粉煤灰负载Fe3非均相光催化降解苯酚研究朱莹佳

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[](07SL011008)ImmobilizedFe3+-flyash:anefficientheterogeneousphoto-FentonoxidationcatalystforthedegradationofphenolZhuYingjia1,2,XiaoYutang1,2,YinYuling1,GaoGuandao1(1.KeyLaboratoryofTianjinMunicipalEcologicalEnvironmentRemedyandPollutionControl,SchoolofEnvironmentalScience&Engineering,NankaiUniversity,Tianjin300071,China;2.NationalKeyLaboratoryofNanjingInstiuteofGeography&Limnology,ChineseAcademyofSciences,Nanjing210008,China)Fe3+1,2,1,2,1,1(1.,,300071;2.,,210008)[]Fe3+,UV/Fenton,,、、H2O2pH,。:Fe-A1,pH3,H2O25.0mmol/L,0.2g/L,500mL100mg/L,60min95%,3,60min93%。[];UV/Fenton;;[]X703.1[]A[]1005-829X(2009)08-0028-04Abstract:HeterogeneouscatalysthasbeenpreparedwithflyashloadedwithFe3+,anditseffectonthedegradationofphenolinUV/Fentonhasbeenstudied.Theeffectsofthepreparationmethodonitscatalyzingefficiencyandsta-bilityarediscussed.Furthermore,theeffectsofitsreactionsystem,loadingcapacityofFe3+,doseofH2O2,andini-tialpHonphenoldegradationefficiencyareinvestigated.Moreover,thereusabilityofthecatalystisexamined.TheexperimentalresultsshowthatcatalystFe-A1preparedbyimpregnationmethodhasbetterstabilityandcatalyzingcapacity.Thestandardconditionsareasfollows:pH=3,H2O2dosage=5.0mmol/L,andthecatalystdosage=0.2g/L,thedegradationefficiencyofphenolreachesabove95%within60minfor500mLofphenolsimulatedwastewaterwithaninitialmassconcentrationof100mg/L.Afterthecatalystisreusedfor3times,thephenoldegradationeffi-ciencyisstillabove93%within60min.Keywords:catalyst;UV/Fenton;phenol;heterogeneousreaction29820098IndustrialWaterTreatmentVol.29No.8Aug.,2009、,Fenton、UV/FentonHO·,,〔1-2〕。FentonFe(),,pH,。,Fe2+/Fe3+Y、Nafion,,,〔3-5〕。,,、,、。,28——2009-08,29(8)2009-08,29(8),〔6-7〕。Fe3+,,。11.1:,60~100,;;,30%;FeCl3·6H2O、。:VIS-723G();pHS-25pH()。1.2Fe3+(1)。,5g50mL1.02gFeCl3·6H2O,110℃,Fe-A1,500℃4h。FeCl3·6H2O(Fe3+)。(2)。,5g100mL6.76gFeCl3·6H2O2.65gNa2CO3,6h,70℃1d,,,,Fe-A2。1.3UV/Fenton,,H2O2,150W,,,。,UV/Fenton:500mL100mg/L,H2O25.0mmol/L,0.2g/L,30℃,pH3。1.44-;。22.1,,,Fe3+Fe-A1Fe3+,41.3mg/g,Fe-A2Fe3+,13.1mg/g。Fe3+Fe3+,FeCl3·6H2OFe3+。,:500mL100mg/L,pH3,H2O25.0mmol/L,0.2g/L,60min。,1。1,Fe-A1Fe-A20.328mg0.115mg,Fe-A2,Fe-A1,7.93%,Fe-A1,,,Fe-A1Fenton。,Fe-A1、Fe-A2(Fe3+=3.78mg/g),,,0.10、0.32、1.00g。1。Fe2O3,Fe2+H2O2Fenton,,60min42%,Fe3+Fe-A1Fe-A2,Fe-A1Fe-A2,,0.10gFe-A130min90%。10080604020010203040506070/minFe-Al(0.10g)Fe-A2(0.32g)(1.00g)/(mg·L-1)11Fe3+/mg/mg/%4.130.3287.931.310.1158.75/gFe-A10.1Fe-A20.1,:Fe3+29——2009-08,29(8)2009-08,29(8),、,Fe3+Fe-A1Fe-A2,Fe-A1。2.2Fe3+UV/Fenton,4(UV、UV/Fe-A1、H2O2/Fe-A1UV/H2O2/Fe-A1),。