低强度超声波对残留H_2O_2的去除
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摘要
化学需氧量(COD)会受到来自众多高级氧化技术中添加的过氧化氢(H_2O_2)的干扰。为了评估低强度超声波辐射结合清除剂(Na_2CO_3或Na HCO_3)分解水样中残留H_2O_2的可行性,对去离子水、葡萄糖模拟废水和印染废水二级处理出水进行超声(超声波频率为39 k Hz,功率分别为75 W、112.5 W和150 W)处理,H_2O_2质量浓度为20 mg/L,时间为60 min或80 min,清除剂用量为50 g/L。以20 min的间隔测定H_2O_2质量浓度和COD。结果表明,COD与H_2O_2质量浓度的比值取决于废水的性质,去离子水、葡萄糖模拟废水和印染废水二级处理出水的比值分别为0.262 6 mg COD/mg H_2O_2、0.209 9 mg COD/mg H_2O_2、0.401 3 mg COD/mg H_2O_2。超声辐照对去除H_2O_2有一定的影响,但在去离子水中超声功率为150 W、60 min时的去除率最高,仅为18.1%。超声辐照联合清除剂Na_2CO_3或Na HCO_3的效果更显著。对于印染废水二次处理出水,加入Na HCO_3作为羟自由基清除剂,80 min时H_2O_2去除率达到97.3%。然而,由于Na HCO_3和H_2O_2形成的高度氧化的超氧离子能降解废水中的有机物质,水样的实际COD降低。用超声辐射结合Na_2CO_3处理80 min,将COD的测定值与通过COD、H_2O_2质量浓度比值得到的计算值进行比较,以确认经超声波联合Na_2CO_3处理的印染废水二级处理出水中的有机物未降解。研究表明,超声波照射与Na_2CO_3结合去除水样中的低浓度H_2O_2是可行的。
The residual of strong oxidant such as hydrogen peroxide(H_2O_2)in treated wastewater is an inevitable interference to chemical oxygen demand(COD)measurement.However,although several methods have been reported,there is no simple and effective method available to address this problem.Thus,in this study,ultrasonic irradiation with low intensity was used to compose the residual H_2O_2in a simple and efficient way.Deionized water,simulated wastewater containing glucose as carbon source,and secondary effluent from treated dyeing wastewater were chosen as the model wastewater.The decomposition of residual H_2O_2through ultrasonic irradiation at 39 k Hz with power input of 75 W,112.5 W and 150 W was investigated.In addition,Na_2CO_3and Na HCO_3were used as scavenging agent.The results show that the interference value of H_2O_2on COD measurement depended on the kinds of wastewater,which equal to 0.262 6 mg COD/mg H_2O_2,0.209 9 mg COD/mg H_2O_2,0.401 3 mg COD/mg H_2O_2in deionized water,simulated wastewater containing glucose as carbon source,and secondary effluent from treated dyeing wastewater,respectively.Further,it was found that Na HCO_3was an activator for H_2O_2to generate active oxygen species superoxide ion(·O_2~-),which would degrade the organic pollutants in wastewater and then have negative effect on COD measurement.Thus,Na_2CO_3was chosen as the suitable scavenging agent,although its scavenge efficiency was lower than that of Na HCO_3.Under optimal conditions,which the ultrasonic irradiation was at 39 k Hz with power input of 112.5 W,more than 87%of H_2O_2in secondary effluent from treated dyeing wastewater was composed after 80 min of irradiation in the presence of 50 g/L Na_2CO_3.Meanwhile,the organic pollutant in secondary effluent from treated dyeing wastewater was stable after the low intensity ultrasonic irradiation.We hope that this simple and effective method can be available to avoid the oxidant interference on COD measurement in practical applications.
The residual of strong oxidant such as hydrogen peroxide(H_2O_2)in treated wastewater is an inevitable interference to chemical oxygen demand(COD)measurement.However,although several methods have been reported,there is no simple and effective method available to address this problem.Thus,in this study,ultrasonic irradiation with low intensity was used to compose the residual H_2O_2in a simple and efficient way.Deionized water,simulated wastewater containing glucose as carbon source,and secondary effluent from treated dyeing wastewater were chosen as the model wastewater.The decomposition of residual H_2O_2through ultrasonic irradiation at 39 k Hz with power input of 75 W,112.5 W and 150 W was investigated.In addition,Na_2CO_3and Na HCO_3were used as scavenging agent.The results show that the interference value of H_2O_2on COD measurement depended on the kinds of wastewater,which equal to 0.262 6 mg COD/mg H_2O_2,0.209 9 mg COD/mg H_2O_2,0.401 3 mg COD/mg H_2O_2in deionized water,simulated wastewater containing glucose as carbon source,and secondary effluent from treated dyeing wastewater,respectively.Further,it was found that Na HCO_3was an activator for H_2O_2to generate active oxygen species superoxide ion(·O_2~-),which would degrade the organic pollutants in wastewater and then have negative effect on COD measurement.Thus,Na_2CO_3was chosen as the suitable scavenging agent,although its scavenge efficiency was lower than that of Na HCO_3.Under optimal conditions,which the ultrasonic irradiation was at 39 k Hz with power input of 112.5 W,more than 87%of H_2O_2in secondary effluent from treated dyeing wastewater was composed after 80 min of irradiation in the presence of 50 g/L Na_2CO_3.Meanwhile,the organic pollutant in secondary effluent from treated dyeing wastewater was stable after the low intensity ultrasonic irradiation.We hope that this simple and effective method can be available to avoid the oxidant interference on COD measurement in practical applications.
