染色残液电化学处理碳素阴极材料性能比较
|
摘要
为实现染色残液的高效处理及废水回用,鉴于染色残液良好的导电性,选用电化学处理技术,以模拟活性红X-3B染色残液为研究对象,在钌铱形稳电极为阳极和合适的电解条件下,比较石墨板、石墨毡、炭毡、ACF(活性炭纤维毡)、碳纤维电极[CFF(碳纤维布)、CFB(碳纤维刷)]等碳素阴极材料的电化学处理效能.结果表明:碳素阴极材料可实现染色残液的完全脱色,活性红X-3B的降解过程符合一级反应动力学特征,其中CFF为阴极时CODCr去除率达到86. 37%,一级动力学反应常数为0. 010 3 min-1,是石墨毡(0. 007 3 min-1)的1. 4倍.相比于石墨板电极,CFB显示出优异的二电子氧还原和产H2O2能力,单位面积产H2O2的浓度为10. 40μmol/L,是石墨板(1. 08μmol/L)的9. 7倍,产生的H2O2导致活性红X-3B的降解,30 min内实现完全脱色.循环伏安曲线表明,碳纤维电极(包括CFF和CFB)的析氧电位明显高于其他电极,可有效抑制析氧副反应,提高有机污染物降解过程中的电催化效率,有利于降低能耗.研究显示,碳纤维可作为阴极材料应用于电化学处理染色残液,具有良好的稳定性.
In order to treat dyeing residual liquid effectively and reuse wastewater and salt,electrochemical oxidation was applied due to its excellent conductivity. The present work focused on comparing the performance of different carbonaceous cathodes materials,including graphite plate,graphite felt,carbon felt,active carbon felt( ACF),carbon fiber electrode( carbon fiber fabric( CFF),and carbon fiber brush( CFB)) using Ru-Ir DSA as an anode. For simulated Reactive Red X-3 B dyeing residual liquids,it was found that carbonaceous cathodes materials could achieve a complete decolorization and the degradation of Reactive Red X-3 B followed the first-order kinetics.Using CFF cathode,the removal of CODCrof dyeing residual liquid was 86. 37%. The first-order kinetic reaction constant on CFF cathodewas 0. 0103 min-1,1. 4 folds of that on carbon felt cathode( 0. 0073 min-1). Comparing to the graphite plate cathode,the CFB cathode exhibited excellent efficacy for 2 e-oxygen reduction reaction and H2 O2 generation capacity,leading to the degradation of Reactive Red X-3 B. The H2 O2 generation per area of CFB cathode was 10. 40 μmol/L,which was 9. 7 folds of that of graphite plate cathode( 1. 08μmol/L). Based on CV examination,the oxygen evolution potential of carbon fiber electrodes,including CFF and CFB,was found to be higher than the other cathodes used in this work,which favors the inhibition of oxygen evolution and improves electro catalytic efficiency.The results of this study show that carbon fiber cathode with desirable stability may have potential industrial applications in dyeing residual liquid treatment.
In order to treat dyeing residual liquid effectively and reuse wastewater and salt,electrochemical oxidation was applied due to its excellent conductivity. The present work focused on comparing the performance of different carbonaceous cathodes materials,including graphite plate,graphite felt,carbon felt,active carbon felt( ACF),carbon fiber electrode( carbon fiber fabric( CFF),and carbon fiber brush( CFB)) using Ru-Ir DSA as an anode. For simulated Reactive Red X-3 B dyeing residual liquids,it was found that carbonaceous cathodes materials could achieve a complete decolorization and the degradation of Reactive Red X-3 B followed the first-order kinetics.Using CFF cathode,the removal of CODCrof dyeing residual liquid was 86. 37%. The first-order kinetic reaction constant on CFF cathodewas 0. 0103 min-1,1. 4 folds of that on carbon felt cathode( 0. 0073 min-1). Comparing to the graphite plate cathode,the CFB cathode exhibited excellent efficacy for 2 e-oxygen reduction reaction and H2 O2 generation capacity,leading to the degradation of Reactive Red X-3 B. The H2 O2 generation per area of CFB cathode was 10. 40 μmol/L,which was 9. 7 folds of that of graphite plate cathode( 1. 08μmol/L). Based on CV examination,the oxygen evolution potential of carbon fiber electrodes,including CFF and CFB,was found to be higher than the other cathodes used in this work,which favors the inhibition of oxygen evolution and improves electro catalytic efficiency.The results of this study show that carbon fiber cathode with desirable stability may have potential industrial applications in dyeing residual liquid treatment.
