脉冲放电等离子体/活性炭协同降解染料废水及过氧化氢的生成
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- 英文论文题名：Production of Hydrogen Peroxide and Degradation of Dye Wastewater by Pulsed Discharge Plasma Combined with Activated Carbon
- 论文作者：郭贺 ; 王慧娟 ; 杨文明 ; 李洋 ; 依成武
- 英文论文作者：GUO He ; WANG Huijuan ; YANG Wenming ; LI Yang ; YI Chengwu ; School of the Environment and Safety Engineering ; Jiangsu University ; School of Material Science and Engineering ; Jiangsu University
- 年：2015
- 作者机构：江苏大学环境与安全工程学院;江苏大学材料科学与工程学院;
- 论文关键词：脉冲放电等离子体 ; 活性炭 ; 酸性橙II ; 协同脱色 ; 过氧化氢
- 英文论文关键词：pulsed discharge plasma ; activated carbon ; acid orange 7 ; synergistic decoloration ; hydrogen peroxide
- 会议召开时间：2015-08-12
- 会议录名称：静电放电：从地面新技术应用到空间卫星安全防护—中国物理学会第二十届全国静电学术会议论文集
- 语种：中文
- 分类号：X788;O539;TQ123.6
- 学会代码：WLJD
- 会议名称：静电放电 ; 从地面新技术应用到空间卫星安全防护—中国物理学会第二十届全国静电学术会议
- 会议地点：中国河北石家庄
- 主办单位：中国物理学会静电专业委员会
- 学会名称：中国物理学会静电专业委员会
- 页数：7
- 文件大小：712k
- 原文格式：D
- 会议级别：全国
摘要
为了提高脉冲放电等离子体(pulsed discharge plasma,PDP)对染料废水的降解效果,以酸性橙Ⅱ(acid orange,AO7)作为目标污染物,建立多针-板电极形式的PDP与活性炭(activated carbon,AC)相联合的循环脱色体系。考察PDP/AC协同体系中,AC的添加、AC粒径、电极间距、溶液pH、载气种类、载气量等关键参数对AO7降解效果的影响,同时考察相同操作参数条件下,以去离子水为介质放电60min后,PDP/AC协同体系中过氧化氢(hydrogen peroxide,H_2O_2)的生成浓度,以说明各参数变化对系统活性物种浓度的影响。研究结果表明:PDP/AC联合体系降解AO7废水的效果优于单独PDP体系;粒径为1-2mm的AC添加更有利于AO7降解,降解效率可以提高20.4%,但此时AC损耗较大;同时,PDP/AC联合体系所产生H_2O_2量高于单独PDP体系H_2O_2生成量,且粒径为1-2 mm的AC添加体系中可以产生更多的H_2O_2;1.5 cm较0.8 cm的电极间距不利于系统中AO7的降解和H_2O_2的生成;酸性溶液条件下AO7降解率较高且相应产生的H_2O_2浓度较高;载氧气流速为2L/min时,AO7降解效果最佳,降解率可达到81.5%,该条件下水溶液中H_2O_2的生成量可达0.5316mmol·L~(-1)。
In order to improve the degradation efficiency of dye wastewater by pulsed discharge plasma(PDP),a cyclic synergistic decoloration system of PDP with a multi-needle-to-plate geometry electrode combined with activated carbon(AC) was established in this paper.Acid Orange 7(AO7) was chosen as the typical pollutant,the influences of many critical parameters in the system,including particle size of AC,electrode distance,solution pH,varieties and bubbling rate of gas,on degradation efficiency of AO7 were investigated.The formation of hydrogen peroxide(H_2O_2)in deionized water after 60 min discharge under the same reaction condition was also reviewed to illustrate the effect of different parameters on active species formation in the synergistic system.The obtained results show that degradation of AO7 in the combined system of PDP and AC was better than that in the sole PDP system;the AC with 1-2 mm particle size was more favorable for AO7 degradation than that of the AC with 2-3 mm size,but the carbon loss was higher in the case of 1-2 mm AC addition;the production of H_2O_2 in the PDP/AC system was higher than that in the sole PDP system,and the production of H_2O_2 in the synergistic system with l-2mm AC addition was also higher than that in the system with 2-3 mm AC addition;compared to 15 mm electrode distance,the degradation of AO7 was higher under the condition of 8 mm electrode distance and the generated H_2O_2 concentration was higher;the acidic solution was benefit for AO7 degradation and H_2O_2 formation in the synergistic system;under the condition of 2 L/min oxygen bubbling rate,the degradation of AO7 in the synergistic system achieved was 81.5%and H_2O_2 concentration was 0.5316 mmol·L~(-1).