引文
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[8]LI Jinlian(李金莲),JIN Yonghui(金永辉),LI Hui(李会).Elimination of the disturbing on COD measurement in degradation of hydrolyze polyacrylamide by Fenton[J].Chemical Engineering of Oil and Gas(石油与天然气化工),2006,35(4):316-318.
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[11]LIU Shengbao(刘生宝),LIU Fen(刘芬),LAN Mingju(蓝明菊).Interference and elimination of residual components on the standard COD test in Fenton technology[J].Contemporary Chemical Industry(当代化工),2016,45(6):1152-1155.
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[13]CHENG Z L,LUO D,DAI M X,et al.Sonophotocatalytic degradation and mineralization of bisphenol A in a sequential ultrasound intensified photocatalytic reactor[J].Properties and Testing Techniques of Inorganic Materials,2016,680:538-542.
[14]WANG Zhengfan.Contrast studies of ultrasonic degradation rhodamine B and methyl orange dynamics[J].Biotechnology,Chemical and Materials Engineering II,2013,641/642(1):113-116.
[15]TIANG Xin(唐欣),QIAO Sen(乔森),ZHOU Jiti(周集体).Influence of the low intensity ultrasound on the activity of the partial nitrification sludge[J].Journal of Safety and Environment(安全与环境学报),2017,17(1):267-272.
[16]XIE Min(谢敏),WANG Cheng(王成),XU Yao(徐瑶),et al.Impact of the ultrasonic lysis pretreatment on the dissolved substances and sludge fracture composition[J].Journal of Safety and Environment(安全与环境学报),2017,17(6):2248-2352.
[17]HJ 738—2015 Ambient air—determination of nitrobenzenes—gas chromatography(环境空气——硝基苯类化合物的测定——气相色谱法)[S].
[18]HJ 828—2017 Water quality—determination of chemical oxygen demand—potassium dichromate method(水质——化学需氧量的测定——重铬酸盐法)[S].
[19]XI Wei(郗伟),LI Xinping(李新平).Contrastive analysis of 3methods for determining H2O2content[J].Paper and Paper Making(纸和造纸),2008,27(2):75-77.
[20]SHEMER H,NARKIS N.Trihalomethanes aqueous solutions sono-oxidation[J].Water Research,2005,39(21):2704-2710.
[21]FUNG P C,POON C S,CHU C W,et al.Degradation kinetics of reactive dye by UV/H2O2/US process under continuous mode operation[J].Water Science and Technology,2001,44(6):67-72.
[22]WU C D,LIU X H,WEI D B,et al.Photosonochemical degradation of phenol in water[J].Water Research,2001,35(16):3927-3933.
[23]LIM M,SON Y,KHIM J.The effects of hydrogen peroxide on the sonochemical degradation of phenol and bisphenol A[J].Ultrasonics Sonochemistry,2014,21(6):1976-1981.
[24]SUESS H U,KRONIS J D.Impact of carbonate ions on H2O2performance in pulp bleaching[C]//Proc of International Pulp Bleaching Conference.Portland,OR:Poster Session,2002:105-119.
[25]SUESS H U,JANIK M.On the decomposition of hydrogen peroxide via the peroxocarbonic acid anion[EB/OL].[2009-04-11].http://www.tappsa.co.za/technical_articles.
[26]JIA Weiguo(贾卫国),ZHANG Peng(张鹏),LIU Zhenrong(刘振荣),et al.Research and application of ultrasound chemistry[J].Journal of Liaoning University(辽宁大学学报),2002,29(3):198-202.
[27]XU A H,LI X X,XIONG H,et al.Efficient degradation of organic pollutants in aqueous solution with bicarbonate-activated hydrogen peroxide[J].Chemosphere,2011,82(8):1190-1195.
[2]MODRZEJEWSKA B,GUWY A,DINSDALE J R,et al.Measurement of hydrogen peroxide in an advanced oxidation process using an automated biosensor[J].Water Research,2007,41(1):260-268.
[3]WU T T,ENGLEHARDT J D.A new method for removal of hydrogen peroxide interference in the analysis of chemical oxygen demand[J].Environmental Science&Technology,2012,46(4):2291-2298.
[4]TALINLI I,ANDERSON G K.Interference of hydrogen peroxide on the standard COD test[J].Water Research,1992,26(11):107-110.