引文
[1] ZHANG Jing,HUANG Guoqing,LIU Chun,et al.Synergistic effect of microbubbles and activated carbon on the ozonation treatment of synthetic dyeing wastewater[J]. Separation and Purification Technology,2018,201:10-18.
[2] ZHANG Congcan,DONG Yongchun,LI Bing,et al. Comparative study of three solid oxidants as substitutes of H2O2,used in Fe(III)-oxalate complex mediated Fenton system for photocatalytic elimination of reactive azo dye[J]. Journal of Cleaner Production,2018,177:245-253.
[3]袁超,李磊,孙应龙,等.零价铝还原处理偶氮染料活性蓝222废水[J].环境科学研究,2016,29(7):1067-1074.YUAN Chao,LI Lei,SUN Yinglong,et al. Treatment of Reactive Blue 222 wastewater by zero-valent aluminum reduction[J].Research of Environmental Sciences,2016,29(7):1067-1074.
[4] CAI Dong,ZHANG Tailiang,ZHANG Fangjie,et al. Quaternary ammoniumβ-cyclodextrin-conjugated magnetic nanoparticles as nano-adsorbents for the treatment of dyeing wastewater:synthesis and adsorption studies[J]. Journal of Environmental Chemical Engineering,2017,5(3):2869-2878.
[5] WANG Hongcheng,CUI Dan,YANG Lihui,et al. Increasing the bio-electrochemical system performance in azo dye wastewater treatment:reduced electrode spacing for improved hydrodynamics[J].Bioresource Technology,2017,245:962-969.
[6]韩志涛,于景奇,杨少龙,等.电解海水对模拟船舶柴油机废气的脱硝应用[J].环境科学研究,2017,30(1):144-151.HAN Zhitao,YU Jingqi,YANG Shaolong,et al. Application of electrolyzed seawater for NO removal from simulated marine diesel engine exhaust gas[J].Research of Environmental Sciences,2017,30(1):144-151.
[7] COTILLAS S,LLANOS J,CANIZARES P,et al. Removal of procion red MX-5B dye from wastewater by conductive-diamond electrochemical oxidation[J].Electrochimica Acta,2018,263:1-7.
[8] LIU Mengjiao,WANG Li,MU Yanlin,et al. A novel Ni CoMnO4anode material:construction of nanosheet architecture and superior electrochemical performances[J].Scripta Materialia,2018,146:13-17.
[9] GOMES F E R,SOUZA N E D,GALINARO C A,et al.Electrochemical degradation of butyl paraben on platinum and glassy carbon electrodes[J].Journal of Electroanalytical Chemistry,2016,769:124-130.
[10] IGLESIAS O,MA F D D,PAZOS M,et al. Using iron-loaded sepiolite obtained by adsorption as a catalyst in the electro-Fenton oxidation of Reactive Black 5[J]. Environmental Science and Pollution Research International,2013,20(9):5983-5993.
[11]王琳,李雪,王丽.复合生物阴极型微生物燃料电池处理废水及同步产电性能[J].环境科学研究,2017,30(7):1098-1104.WANG Lin,LI Xue,WANG Li.Performance of a hybrid biocathode microbial fuel cell for wastewater treatment and electricity generation[J].Research of Environmental Sciences,2017,30(7):1098-1104.
[12] BOCOS E,ALFAYA E,IGLESIAS O,et al. Application of a new sandwich of granular activated and fiber carbon as cathode in the electrochemical advanced oxidation treatment of pharmaceutical effluents[J]. Separation and Purification Technology,2015,151:243-250.
[13] MEIJIDE J,GOMEZ J,PAZOS M,et al. Degradation of thiamethoxam by the synergetic effect between anodic oxidation and Fenton reactions[J].Journal of Hazardous Materials,2016,319:43-50.
[14] LE T X H,BECHELANY M,CRETIN M. Carbon felt basedelectrodes for energy and environmental applications:a review[J].Carbon,2017,122:564-591.
