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微波诱导催化氧化降解染料废水的研究重庆大学硕士学位论文（学术学位）学生姓名：汪春燕指导教师：汪昆平副教授专业：环境工程学科门类：工学重庆大学城市建设与环境工程学院二O一二年五月StudyontheMicrowaveInducedCatalyticOxidationofDyeWastewaterAThesisSubmittedtoChongqingUniversityinPartialFulfillmentoftheRequirementfortheMaster’sDegreeofEngineeringByWangchunyanSupervisedbyAss.Prof.WangKunpingMajor:EnviornmentEngineeringFacultyofUrbanConstructionandEnvironmentalEngineering,ChongqingUniversity,Chongqing,ChinaMay,2012中文摘要I摘要针对染料废水排放量大、有机物含量高、色度深、难降解、处理耗资大等情况，以阳离子偶氮染料酸性红B和阳离子碱性品红为目标污染物，以改性颗粒活性炭为载体，制备金属离子负载型催化剂，采用批式实验，研究了其微波诱导催化氧化降解的特征及规律。通过条件试验、正交试验、对比试验、重复试验和动力学试验分别探讨了催化剂载体制备条件、催化剂种类选取，两种染料的最佳处理实验条件、动力学特性以及反应体系中ORP变化规律等。通过催化剂表征试验得出：载体微波改性条件对载体表面官能团的种类影响不大，对总含氧官能团所占比例影响较大，载体比表面积越大越有利于染料的降解。载体预处理条件对染料降解影响不大，催化剂的种类对染料降解影响较大。通过单因素试验得出：对于酸性红B模拟染料废水，最佳处理条件为：初始pH值3、催化剂Fe3+-Cu2+/AC投加量1000mg/L、H2O2投加量101.1mg/L、微波功率300w，辐射5min后酸性红B的去除率超过99%。对于碱性品红模拟染料废水，最佳处理条件为：初始pH值2.5、催化剂投加量1000mg/L、H2O2投加量67.4mg/L、微波功率300w，辐射7min后碱性品红去除率超过94%。通过正交试验得出：影响酸性红B和碱性品红降解因素的主次顺序分别为：微波辐射时间微波功率过氧化氢投加量；微波功率微波辐射时间过氧化氢投加量。通过对比试验得出：微波诱导催化氧化降解水中染料效果最好。催化剂重复使用试验得出：催化剂使用10次后，对两种模拟染料废水的去除率仍超过90%。体系微波辐射期间，溶液ORP与染料降解反应速率不存在对应关系，体系ORP不是影响染料降解反应速率的关键因素，非均相催化性质发挥着重要作用。体系微波辐射停止后，溶液ORP变化与染料降解反应速率存在对应关系，随着反应的进行染料浓度缓慢减少，ORP缓慢上升，染料的降解决定于溶液中的氧化性物质。“微波/催化剂/H2O2”体系降解酸性红B和碱性品红均符合一级动力学模型dC/dt=-k(C-Ce)，反应速率常数分别为0.63min-1和0.47min-1。本研究通过考察实验条件对反应过程的影响、不同反应体系对目标染料的降解及其动力学过程特点，认识和揭示了微波诱导催化氧化降解水中酸性红B和碱性品红的规律，为解决印染废水处理中催化剂回收、二次污染问题以及高效经济处理印染废水提供技术支持和参考。关键词：微波催化氧化，酸性红B，碱性品红，ORP，动力学重庆大学硕士学位论文II英文摘要IIIABSTRACTBasingonthesituationofdyewastewater:largedischarge,highorganicmattercontents,deepcoloranddifficulttodegrade,processingcostetc.WithCationicazodyeacidredBandcationicbasicfuchsinastargetpollutants,withmodifiedgranularactivatedcarbonascarriertopreparemetalioncatalyst.Usingbatchexperimentstostudythecharacteristicsandlawsofmicrowaveinducedcatalyticoxidationdegradation.Throughconditionaltest,orthogonaltest,comparisontest,repeatedtestanddynamictestdiscussedcatalystcarrierpreparationcondition,catalystslection,thebesttreatmentconditionsoftwokindsofdye,anddynamiccharacteristicandrulesofORPvariations.Throughthecatalystcharacterizationtests:thelargercarrierspecificsurfaceareawas,thehigherdye’sdegradationrate.Microwavemodificationconditionshadlittleeffectonsurfacefunctionalgroupsspecies.But,hadobviouseffectontheproportionoftotaloxygenfunctionalgroups,whichwerecorrespondingtotheireffectondegradiationofdye.Throughthesinglefactorexperiments:ForacidredB,theoptimalprocessingconditionswere:initialpHvaluewas3,thedosageofcatalystFe3+-Cu2+/ACwas1000mg/L,H2O2dosagewas101.1mg/L,themicrowavepowerwas300w,after5min’sirradiation,acidredBremovalratewasover99%.Forbasicfuchsin,theoptimalprocessingconditionswere:initialpHvaluewas2.5,catalystdosagewas1000mg/L,H2O2dosagewas67.4mg/L,themicrowavepowerwas300w,after7min’sirradiation,basicfuchsinremovalratewasover94%.Throughthecontrastexperiment:microwaveoncatalyticoxidationdegradationofsimulateddyewastewaterwasnecessary.Throughthecatalystreusetests:after10timesreused,theremovalrateofsimulateddyewastewater,wasstillover90%.Throughorthogonalexperimentsobtained:theorderoffactorsinfectdegradiationofacidredBandbasicfuchsinrespectivelywere:irradiationtimemicrowavepowerH2O2dosageandmicrowavepowerirradiationtimeH2O2dosage.Duringthereactionofmicrowaveirradiationsystem,therewasnocorrespondingrelationshipbetweenreactionrateofdyeandsolutionORP.Thedegradationoccuredonthesolid-liquidinterfacebetweencatalystandsolution,degradationdependsoncatalystsurfaceproperties.Afterthereactionofmicrowaveirradiation,therewasgood重庆大学硕士学位论文IVcorrespondingrelationshipbetweendye’sdegradiationandsolutionORP.Whenthereactionprogressed,thedyeconcentrationdecreasedandsolutionORPincreasedslowly,thedegradationdependsontheoxidizingspeciesofthesolution.Inthesystemof“microwave/catalyst/H2O2”,thedegradationofacidredBandbasicfuchsinconformedfirst-orderreactionkineticsmodeldC/dt=-k(C-Ce),reactioncoefficientwere0.63min-1and0.47min-1.Thisstudyinvestigatedtheeffectsofexperimentalconditionsonthereactionprocess,thedifferentreactionsystemsfordegradationofdyewastewaterandthecharacteristicsofkineticsprocess.UnderstandedandrevealedthelawsofmicrowaveinducedcatalyticoxidationdegradationofacidredBandbasicfuchsin.Suppliedefficientlyandeconomicaltreatmentofdyewastewaterwithtechnologysupportandreference.Alsosuppliedatechnologytosolvetheproblemofcatalystrecoveryandmetalionsecondpollution.Keywords:MicrowaveCatalyticOxidation,AcidRedB,BasicFuchsin,ORP,Dynamics目录V目录中文摘要..........................................................................................................................................I英文摘要.......................................................................................................................................III1引言.........................................................................................................................................91.1课题研究背景和意义...........................................................................................................91.2目标染料废