UV/FentonUV/Fenton,,Fe-A1Fe3+。2。2,UV,,30min10%;H2O2/Fe-A1UV/Fe-A1,30min19.2%25.7%,Fe-A1Fe3+,UV/Fe-A1H2O2/Fe-A1,UV/H2O2/Fe-A1,30min91.7%,UV/Fe-A1H2O2/Fe-A1,H2O2UV/Fe-A1。Fenton,UV/Fenton,,,Fe-A1Fe3+,〔8〕,FentonHO·,。2.32.3.1H2O2H2O20.5、5.0、50.0mmol/L,,Fe-A1UV/Fen-ton。H2O2,3。3,H2O2,H2O25.0mmol/L,60min,95%,H2O250.0mmol/L,,H2O2,〔9〕,,。Fe-A1UV/FentonH2O25.0mmol/L。2.3.2Fe3+Fe3+,10.1、41.3、91.4mg/gFe-A1。,Fe-A1UV/FentonFe-A1,4。4,Fe-A1Fe3+,;41.3mg/g,Fe3+91.4mg/g,。Fe3+,Fe3+,,〔3,10〕。Fe3+,,。,Fe3+。2.3.3pH,pH12010080604020010203040506070/minFe3+10.1mg/gFe3+41.3mg/gFe3+91.4mg/g/(mg·L-1)4Fe-A1Fe3+120100806040200010203040506070/min/(mg·L-1)UVUV/Fe-A1H2O2/Fe-A1UV/H2O2/Fe-A1UV/H2O2/Fe3+212010080604020010203040506070H2O20.5mmol/LH2O25.0mmol/LH2O250.0mmol/L/min3H2O2/(mg·L-1)30——2009-08,29(8)2009-08,29(8)12010080604020010203040506070/min/(mg·L-1)1236Fe-A1,:Fe3+3、6、8,Fe-A1UV/Fenton,5。5,60min,pH397.8%,pH6,91.7%,pH8,76.8%,Fe-A1UV/FentonpH,pH〔11〕,。(pH3)Fe2+〔12〕,Fe-A1,Fe-A1pH3。2.4Fe3+,Fe-A1UV/Fenton,Fe-A1,,,6。6,3,Fe-A1,60min93.4%,,Fe3+,。3,Fe-A1,UV/Fenton,,FentonpH。100mg/L,H2O25.0mmol/L,0.2g/L,pH3,60min97.8%,。[][1]GrigoropoulouH,PhilippopoulosC.Homogeneousoxidationofphe-nolsinaqueoussolutionwithhydrogenperoxideandferricions[J].WaterSci.Technol.,1997,36(2/3):151-154.[2]KangN,LeeDS,YoonJ.KineticmodelingofFentonoxidationofphenolandmonochlorophenols[J].Chemosphere,2002,47(9):915-924.[3]PhuNH,HoaTTK,TanNV,etal.Characterizationandactiv-ityofFe-ZSM-5catalystsforthetotaloxidationofphenolinaqueoussolutions[J].AppliedCatalysisB:Environmental,2001,34(4):267-275.[4]KariP,MikaS.Heterogeneouswaterphasecatalysisasanenvi-ronmentalapplication:areview[J].Chemosphere,2002,48(10):1047-1060.[5]LiouR,ChenSH,HungMY.Fe()supportedonresinasef-fectivecatalystfortheheterogeneousoxidationofphenolinaque-oussolution[J].Chemosphere,2005,59(1):117-125.[6]WangX,WuH.Environmental-benignutilisationofflyashaslow-costadsorbents[J].JournalofHazardousMaterials,2006,136(3):482-501.[7]YolandaF,RobertoF,AlbertoAG,etal.HeterogeneouscatalysisintheFenton-typesystemreactiveblack5/H2O2[J].JournalofMolecularCatalysisA:Chemical,2008,281(1/2):184-191.[8]NoorjahanM,DurgaKumariV,SubrahmanyamM,etal.Immobi-lizedFe()-HY:anefficientandstablephoto-Fentoncatalyst[J].AppliedCatalysisB:Environmental,2005,57(4):291-298.[9]CentiG,PerathonerS,TorreS,etal.CatalyticwetoxidationwithH2O2ofcarboxylicacidsonhomogeneousandheterogeneousFen-ton-typecatalysts[J].Catal.Today,2000,55(1/2):61-69.[10]KavithaV,PalaniveluK.TheroleofferrousioninFentonandphoto-Fentonprocessesfort
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