[15] MOREIRA F C,GARCIA S S,RUI A R B,et al.Degradation of the antibiotic trimethoprim by electrochemical advanced oxidation processes using a carbon-PTFE air-diffusion cathode and a borondoped diamond or platinum anode[J]. Applied Catalysis B:Environmental,2014,160-161(1):492-505.
[16] KHATAEE A,FATHINIA M,BEHROUZ V,et al.Kinetic modeling of photoassisted-electrochemical process for degradation of an azo dye using boron-doped diamond anode and cathode with carbon nanotubes[J]. Journal of Industrial and Engineering Chemistry,2013,19(6):1890-1894.
[17] KOUSHANPOUR A,GUZ N,GAMELLA M,et al. Graphene functionalized 3D-carbon fiber electrodes preparation and electrochemical characterization[J]. Electroanalysis,2016,28(9):1943-1946.
[18] CAMPOS B G,ACOSTA D M,RAMIREZ A H,et al.Air diffusion electrodes based on synthetized mesoporous carbon for pplication in amoxicillin degradation by electro-Fenton and solarphoto electroFenton[J].Electrochimica Acta,2018,269:232-240.
[19]张冬梅,刘蕾,褚衍洋.电-Fenton氧化降解2,4-二氯酚[J].环境科学研究,2012,25(9):1041-1046.ZHANG Dongmei,LIU Lei,CHU Yanyang. Degradation of 2,4-dichlorophenol by electro-Fenton oxidation process[J].Research of Environmental Sciences,2012,25(9):1041-1046.
[20] BANUELOS J A,GARCIA R O,EL-GHENYMY A,et al.Advanced oxidation treatment of malachite green dye using a low cost carbon-felt air-diffusion cathode[J]. Journal of Environmental Chemical Engineering,2016,4(2):2066-2075.
[21] LI Kunquan,LIU Jiaming,LI Jun,et al.Effects of N mono-and NP dual-doping on H2O2,·OH generation,and MB electrochemical degradation efficiency of activated carbon fiber electrodes[J].Chemosphere,2017,193:800-810.
[22] CHOI J,SUN H H,JANG J,et al. High yield hydrogen peroxide production in a solid polymer electrolyte electrolyzer with a carbon fiber coated mesh substrate[J]. Electrochemistry Communications,2013,30(30):95-98.
[23] MINKE C,KUNZ U,TUREK T. Carbon felt and carbon fiber-A techno-economic assessment of felt electrodes for redox flow battery applications[J].Journal of Power Sources,2017,342:116-124.
[24] LUO Shuai,HE Zhen. Ni-coated carbon fiber as an alternative cathode electrode material to improve cost efficiency of microbial fuel cells[J].Electrochimica Acta,2016,222:338-346.
[25] ZHANG Jianan,LIU Ping,JIN Chun,et al. Flexible threedimensional carbon clothcarbon fibersNiCo2O4, composite electrode materials for high-performance all-solid-state electrochemical capacitors[J].Electrochimica Acta,2017,256:90-99.
[26] LAN Huachun,HE Wenjing,WANG Aimin,et al. An activated carbon fiber cathode for the degradation of glyphosate in aqueous solutions by the electro-Fenton mode:optimal operational conditions and the deposition of iron on cathode on electrode reusability[J].Water Research,2016,105:575-582.
[27] HU Jingjing,SUN Jie,YAN Junkun,et al. A novel efficient electrode material:activated carbon fibers grafted by ordered mesoporous carbon[J].Electrochemistry Communications,2013,28(1):67-70.
[28] CHEN Kunfeng,XUE Dongfeng. From graphite-clay composites to graphene electrode materials:in-situ electrochemical oxidation and functionalization[J].Materials Research Bulletin,2017,96:281-285.
[29]杜利顺.TiSnO2+Sb2O3电极优化及电解氧化对纳滤处理染料废水的影响[D].天津:天津大学,2012:27-28.
[30] POPESCU M,SANDU C,ROSALES E,et al.Evaluation of different cathodes and reaction parameters on the enhancement of the electro-Fenton process[J]. Journal of Electroanalytical Chemistry,2017,808:455-463.
[31] XU Haibo,XIA Guangsen,LIU Haining,et al. Electrochemical activation of commercial polyacrylonitrile-based carbon fiber for the oxygen reduction reaction[J]. Physical Chemistry Chemical Physics,2015,17(12):7707-7713.