In order to improve the degradation efficiency of dye wastewater by pulsed discharge plasma(PDP),a cyclic synergistic decoloration system of PDP with a multi-needle-to-plate geometry electrode combined with activated carbon(AC) was established in this paper.Acid Orange 7(AO7) was chosen as the typical pollutant,the influences of many critical parameters in the system,including particle size of AC,electrode distance,solution pH,varieties and bubbling rate of gas,on degradation efficiency of AO7 were investigated.The formation of hydrogen peroxide(H_2O_2)in deionized water after 60 min discharge under the same reaction condition was also reviewed to illustrate the effect of different parameters on active species formation in the synergistic system.The obtained results show that degradation of AO7 in the combined system of PDP and AC was better than that in the sole PDP system;the AC with 1-2 mm particle size was more favorable for AO7 degradation than that of the AC with 2-3 mm size,but the carbon loss was higher in the case of 1-2 mm AC addition;the production of H_2O_2 in the PDP/AC system was higher than that in the sole PDP system,and the production of H_2O_2 in the synergistic system with l-2mm AC addition was also higher than that in the system with 2-3 mm AC addition;compared to 15 mm electrode distance,the degradation of AO7 was higher under the condition of 8 mm electrode distance and the generated H_2O_2 concentration was higher;the acidic solution was benefit for AO7 degradation and H_2O_2 formation in the synergistic system;under the condition of 2 L/min oxygen bubbling rate,the degradation of AO7 in the synergistic system achieved was 81.5%and H_2O_2 concentration was 0.5316 mmol·L~(-1).
引文
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[15]ZHANG Yanzong,ZHENG Jingtang,QUXiangfeng,et al.Effect of granular activated carbon on degradation of methyl orange when applied in combination with high-voltage pulse discharge[J].Journal of colloid and interface science,2007,316(2):523-530.
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[27]曹志荣.DBD等离子体-活性炭联用降解碱性品红的实验研究[D].南昌大学,2011.CAO Zhirong.Experimental research on the degradation of basic fuchsin with DBD plasma-activated carbon[D].Nanchang University,2011.
[28]Zhang Xingwang,Zhou Minghua I,Lei Leicheng.Preparation of photocatalytic Ti O2 coatings of nanosized particles on activated carbon by AP-MOCVD[J].Carbon,2005,43(8):1700-1708.
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[30]Wen Yuezhong,Jiang Xuanzhen.Pulsed corona discharge-induced reactions of acetophenone in water[J].Plasma Chemistry and Plasma Processing,2001,21(3):345-354.
[2]杨威,孔德骞,车春波,等.Fenton试剂对染料废水的降解脱色作用研究[J].化学与粘合,2009,31(04):15-17.YANG Wei,KONG Deqian,CHE Chunbo,et al.Research on treating dye wastewater by Fenton reagent[J].Chemistry and Adhesion,2009,31(04):15-17.
[3]陈长琦,岑科达,殷福才,等.酸性大红GR染料废水超声降解的实验研究[J].安徽化工,2007,33(01):50-53.CHEN Changqi,CEN Keda,YIN Fucai,et al.Research on ultrasonic dgradation of acid brilliant scarlet GR dye wastewater[J].Anhui Chemical Industry,2007,33(01):50-53.
[4]徐瑞银,王殿芳,王禹,等.用于染料废水光降解处理的催化剂及其作用机制[J].北京石油化工学院学报,2004,12(2):26-31.XU Ruiyin,WANG Dianfang,WANG Yu,et al.Catalysts for photodegradation of dye wastewater and their reaction mechanism[J].Journal of Beijing Institute of Petro-chemical Technology,2004,12(2):26-31.
[5]雷乐成,汪大辉.湿式氧化法处理高浓度活性染料废水[J].中国环境科学,1999,19(1):43-47.LEI Lecheng,WANG Da Hui.Wet oxidation of high concentration reactive dyes wastewater[J].China Environmental Science,1999,19(1):43-47.
[6]李善评,姜艳艳,阴文杰,等.低温等离子体处理次甲基蓝染料废水实验[J].实验室研究与探索,2013,32(2):17-20.LI Shanping,JIANG Yanyan,YIN Wenjie,et al.Degradation of methyllene blue dye wastewater by low-temperature plasma[J].Research and Exploration in Laboratory,2013,32(2):17-20.
[7]Sugiarto A T,Ito S,Ohshima T,et al.Oxidative decoloration of dyes by pulsed discharge plasma in water[J].Journal of Electrostatics,2003,58(1):135-145.
[8]Zhang Ruobing,Zhang Chi,Cheng Xingxin,et al.Kinetics of decolorization of azo dye by bipolar pulsed barrier discharge in a three-phase discharge plasma reactor[J].Journal of Hazardous materials,2007,142(1):105-110.
[9]王慧娟,李杰,全燮.高压脉冲放电等离子体处理酸性橙Ⅱ染料废水的实验研究[J].北京理工大学学报,2005,25(S1):222-225.Wang Huijuan,LI Jie,QUAN Xie.Deeoloration of acid orange7 dye aqueous solution by a multi-needle-to-plate high voltage pulsed diseharge plasma system[J].Transactions of Beijing Institute of Technology,2005,25(S1):222-225.
