in synergistic catalysis over heterometallic nanoparticles[J]. Journal of Materials Chemistry, 2011, 21(36):13705-13725.
高金龙,陈轶凡,李纪薇,等.Ti/PbO2电化学法降解废水中三种氟喹诺酮类抗生素[J]. 中国环境科学, 2020,40(6):2454-2463. Gao J L, Chen Y F, Li J W, et al. Degradation of three fluoroquinolones in wastewater by Electrochemical method of Ti/PbO2[J]. China Environmental Science, 2020,40(6):2454-2463.
岳文清,倪月,孙则朋,等.改性钛基PbO2电极对有机污染物的降解性能-以甲基橙和4-硝基苯酚为例[J]. 中国环境科学, 2022,42(2):706-716. Yue W Q, Ni Y, Sun Z P, et al. Degradation of organic pollutants by modified Titanium PbO2 electrode:Methyl orange and 4-nitrophenol as an example[J]. China Environmental Science, 2022,42(2):706-716.
He Y P, Lin H B, Guo Z C, et al. Recent developments and advances in boron-doped diamond electrodes for electrochemical oxidation of organic pollutants[J]. Separation and Purification Technology, 2019, 212:802-821.
苏冰琴,刘一清,林昱廷,等.Fe3O4活化过硫酸盐体系同步去除诺氟沙星和铅[J]. 中国环境科学, 2022,42(2):717-727. Su B Q, Liu Y Q, Lin Y T, et al. Simultaneous removal of Norfloxacin and Lead by Fe3O4 activated persulfate system[J]. China Environmental Science, 2022,42(2):717-727.
周爱娟,赵玉珏,刘芝宏,等.Fe(Ⅱ)活化过硫酸盐处理喹啉工艺参数优化及生物毒性[J]. 中国环境科学, 2020,40(11):4795-4803. Zhou A J, Zhao Y J, Liu Z H, et al. Treatment of quinoline by activated persulfate with Fe (Ⅱ) and its biotoxicity[J]. China Environmental Science, 2020,40(11):4795-4803.
Rieger R, Klaus M. Forever young:polycyclic aromatic hydrocarbons as model cases for structural and optical studies[J]. Journal of Physical Organic Chemistry, 2010,23(4):315-325.
谢成,晏波,韦朝海,等.焦化废水Fenton氧化预处理过程中主要有机污染物的去除[J]. 环境科学学报, 2007,(7):1101-1106. Xie C, Yan B, Wei C H, et al. Removal of organic pollutants from coking wastewater by Fenton oxidation pretreatment[J]. Chinese Journal of Environmental Science, 2007,(7):1101-1106.
许俊强,郭芳,全学军,等.焦化废水中的杂环化合物及多环芳烃降解的研究进展[J]. 化工进展, 2008,(7):973-976. Xu J Q, Guo F, Quan X J, et al. Progress in degradation of heterocyclic Compounds and polycyclic aromatic hydrocarbons in coking wastewater[J]. Chemical Industry and Engineering Progress, 2008,(7):973-976.
伍艳辉,傅晓廷,占志恒.TiO2/ZSM-5复合光催化剂降解多环芳烃(PAHs)废水[J]. 环境科学与技术, 2015,38(2):151-157. Wu Y H, Fu X T, Zhan Z H. Degradation of polycyclic aromatic hydrocarbons (PAHs) by TiO2/ZSM-5composite photocatalyst[J]. Environmental Science & Technology, 2015,38(2):151-157.