SA/GO@Fe3O4磁性粒子电极降解甲基橙废水的研究

doi:10.19741/j.issn.1673-4831.2019.0686

生态与农村环境学报 ›› 2020, Vol. 36 ›› Issue (6): 803-810.doi: 10.19741/j.issn.1673-4831.2019.0686

SA/GO@Fe₃O₄磁性粒子电极降解甲基橙废水的研究

张书陵^1,2, 封金财¹, 徐斌², 张毅敏^1,2, 杨飞², 张志伟²

1. 常州大学环境与安全工程学院, 江苏常州 213164;
2. 生态环境部南京环境科学研究所, 江苏南京 210042

收稿日期:2019-08-30 出版日期:2020-06-25 发布日期:2020-06-22
通讯作者: 徐斌 E-mail:xubinnies@163.com
作者简介:张书陵(1995-),男,江苏泰州人,硕士生,主要从事石墨烯电极材料以及电化学技术降解废水研究。E-mail:1914531980@qq.com
基金资助:
国家水体污染控制与治理科技重大专项（2017ZX07203-004）；江苏省自然科学基金青年科学基金（BK20170111）；国家自然科学基金青年科学基金（51808251）；江苏省科协青年科技人才托举工程

Degradation of Methyl Orange Wastewater by SA/GO@Fe₃O₄ Magnetic Particle Electrode

ZHANG Shu-ling^1,2, FENG Jin-cai¹, XU Bin², ZHANG Yi-min^1,2, YANG Fei², ZHANG Zhi-wei²

1. College of Environmental and Safety Engineering, Changzhou University, Changzhou 213164, China;
2. Nanjing Institute of Environmental Sciences, Ministry of Ecology and Environment, Nanjing 210042, China

Received:2019-08-30 Online:2020-06-25 Published:2020-06-22

摘要/Abstract

摘要： 该研究制备了SA/GO@Fe₃O₄磁性粒子电极，利用扫描电子显微镜、傅里叶红外变换光谱、X射线粉末衍射仪等手段研究了粒子电极的结构。选用甲基橙为目标污染物，考察初始pH、粒子电极投加量、电解时间和电流密度4个因素对甲基橙TOC去除率的影响。结果表明，4个因素影响由大到小依次为电流密度、电解时间、粒子电极投加量和初始pH。通过Box-Benhnken中心复合响应面设计评价实验效果，预测最佳反应条件为粒子电极投加量2.99 g·L^-1、电流密度29.58 mA·cm^-2，反应时间79.7 min、初始pH值4.31，此时甲基橙的总有机碳（TOC）去除率为80.03%。采用紫外可见吸收光谱、傅里叶变换红外光谱以及气相质谱联用对甲基橙降解过程产生的中间产物和机理进行了分析，推测了甲基橙的降解途径。粒子电极5 s可以快速磁分离，复用5次后降解率仅降低4.3%，具有优异的回收和复用性能。

关键词: 磁性粒子电极, 石墨烯, 甲基橙, 响应面法

Abstract: In this research, SA/GO@Fe₃O₄ magnetic particle electrode was prepared and the structure was characterized by means of scanning electron microscopy, Fourier transform infrared spectroscopy and X-ray powder diffraction. Methyl orange was selected as the target pollutant. The influence of four factors, including initial pH, particle electrode dosage, electrolysis time and current density, on TOC removal efficiency were investigated. The order influence degrees of the factors were as follows: current density > electrolysis time > particle electrode dosage > initial pH. In addition, the experimental results were evaluated by Box-Benhnken central composite response surface design. The optimum reaction conditions were predicted as particle electrode dosage 2.99 g·L^-1, current density 29.58 mA·cm^-2, reaction time 79.7 min and initial pH 4.31. On this condition, the TOC removal efficiency of methyl orange was 80.03%. The intermediate products and mechanism of the degradation process of methyl orange were analyzed by UV-Vis absorption spectroscopy and Fourier transform infrared spectroscopy, and the degradation pathway was speculated. Besides, particle electrode could be rapidly separated by magnetic field in five seconds. Meanwhile, the degradation efficiency decreased by only 4.3% after five reuses, which proves that SA/GO@Fe₃O₄ magnetic particle electrode has excellent recovery and reuse performance.

Key words: magnetic particle electrode, graphene, methyl orange, response surface methodology

中图分类号:

X703.5

张书陵, 封金财, 徐斌, 张毅敏, 杨飞, 张志伟. SA/GO@Fe₃O₄磁性粒子电极降解甲基橙废水的研究[J]. 生态与农村环境学报, 2020, 36(6): 803-810.

ZHANG Shu-ling, FENG Jin-cai, XU Bin, ZHANG Yi-min, YANG Fei, ZHANG Zhi-wei. Degradation of Methyl Orange Wastewater by SA/GO@Fe₃O₄ Magnetic Particle Electrode[J]. Journal of Ecology and Rural Environment, 2020, 36(6): 803-810.

