响应曲面法优化电化学氧化处理染料废水工艺参数的研究
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摘要
采用响应曲面分析中的Box-Behnken设计法,以电流密度、初始pH值、氯化钠浓度和反应时间为实验因素,以电化学氧化处理酸性粒子元青染料废水过程中的TOC去除率和能耗为响应值,通过响应曲面法结合优化期望函数得出电化学氧化最优效能的工艺参数。结果表明,分析得出的TOC去除率与反应能耗的多元二次回归模型均达到显著并有很好的相关性。电化学氧化最优工艺参数为电流密度55mA/cm~2,初始pH值为6,氯化钠浓度0.15mol/L,反应时间120min,在此条件下,TOC去除率为80.20%,能耗为19.85kWh/g(TOC),预测值与实际值之间的相对误差分别为2.2%与4.6%。表明此方法可用于优化电化学氧化处理染料废水工艺参数,为实际工程应用中制定高效节能的处理方案提供参考。
The Box-Behnken design was with current density,pH value,sodium chloride concentration,reactive time as independent variable,and TOC removal,energy consumption of electrochemical oxidation of Acid black 2 dye wastewater as responses.The electrochemical process parameters was optimized by response surface methodology and desirability function.The result indicated the multi-quadratic regression models for TOC removal rate and reaction energy consumption obtained by the analysis were significant and had good correlation.The optimal process parameters were as follow:current density of 55 mA/cm~2,initial pH value of 6,with a sodium chloride concentration of 0.15 mol/L and a reaction time of 120 min.Under optimal condition,a TOC removal of 80.20% and a energy consumption of 19.85 kWh/g(TOC)were achieved.Compared to the verification experiment consequence,the relative error was 2.2% and4.6%,respectively.The results showed that this method could be used to optimize the process parameters of electrochemical oxidation treatment of dye wastewater,and provided useful information for formulating a high efficiency and energy saving treatment proposal in practical project.
The Box-Behnken design was with current density,pH value,sodium chloride concentration,reactive time as independent variable,and TOC removal,energy consumption of electrochemical oxidation of Acid black 2 dye wastewater as responses.The electrochemical process parameters was optimized by response surface methodology and desirability function.The result indicated the multi-quadratic regression models for TOC removal rate and reaction energy consumption obtained by the analysis were significant and had good correlation.The optimal process parameters were as follow:current density of 55 mA/cm~2,initial pH value of 6,with a sodium chloride concentration of 0.15 mol/L and a reaction time of 120 min.Under optimal condition,a TOC removal of 80.20% and a energy consumption of 19.85 kWh/g(TOC)were achieved.Compared to the verification experiment consequence,the relative error was 2.2% and4.6%,respectively.The results showed that this method could be used to optimize the process parameters of electrochemical oxidation treatment of dye wastewater,and provided useful information for formulating a high efficiency and energy saving treatment proposal in practical project.
引文
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[20]盛贵尚.掺硼金刚石电极电化学氧化晚期垃圾渗滤液试验研究[D].重庆:重庆大学,2015.Sheng G S.Experimental Research on Electrochemical Oxidation of Mature Landfill Leachate on Boron-Doped Diamond Anode[D].Chongqing:Chongqing University,2015.
[21]Li J,Liu Q,Qing Ji Q,et al.Degradation of p-nitrophenol(PNP)in aqueous solution by Fe0-PM-PS system through response surface methodology(RSM)[J].Applied Catalysis B:Environmental,2017,200:633-646.
[22]Zou J,Peng X,Li M,et al.Electrochemical oxidation of COD from real textile wastewaters:Kinetic study and energy consumption[J].Chemosphere,2017,171:332-338.
[23]Tavares M G,da Silva L V A,Solano A M S,et al.Electrochemical oxidation of methyl red using Ti/Ru0.3Ti0.7O2and Ti/Pt anodes[J].Chemical Engineering Journal,2012,204:141-150.
[24]孙海波.超声电化学氧化降解偶氮染料废水的研究[D].南京:南京航空航天大学,2008.Sun H B.Research on Ultrasonic and Electrical Oxidation Degradation of Azo Dyes Wastewater[D].Nanjing:Nanjing University of Aeronautics and Astronautics,2008.
[25]Panizza M,Delucchi M,Sirés I.Electrochemical process for the treatment of landfill leachate[J].Journal of Applied Electrochemistry,2010,40(10):1721-1727.
[26]Derringer G,Suich R.Simultaneous optimization of several response variables[J].Journal of Quality Technology,1980,12(4):214-219.
[2]付莉燕,文湘华,吕秋丽,等.改良型SBR系统处理染料废水的研究[J].中国环境科学,2001,21(2):128-132.Fu L Y,Wen X H,Lu Q L,et al.Study on improved SBR systems in treating dyeing wastewater[J].China Environmental Science,2001,21(2):128-132.
[3]王慧,王建龙,占新民,等.电化学法处理含盐染料废水[J].中国环境科学,1999,19(5):441-444.Wang H,Wang J L,Zhan X M,et al.Electrochemical method treatment of dye effluents containing NaCl of high concentration[J].China Environmental Science,1999,19(5):441-444.
[4]Yazdanbakhsh M R,Ghanadzadeh A,Moradi E.Synthesis of some new azo dyes derived from 4-hydroxy coumarin and spectrometric determination of their acidic dissociation constants[J].Journal of Molecular Liquids,2007,136(1-2):165-168.