[10]李月生.脉冲放电等离子体处理染料废水的实验研究[D].江西理工大学,2007.LI Yuesheng.Experimental research on dye wastewater treatment with pulsed discharge plasma[D].Jiangxi University of Science and Technology,2007.
[11]李凤镱,谭君山.活性炭吸附法处理染料废水研究的进展概况[J].广州环境科学,2010,25(01):5-8.LI Fengyi,TAN Junshan.Development in research on dye wastewater treatment with activated carbon[J].Guangzhou Environmental sciences,2010,25(01):5-8
[12]张小璇.染料废水的活性炭吸附及其热再生研究[D].厦门大学,2005.ZHANG Xiaoxuan.Adsorption and regeneration dye wastewater of activated carbon in treatment.Xiamen university,2005.
[13]Malik P K.Dye removal from wastewater using activated carbon developed from sawdust:adsorption equilibrium and kinetics[J].Journal of Hazardous Materials,2004,113(1):81-88.
[14]ZHANG Yanzong,SUN Bing,DENG Shihuai,et al.Methyl orange degradation by pulsed discharge in the presence of activated carbon fibers[J].Chemical Engineering Journal,2010,159(1):47-52.
[15]ZHANG Yanzong,ZHENG Jingtang,QUXiangfeng,et al.Effect of granular activated carbon on degradation of methyl orange when applied in combination with high-voltage pulse discharge[J].Journal of colloid and interface science,2007,316(2):523-530.
[16]Grymonpre D R,Finney W C,Locke B R.Aqueous-phase pulsed streamer corona reactor using suspended activated carbon particles for phenol oxidation:model-data comparison[J].Chemical Engineering Science,1999,54(15):3095-3105.
[17]Valdés H,Zaror C A.Ozonation of benzothiazole saturated-activated carbons:influence of carbon chemical surface properties[J].Journal of hazardous materials,2006,137(2):1042-1048.
[18]杨彬.高压脉冲放电降解染料废水的研究[D].浙江大学,2004.YANG Bin.Degradation of dyes in aqueous solution using high-voltage pulsed discharges.Zhengjiang University.2004.
[19]Locke B R,Sato M,Sunka P,et al.Electrohydraulic discharge and nonthermal plasma for water treatment[J].Industrial&engineering chemistry research,2006,45(3):882-905.
[20]Sun B,Sato M,Clements J S.Oxidative processes occurring when pulsed high voltage discharges degrade phenol in aqueous solution[J].Environmental science&technology,2000,34(3)509-513.
[21]Sun B,Sato M,Clements J S.Optical study of active species produced by a pulsed streamer corona discharge in water[J].Journal of Electrostatics,1997,39(3):189-202.
[22]Sugiarto A T,Sato M.Pulsed plasma processing of organic compounds in aqueous solution[J].Thin solid films,2001,386(2):295-299.
[23]Yan J H,Liu Y N,Bo Z,et al.Degradation of gas-liquid gliding arc discharge on acid orange II[J].Journal of Hazardous Materials,2008,157(2/3):441-447.
[24]Sánchez-Polo M,Von Gunten U,Rivera-Utrilla J.Efficiency of activated carbon to transform ozone into OH radicals:influence of operational parameters[J].Water research,2005,39(14):3189-3198.
[25]Beltrán F J,Rivas J,Alvarez P,et al.Kinetics of heterogeneous catalytic ozone decomposition in water on an activated carbon[J].Ozone:science&engineering,2002,24(4):227-237.
[26]Wang Huijuan,Li Jie,Quan Xie,et al.Formation of hydrogen peroxide and degradation of phenol in synergistic system of pulsed corona discharge combined with Ti O2 photocatalysis[J].Journal of hazardous materials,2007,141(1):336-343.
[27]曹志荣.DBD等离子体-活性炭联用降解碱性品红的实验研究[D].南昌大学,2011.CAO Zhirong.Experimental research on the degradation of basic fuchsin with DBD plasma-activated carbon[D].Nanchang University,2011.
[28]Zhang Xingwang,Zhou Minghua I,Lei Leicheng.Preparation of photocatalytic Ti O2 coatings of nanosized particles on activated carbon by AP-MOCVD[J].Carbon,2005,43(8):1700-1708.
[29]Mukkavilli S,Lee C K,Varghese K,et al.Modeling of the electrostatic corona discharge reactor[J].Plasma Science,IEEETransactions on,1988,16(6):652-660.
[30]Wen Yuezhong,Jiang Xuanzhen.Pulsed corona discharge-induced reactions of acetophenone in water[J].Plasma Chemistry and Plasma Processing,2001,21(3):345-354.