参考文献 27

[1]	SARATAL R G,SAEATALE G D,CHANG J S,et al.Bacterial Decolorization and Degradation of Azo Dyes:A Review[J].Journal of the Taiwan Institute of Chemical Engineers,2011,42(1):138-157.
[2]	XU L,ZHAO H,SHI S,et al.Electrolytic Treatment of C.I.Acid Orange 7 in Aqueous Solution Using a Three-Dimensional Electrode Reactor[J].Dyes and Pigments,2008,77(1):158-164.
[3]	HOU Y,GAN Y,YU Z,et al.Solar Promoted Azo Dye Degradation and Energy Production in the Bio-Photoele Ctrochemical System With a g-C3N4/BiOBr Heterojunction Photocathode[J].Journal of Power Sources,2017,371:26-34.
[4]	CHEN Z,ZHANG Y,ZHOU L,et al.Performance of Nitrogen-Doped Graphene Aerogel Particle Electrodes for Electro-Catalytic Oxidation of Simulated Bisphenol A Wastewaters[J].Journal of Hazardous Materials,2017,332:70-78.
[5]	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.
[6]	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.
[7]	JIAO C L,LIU B C,JING Z X,et al.Sodium Alginate/Graphene Oxide Aerogel With Enhanced Strength-Toughness and Its Heavy Metal Adsorption Study[J].International Journal of Biological Macromolecules,2016,83:133-141.
[8]	SUN X F,LIU B,JING Z,et al.Preparation and Adsorption Property of Xylan/Poly(Acrylic Acid) Magnetic Nanocomposite Hydrogel Ddsorbent[J].Carbohydrate Polymers,2015,118:16-23.
[9]	吴先亮,黄先飞,张珍明.Fe3O4/GO对水溶液中Cd(Ⅱ)去除的影响因素[J].中国环境科学,2019,39(6):2411-2421.[WU Xian-liang,HUANG Xian-fei,ZHANG Zhen-ming.Influencing factors of Cd(Ⅱ) Removal From Aqueous Solution by Fe3O4/GO[J].China Environmental Science,2019,39(6):2411-2421.]
[10]	WANG Y,LI L L,LUO C N,et al.Removal of Pb2+ From Water Environment Using a Novel Magnetic Chitosan/Graphene Oxide Imprinted Pb2+[J].International Journal of Biological Macromolecules,2016,86:505-511.
[11]	GANJAR F,TAWFIK A S,SAYEKTI W,et al.Electrochemical Removal of Methylene Blue Using Alginate-Modified Graphene Adsorbents[J].Chemical Engineering Journal,2019,378:122-140.
[12]	WU Z,DENG W,ZHOU W,et al.Novel Magnetic Polysaccharide/Graphene Oxide@Fe3O4 Gel Beads for Adsorbing Heavy Metal Ions[J].Carbohydrate Polymers,2019,216:119-128.
[13]	SANG G,BARDAJEE G R,MIRSHOKRAIE A,et al.A Thermo/pH/Magnetic-Responsive Nanogel Based on Sodium Alginate by Modifying Magnetic Graphene Oxide:Preparation,Characterization,and Drug Delivery[J].Iranian Polymer Journal,2018,27(3):1-8.
[14]	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 Zhe-ren,CHEN Quan-yuan,DENG Dong-sheng,et al.COD Treatment of Vinylon Wastewater by Electro-Fenton Oxidation Using Chalcopyrite as Three-Dimensional Particle Electrode[J].China Environmental Science,2017,37(1):95-101.]
[15]	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.
[16]	LI R,JIN X,MEGHARAJ M,et al.Heterogeneous Fenton Oxidation of 2,4-Dichlorophenol Using Iron-Based Nanoparticles and Persulfate System[J].Chemical Engineering Journal,2015,264:587-594.
[17]	CHEN Y,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.
[18]	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.
[19]	陈磊,张杰,龙琦,等.Ce-Mn/Al2O3-H2O2催化氧化皮革废水的研究[J].环境科学学报,2019,39(3):84-90.[CHEN Lei,ZHANG Jie,LONG Qi,et al.Study on Catalytic Oxidation of Leather Wastewater by Ce-Mn/Al2O3-H2O2[J].Journal of Environmental Science,2019,39(3):84-90.]
[20]	JUNG K W,HWANG M J,PARK D S,et al.Combining Fluidized Metal-Impregnated Granular Activated Carbon in Three-Dimensional Electrocoagulation System:Feasibility and Optimization Test of Color and COD Removal From Real Cotton Textile Wastewater[J].Separation and Purification Technology,2015,146:154-167.
[21]	ZHANG B G,HANY P,YUZ B,et al.Three-Dimensional Electro-Fenton Degradation of Rhodamine B With Efficient Fe-Cu/Kaolin Particle Electrodes:Electrodes Optimization,Kinetics,Influencing Factors and Mechanism[J].Separation and Purification Technology,2019,210:60-68.
[22]	LI S H,ZHAO Y,CHU J,et al.Electrochemical Degradation of Methyl Orange on Pt-Bi/C Nanostructured Electrode by a Square-Wave Potential Method[J].Electrochimica Acta,2013,92:93-101.
[23]	PARSHETTI G K,TEIKE A A,KALYANI D C,et al.Decolorization and Detoxification of Sulfonated Azo Dye Methyl Orange by Kocuriarosea MTCC 1532[J].Journal of Hazardous Materials,2010,176(1/2/3):503-509.
[24]	HAN J,ZENG H Y,XU S,et al.Catalytic properties of CuMgAlO Catalyst and Degradation Mechanism in CWPO of Methyl Orange[J].Applied Catalysis A General,2016,527:72-80.
[25]	HE Y,GRIESER F,ASHOKKUMAR M.The Mechanism of Sonophotocatalytic Degradation of Methyl Orange and Its Products in Aqueous Solutions[J].Ultrasonics Sonochemistry,2011,18(5):974-980.
[26]	CECILIA R,SALDA A A,BERENICE H,et al.Electrochemical Oxidation of Methyl Orange Azo Dye at Pilot Flow Plant Using BDD Technology[J].Journal of Industrial & Engineering Chemistry,2013,19(2).
[27]	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.

SA/GO@Fe₃O₄磁性粒子电极降解甲基橙废水的研究

Degradation of Methyl Orange Wastewater by SA/GO@Fe₃O₄ Magnetic Particle Electrode

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