电场效应与催化湿式氧化协同作用研

©1994-2009ChinaAcademicJournalElectronicPublishingHouse.Allrightsreserved.(,200092):,Mn2Sn2Sb23P2Al2O3,.,(T=130)(pO2=110MPa),27minTOC9410%8814%.,,.:;;:X70311:A:025023301(2009)0721925206:2008210217;:2008212229:(50378066):(1966),,,,,E2mail:[e-mail]biningElectrochemicalOxidationandCatalyticWetOxidationWANGHua,LIGuang2ming,ZHANGFang,HUANGJu2wen(StateKeyLaboratoryofPollutionControlandResourcesReuse,TongjiUniversity,Shanghai200092,China)Abstract:Anewcatalyticwetoxidationfixed2bedreactorcombinedwiththree2dimensionalelectric2fieldwasdevelopedtoinvestigatecatalyticwetoxidation,electrochemicaloxidationandelectroassistedcatalyticwetoxidationofthesolutioncontainingphenolinthepresenceofacatalystMn2Sn2Sb23P2Al2O3.Goodelectroassistedcatalyticwetoxidationefficiencywasobtainedinthesetupforthecombinationsystemevenatmildconditions(T=130,pO2=110MPa)thatthephenolconversionandTOCreductionwereupto9410%and8814%after27mintreatment,respectively.Theresultalsoshowsthattherateconstantsofelectroassistedcatalyticwetoxidationaremuchhigherthanthatofnotonlybothcatalyticwetoxidationandelectrochemicaloxidationprocessalonebutalsoadditiveefficienciesofcatalyticwetoxidationandelectrochemicaloxidationprocesses,whichindicatesanapparentsynergeticeffectbetweenCWOandECOprocesses.Keywords:catalyticwetoxidation;electro2chemicaloxidation;synergy,,,,(wetoxidation,WO).(catalyticwetoxidation,CWO).,,,HO,[1,2].,[310].,,[11],,,.(ECO)(CWO)(CWOPECO),CWOECO.CWO,(),HO,,1+12,CWO,CWO.111130720097ENVIRONMENTALSCIENCEVol.30,No.7Jul.,2009©1994-2009ChinaAcademicJournalElectronicPublishingHouse.Allrightsreserved.(1014),186m2Pg,014889cm3Pg.Mn2Sn2Sb23P2Al2O32Al2O350%Mn(NO3)2(01570molPL),902h5504h;SnCl45H2O(01285molPL)+SbCl3(4138mmolPL)+HCl(015molPL)+C2H5OH,10512h5504h,Mn2Sn2Sb23P2Al2O3.1121,,,,,,;,;,,,;,,,;(),;.,H2,H2O2.Mn2Sn2Sb23P2Al2O3,1.,,,.1131.;2.;3.;4.;5.;6.;7.;8.;9.;10.;11.;12.;13.;14.;15.;16.;17.;18.;19.;20.;21.;22.;23.;24.;25.1Fig.1Experimentalset2upofelectroassisstedCWO(up2flow)629130©1994-2009ChinaAcademicJournalElectronicPublishingHouse.Allrightsreserved.(STP)PmLmin-1250Pmm1170Pg36LHSVPh-11251131142:5mgPL,015mL,,42110mL.110mL,,10min510nm.11312CODCOD.11313TOCTOC,.TOCSHIMADZUTOC2VCPN,0100mgPL.(TC),H3PO4(IC),TCIC(TOC).21301401503(ECO)(CWO)(CWOPECO),CWOECO.22500mgPL130CWOECOCWOPECO3.ECO:I=015A,T=25,pH0=615,Qg=250mLPmin(STP);CWO:T=130,pH0=615,pO2=110MPa,Qg=250mLPmin(STP);CWOPECO:I=015A,T=130,pH0=615,pO2=110MPa,Qg=250mLPmin(STP).2130CWOPECOFig.2Phenolremovalsat403Kand110MPaunderCWOPECOprocess2(a),6min,118%(ECO)418%(CWO)2412%(CWOPECO);1017min,615%(ECO)72917:©1994-2009ChinaAcademicJournalElectronicPublishingHouse.Allrightsreserved.(CWO)5819%(CWOPECO);,27min,1318%(ECO)4413%(CWO)9410%(CWOPECO).,,CWOPECO,6min2412%118%+418%;1017min5819%615%+1115%;27min9410%1318%+4413%.CWOPECO,1+12.[12],[13],3.ln(c0Pc)=kt,c0ct(mgPL),k(s-1).32.3Fig.3Phenolremovalkineticsforvariousprocesses2,CWOPECOCWOECO,kCWO2ECO,:-dRdt=kCWOPECO[R]=kCWO[R]+kECO[R]+kCWO2ECO[R],kECOkCWOkCWOPECOECOCWOCWOPECO3(s-1).CWOPECO.,2HO,HO,kCWOPECOHO(s-1).CWOPECO,SF:SF=kCWOPECOkCWO+kECOSF1,.SF,.,SF1,.2Table2Kineticregressionequationsandparametersinvariousprocesses(k)Ps-1ECOy=412610-3t019807412610-3CWOy=119410-2t019802119410-2CWOPECOy=917410-2t019930917410-22SF4112,,130CWOPECO.CWOPECO.42500mgPL140CWOECOCWOPECO3.(CWO)CWOPECO140,130.4(a),6min,118%(ECO)816%(CWO)3016%(CWOPECO);1017min,615%(ECO)2114%(CWO)6018%(CWOPECO);27min,1318%(ECO)7817%(CWO)9816%(CWOPECO).,,CWOPECO,6min3016%118%+816%;829130©1994-2009ChinaAcademicJournalElectronicPublishingHouse.Allrightsreserved.(18min)TOC,18min9816%(CWOPECO)1318%(ECO)+7817%(CWO),TOC8916%(CWOPECO)516%(ECO)+7416%(CWO).27min,9918%(CWOPECO)1318%(ECO)+9016%(CWO),TOC9314%(CWOPECO)1015%(ECO)+8311%(CWO).,150kECOkCWOkCWOPECO,412610-3816392917:©1994-2009ChinaAcademicJournalElectronicPublishingHouse.Allrightsreserved.(27min)(T=130,pO2=110MPa)TOC9410%8814%.,150,TOC9016%8311%,20.,,.3(1),(27min)(T=130,pO2=110MPa),9410%,TOC8814%.,150,TOC9016%8311%,20.(2),,,SF1304112.:[1]VittJE,JohnsonDC.TheimportanceofanodicdischargeofH2Oinacidicoxygen2transferreactions[J].JElectrochemSoc,1992,139:7742780.[2],,.[J].,2001,17(3):2632271.[3]FockedeyE,VanLierdeA.Couplingofanodicandcathodicreactionsforphenolelectro2oxidationusingthree2dimensionalelectrodes[J].WaterRes,2002,36(16):416924175.[4]SharifianH,KirkDW.Electrochemicaloxidationofphenol[J].JElectrochemSoc,1986,133(5):92129