[5]KUO W K.Decolorizing dye wastewater with Fenton’s reagent[J].Water Research,1992,26(7):881-886.
[6]KANG Y,CHO M J,HWANG K Y.Correction of hydrogen peroxide interference on standard chemical oxygen demand test[J].Water Research,1999,33(5):1247-1251.
[7]LEE E,LEE H,KIM Y K,et al.Hydrogen peroxide interference in chemical oxygen demand during ozone based advance oxidation of anaerobically digested livestock wastewater[J].International Journal of Environmental Science and Technology,2011,8(2):381-388.
[8]LI Jinlian(李金莲),JIN Yonghui(金永辉),LI Hui(李会).Elimination of the disturbing on COD measurement in degradation of hydrolyze polyacrylamide by Fenton[J].Chemical Engineering of Oil and Gas(石油与天然气化工),2006,35(4):316-318.
[9]LIU Junxia(刘君侠),LIU Qiongyu(刘琼玉).Interference and removal method of H2O2in COD determinations[J].Journal of Jianghan University:Natural Sciences(江汉大学学报:自然科学版),2010,38(6):46-48.
[10]WANG Yalin(王亚林),XU Qianqian(徐乾前),ZHANG Qinqin(章琴琴).Study on the interference of H2O2on COD test and the correction method[J].Environmental Pollution&Control(环境污染与防治),2012,34(12):52-60.
[11]LIU Shengbao(刘生宝),LIU Fen(刘芬),LAN Mingju(蓝明菊).Interference and elimination of residual components on the standard COD test in Fenton technology[J].Contemporary Chemical Industry(当代化工),2016,45(6):1152-1155.
[12]RICHARDS W T,LOOMIS A L.The chemical effects of high-frequency sound waves:I.A preliminary survey[J].Journal of the American Chemical Society,1927,49:3086-3100.
[13]CHENG Z L,LUO D,DAI M X,et al.Sonophotocatalytic degradation and mineralization of bisphenol A in a sequential ultrasound intensified photocatalytic reactor[J].Properties and Testing Techniques of Inorganic Materials,2016,680:538-542.
[14]WANG Zhengfan.Contrast studies of ultrasonic degradation rhodamine B and methyl orange dynamics[J].Biotechnology,Chemical and Materials Engineering II,2013,641/642(1):113-116.
[15]TIANG Xin(唐欣),QIAO Sen(乔森),ZHOU Jiti(周集体).Influence of the low intensity ultrasound on the activity of the partial nitrification sludge[J].Journal of Safety and Environment(安全与环境学报),2017,17(1):267-272.
[16]XIE Min(谢敏),WANG Cheng(王成),XU Yao(徐瑶),et al.Impact of the ultrasonic lysis pretreatment on the dissolved substances and sludge fracture composition[J].Journal of Safety and Environment(安全与环境学报),2017,17(6):2248-2352.
[17]HJ 738—2015 Ambient air—determination of nitrobenzenes—gas chromatography(环境空气——硝基苯类化合物的测定——气相色谱法)[S].
[18]HJ 828—2017 Water quality—determination of chemical oxygen demand—potassium dichromate method(水质——化学需氧量的测定——重铬酸盐法)[S].
[19]XI Wei(郗伟),LI Xinping(李新平).Contrastive analysis of 3methods for determining H2O2content[J].Paper and Paper Making(纸和造纸),2008,27(2):75-77.
[20]SHEMER H,NARKIS N.Trihalomethanes aqueous solutions sono-oxidation[J].Water Research,2005,39(21):2704-2710.
[21]FUNG P C,POON C S,CHU C W,et al.Degradation kinetics of reactive dye by UV/H2O2/US process under continuous mode operation[J].Water Science and Technology,2001,44(6):67-72.
[22]WU C D,LIU X H,WEI D B,et al.Photosonochemical degradation of phenol in water[J].Water Research,2001,35(16):3927-3933.
[23]LIM M,SON Y,KHIM J.The effects of hydrogen peroxide on the sonochemical degradation of phenol and bisphenol A[J].Ultrasonics Sonochemistry,2014,21(6):1976-1981.
[24]SUESS H U,KRONIS J D.Impact of carbonate ions on H2O2performance in pulp bleaching[C]//Proc of International Pulp Bleaching Conference.Portland,OR:Poster Session,2002:105-119.
[25]SUESS H U,JANIK M.On the decomposition of hydrogen peroxide via the peroxocarbonic acid anion[EB/OL].[2009-04-11].http://www.tappsa.co.za/technical_articles.
[26]JIA Weiguo(贾卫国),ZHANG Peng(张鹏),LIU Zhenrong(刘振荣),et al.Research and application of ultrasound chemistry[J].Journal of Liaoning University(辽宁大学学报),2002,29(3):198-202.
[27]XU A H,LI X X,XIONG H,et al.Efficient degradation of organic pollutants in aqueous solution with bicarbonate-activated hydrogen peroxide[J].Chemosphere,2011,82(8):1190-1195.