[5]Labiadh L,Barbucci A,Carpanese M P,et al.Comparative depollution of Methyl Orange aqueous solutions by electrochemical incineration using TiRuSnO2,BDD and PbO2as high oxidation power anodes[J].Journal of Electroanalytical Chemistry,2016,766:94-99.
[6]Lin S H,Peng C F.Continuous treatment of textile wastewater by combined coagulation,electrochemical oxidation and activated sludge[J].Water Research,1996,30(3):587-592.
[7]张明全,王一佳,曾思超,等.硼掺杂金刚石电极降解活性橙XGN偶氮染料废水的研究[J].表面技术,2017,46(7):128-133.Zhang M Q,Wang Y J,Zeng S C,et al.Degradation of reactive brilliant orange X-GN azo dye effluent on boron-doped diamond electrode[J].Surface Technology,2017,46(7):128-133.
[8]管玉江,杨卫身.复极性固定床电解反应器对活性染料的降解[J].环境化学,1999,18(3):270-273.Guan Y J,Yang W S.Degradation of reactive dyes by bipolar fixed-bed electrolysis reactor[J].Environmental Chemistry,1999,18(3):270-273.
[9]许海梁,杨卫身,周集体,等.偶氮染料废水的电解处理[J].化工环保,1999,19(1):32-36.Xu H L,Yang W S,Zhou J T,et al.Treatment of wastewater from azo dye production by electrolysis[J].Environmental Protection of Chemical Industry,1999,19(1):32-36.
[10]Mook W T,Ajeel M A,Aroua M K,et al.The application of iron mesh double layer as anode for the electrochemical treatment of Reactive Black 5dye[J].Journal of Environmental Sciences,2017,54(4):184-195.
[11]王栗,岳琳,王开红,等.响应曲面法优化电化学氧化技术处理染料废水[J].环境工程学报,2014,8(3):990-996.Wang L,Yue L,Wang K H,et al.Optimization of electrochemical oxidation of dye wastewater using response surface methodology[J].Chinese Journal of Environmental Engineering,2014,8(3):990-996.
[12]Liyana-Pathirana C,Shahidi F.Optimization of extraction of phenolic compounds from wheat using response surface methodology[J].Food Chemistry,2005,93(1):47-56.
[13]Li M,Feng C,Zhang Z,et al.Optimization of process parameters for electrochemical nitrate removal using Box-Behnken design[J].Electrochimica Acta,2010,56(1):265-270.
[14]程正军.运用响应曲面法优化有机污染物吸附过程参数及其吸附平衡和动力学研究[D].成都:西南石油大学,2015.Cheng Z J.Optimizing Adsorption Process Parameters of Organic Pollutants by Response Surface Methodology and Investigating Their Adsorption Equilibrium and Kinetics[D].Chengdu:Southwest Petroleum University,2015.
[15]He Y,Wang X,Huang W,et al.Application of porous borondoped diamond electrode towards electrochemical mineralization of triphenylmethane dye[J].Journal of Electroanalytical Chemistry,2016,775:292-298.
[16]朱维.脉冲三维电极反应器的开发与柠檬酸废水处理应用研究[D].北京:清华大学,2014.Zhu W.Development and Application of a Pulse Three-Dimensional Electrode Reactor in Citric acid Wastewater Treatment[D].Beijing:Tsinghua University,2014.
[17]Comninellis C,Nerini A.Anodic oxidation of phenol in the presence of NaCl for wastewater treatment[J].Journal of Applied Electrochemistry,1995,25(1):23-28.
[18]Simond O,Schaller V,Comninellis C.Theoretical model for the anodic oxidation of organics on metal oxide electrodes[J].Electrochimica Acta,1997,42(13-14):2009-2012.
[19]Feng J,Houk L L,Johnson D C,et al.Electrocatalysis of anodic oxygen-transfer reactions:The electrochemical incineration of benzoquinone[J].Journal of the Electrochemical Society,1995,142(11):3626-3632.
[20]盛贵尚.掺硼金刚石电极电化学氧化晚期垃圾渗滤液试验研究[D].重庆:重庆大学,2015.Sheng G S.Experimental Research on Electrochemical Oxidation of Mature Landfill Leachate on Boron-Doped Diamond Anode[D].Chongqing:Chongqing University,2015.
[21]Li J,Liu Q,Qing Ji Q,et al.Degradation of p-nitrophenol(PNP)in aqueous solution by Fe0-PM-PS system through response surface methodology(RSM)[J].Applied Catalysis B:Environmental,2017,200:633-646.
[22]Zou J,Peng X,Li M,et al.Electrochemical oxidation of COD from real textile wastewaters:Kinetic study and energy consumption[J].Chemosphere,2017,171:332-338.
[23]Tavares M G,da Silva L V A,Solano A M S,et al.Electrochemical oxidation of methyl red using Ti/Ru0.3Ti0.7O2and Ti/Pt anodes[J].Chemical Engineering Journal,2012,204:141-150.
[24]孙海波.超声电化学氧化降解偶氮染料废水的研究[D].南京:南京航空航天大学,2008.Sun H B.Research on Ultrasonic and Electrical Oxidation Degradation of Azo Dyes Wastewater[D].Nanjing:Nanjing University of Aeronautics and Astronautics,2008.
[25]Panizza M,Delucchi M,Sirés I.Electrochemical process for the treatment of landfill leachate[J].Journal of Applied Electrochemistry,2010,40(10):1721-1727.
[26]Derringer G,Suich R.Simultaneous optimization of several response variables[J].Journal of Quality Technology,1980,12(4):214-219.