[32] KARUPPIAH M T,RAJU G B.Anodic degradation of CI Reactive Blue 221 using graphite and Ir O2TaO2RuO2coated titanium electrodes[J]. Industrial and Engineering Chemistry Research,2009,48(4):2149-2156.
[2] ZHANG Congcan,DONG Yongchun,LI Bing,et al. Comparative study of three solid oxidants as substitutes of H2O2,used in Fe(III)-oxalate complex mediated Fenton system for photocatalytic elimination of reactive azo dye[J]. Journal of Cleaner Production,2018,177:245-253.
[3]袁超,李磊,孙应龙,等.零价铝还原处理偶氮染料活性蓝222废水[J].环境科学研究,2016,29(7):1067-1074.YUAN Chao,LI Lei,SUN Yinglong,et al. Treatment of Reactive Blue 222 wastewater by zero-valent aluminum reduction[J].Research of Environmental Sciences,2016,29(7):1067-1074.
[4] CAI Dong,ZHANG Tailiang,ZHANG Fangjie,et al. Quaternary ammoniumβ-cyclodextrin-conjugated magnetic nanoparticles as nano-adsorbents for the treatment of dyeing wastewater:synthesis and adsorption studies[J]. Journal of Environmental Chemical Engineering,2017,5(3):2869-2878.
[5] WANG Hongcheng,CUI Dan,YANG Lihui,et al. Increasing the bio-electrochemical system performance in azo dye wastewater treatment:reduced electrode spacing for improved hydrodynamics[J].Bioresource Technology,2017,245:962-969.
[6]韩志涛,于景奇,杨少龙,等.电解海水对模拟船舶柴油机废气的脱硝应用[J].环境科学研究,2017,30(1):144-151.HAN Zhitao,YU Jingqi,YANG Shaolong,et al. Application of electrolyzed seawater for NO removal from simulated marine diesel engine exhaust gas[J].Research of Environmental Sciences,2017,30(1):144-151.
[7] COTILLAS S,LLANOS J,CANIZARES P,et al. Removal of procion red MX-5B dye from wastewater by conductive-diamond electrochemical oxidation[J].Electrochimica Acta,2018,263:1-7.
[8] LIU Mengjiao,WANG Li,MU Yanlin,et al. A novel Ni CoMnO4anode material:construction of nanosheet architecture and superior electrochemical performances[J].Scripta Materialia,2018,146:13-17.
[9] GOMES F E R,SOUZA N E D,GALINARO C A,et al.Electrochemical degradation of butyl paraben on platinum and glassy carbon electrodes[J].Journal of Electroanalytical Chemistry,2016,769:124-130.
[10] IGLESIAS O,MA F D D,PAZOS M,et al. Using iron-loaded sepiolite obtained by adsorption as a catalyst in the electro-Fenton oxidation of Reactive Black 5[J]. Environmental Science and Pollution Research International,2013,20(9):5983-5993.
[11]王琳,李雪,王丽.复合生物阴极型微生物燃料电池处理废水及同步产电性能[J].环境科学研究,2017,30(7):1098-1104.WANG Lin,LI Xue,WANG Li.Performance of a hybrid biocathode microbial fuel cell for wastewater treatment and electricity generation[J].Research of Environmental Sciences,2017,30(7):1098-1104.
[12] BOCOS E,ALFAYA E,IGLESIAS O,et al. Application of a new sandwich of granular activated and fiber carbon as cathode in the electrochemical advanced oxidation treatment of pharmaceutical effluents[J]. Separation and Purification Technology,2015,151:243-250.
[13] MEIJIDE J,GOMEZ J,PAZOS M,et al. Degradation of thiamethoxam by the synergetic effect between anodic oxidation and Fenton reactions[J].Journal of Hazardous Materials,2016,319:43-50.
[14] LE T X H,BECHELANY M,CRETIN M. Carbon felt basedelectrodes for energy and environmental applications:a review[J].Carbon,2017,122:564-591.
[15] MOREIRA F C,GARCIA S S,RUI A R B,et al.Degradation of the antibiotic trimethoprim by electrochemical advanced oxidation processes using a carbon-PTFE air-diffusion cathode and a borondoped diamond or platinum anode[J]. Applied Catalysis B:Environmental,2014,160-161(1):492-505.
[16] KHATAEE A,FATHINIA M,BEHROUZ V,et al.Kinetic modeling of photoassisted-electrochemical process for degradation of an azo dye using boron-doped diamond anode and cathode with carbon nanotubes[J]. Journal of Industrial and Engineering Chemistry,2013,19(6):1890-1894.
[17] KOUSHANPOUR A,GUZ N,GAMELLA M,et al. Graphene functionalized 3D-carbon fiber electrodes preparation and electrochemical characterization[J]. Electroanalysis,2016,28(9):1943-1946.
[18] CAMPOS B G,ACOSTA D M,RAMIREZ A H,et al.Air diffusion electrodes based on synthetized mesoporous carbon for pplication in amoxicillin degradation by electro-Fenton and solarphoto electroFenton[J].Electrochimica Acta,2018,269:232-240.
[19]张冬梅,刘蕾,褚衍洋.电-Fenton氧化降解2,4-二氯酚[J].环境科学研究,2012,25(9):1041-1046.ZHANG Dongmei,LIU Lei,CHU Yanyang. Degradation of 2,4-dichlorophenol by electro-Fenton oxidation process[J].Research of Environmental Sciences,2012,25(9):1041-1046.
[20] BANUELOS J A,GARCIA R O,EL-GHENYMY A,et al.Advanced oxidation treatment of malachite green dye using a low cost carbon-felt air-diffusion cathode[J]. Journal of Environmental Chemical Engineering,2016,4(2):2066-2075.
[21] LI Kunquan,LIU Jiaming,LI Jun,et al.Effects of N mono-and NP dual-doping on H2O2,·OH generation,and MB electrochemical degradation efficiency of activated carbon fiber electrodes[J].Chemosphere,2017,193:800-810.
[22] CHOI J,SUN H H,JANG J,et al. High yield hydrogen peroxide production in a solid polymer electrolyte electrolyzer with a carbon fiber coated mesh substrate[J]. Electrochemistry Communications,2013,30(30):95-98.
[23] MINKE C,KUNZ U,TUREK T. Carbon felt and carbon fiber-A techno-economic assessment of felt electrodes for redox flow battery applications[J].Journal of Power Sources,2017,342:116-124.
[24] LUO Shuai,HE Zhen. Ni-coated carbon fiber as an alternative cathode electrode material to improve cost efficiency of microbial fuel cells[J].Electrochimica Acta,2016,222:338-346.
[25] ZHANG Jianan,LIU Ping,JIN Chun,et al. Flexible threedimensional carbon clothcarbon fibersNiCo2O4, composite electrode materials for high-performance all-solid-state electrochemical capacitors[J].Electrochimica Acta,2017,256:90-99.
[26] LAN Huachun,HE Wenjing,WANG Aimin,et al. An activated carbon fiber cathode for the degradation of glyphosate in aqueous solutions by the electro-Fenton mode:optimal operational conditions and the deposition of iron on cathode on electrode reusability[J].Water Research,2016,105:575-582.
[27] HU Jingjing,SUN Jie,YAN Junkun,et al. A novel efficient electrode material:activated carbon fibers grafted by ordered mesoporous carbon[J].Electrochemistry Communications,2013,28(1):67-70.
[28] CHEN Kunfeng,XUE Dongfeng. From graphite-clay composites to graphene electrode materials:in-situ electrochemical oxidation and functionalization[J].Materials Research Bulletin,2017,96:281-285.
[29]杜利顺.TiSnO2+Sb2O3电极优化及电解氧化对纳滤处理染料废水的影响[D].天津:天津大学,2012:27-28.
[30] POPESCU M,SANDU C,ROSALES E,et al.Evaluation of different cathodes and reaction parameters on the enhancement of the electro-Fenton process[J]. Journal of Electroanalytical Chemistry,2017,808:455-463.
[31] XU Haibo,XIA Guangsen,LIU Haining,et al. Electrochemical activation of commercial polyacrylonitrile-based carbon fiber for the oxygen reduction reaction[J]. Physical Chemistry Chemical Physics,2015,17(12):7707-7713.
[32] KARUPPIAH M T,RAJU G B.Anodic degradation of CI Reactive Blue 221 using graphite and Ir O2TaO2RuO2coated titanium electrodes[J]. Industrial and Engineering Chemistry Research,2009,48(4):2149-2156.