催化湿式氧化法处理废水的研究进展

2007274ENVIRONMENTALPROTECTIONOFCHEMICALINDUSTRY[]2007-03-30;[]2007-04-05[](1978)),,,,,:010-62784527-815;:[e-mail][],:010-62784527-820;:[e-mail]1,2,1,3,1,2,4(1.,100084;2.(),100083;3.,102206;4.,100083)[](CWAO);CWAO[];;;[]X703.1[]A[]1006-1878(2007)04-0295-06AdvancesinResearchonWastewaterTreatmentbyCatalyticWetAirOxidationProcessWangJianbing1,2,YangShaoxia1,3,ZhuWanpeng1,WangWei2,LiXiang4(1.DepartmentofEnvironmentalScienceandEngineering,TsinghuaUniversity,Beijing100084,China;2.SchoolofChemicalandEnvironmentalEngineering,ChinaUniversityofMiningIndustry(BeijingCampus),Beijing100083,China;3.DepartmentofPowerEnergyEngineering,NorthChinaElectricPowerUniversity,Beijing102206,China;4.SchoolofCivilandEnvironmentalEngineering,UniversityofScienceandTechnologyBeijing,Beijing100083,China.)Abstract:Theadvancesintheresearchonwastewatertreatmentbycatalyticwetairoxidation(CWAO)processaresummarizedinaspectsofcatalystdevelopmen,treactionmechanisminvestigationandreactionkineticsstudy.Itispointedoutthatthepreparationofactiveandstablecatalysts,theinvestigationonreactionmechanismsandthestudyonreactionkineticsmodelsareveryimportantforthepromotionofCWAOapplication.Keywords:catalyticwetairoxidation;catalys;treactionmechanism;reactionkinetics,,(WAO)(120~374e)(0.5~20MPa)(),,()(CWAO)WAO,,,CWAO[1],CWAO,CWAO#295#ENVIRONMENTALPROTECTIONOFCHEMICALINDUSTRY2007271CWAO催化剂的研究进展CWAO,,,,,,1.1Cu,Mn,Co,N,iBi,,,Barbier[2]CWAO,:RuIrPdUFeUCuAgUNiUCoUCrUCeO2TiO2ZrO2,CuFeFortuny[3]Cu,CuOCWAO,5000mg/L140e0.9MPa,120min80%,CuXu[4]FeCu,Cu0.5-xFexZn0.5Al2O4CWAO,1500mg/L150e1.0MPa,120minCOD90%,FeCu8@10-6mg/LLeitenburg[5]CeO2-ZrO2-CuOCeO2-ZrO2-MnOx,,,CuMn1@10-6mg/LBeziat[6]TiO2ZrO2CeO2CWAOLin[7]CeO2,CWAO400~2500mg/L0.5~1.0MPa160e,4h90%,CO280%[8,9]CeO2-TiO2CeO2-ZrO2,:n(Zr)Bn(Ce)1B9,CWAO,5000mg/L230e5MPa,120minCOD76%,Ce2@10-7mg/L,Zr1@10-8mg/L;n(Ti)Bn(Ce)1B1,5000mg/L230e5MPa,180minCOD64%,Ce6.1@10-7mg/L,Ti5@10-8mg/L;CeTiCeZr,,,;,1.2Ru,Rh,P,tIr,Au,Ag,CWAO,Al2O3Lee[10]Pd/Al2O3,Rh/Al2O3,Ru/Al2O3,Pt-Pd/Al2O3CWAO,Pd/Al2O3,Al2O3,[11]Gallezot[12,13],CWAO:RhPdIrP,tCWAOAtwater[14]Pt1.5%Pt/CWAO,160eBeziat[6],,TiO2,CeO2,ZrO2Maugans[15]Pt4.45%Pt/TiO2CWAO,1150mg/L176e4.8MPa4g/L,30min100%Besson[16]Au/TiO2CWAO,,Pintar[17]#296#4.Ru/ZrO2Ru/TiO2CWAO,TOC665mg/L,TOC1380mg/L,190e5.5MPa,8hTOC90%,TiZrBarbier[2,18]CWAO,1%~5%RuCeO2TiO2ZrO2,Ru/CeO2Oliviero[19]Ru/CeO2Ru/C,Ru/CeO2TOCRu/C1.3(CNTs),Gomes[20],Pt,CWAO,Pt/CNTsCWAO,,2000mg/L200e0.69MPa,2h98.8%,CO286.9%CO2Garcia[21,22]Gomes,3Pt,Pt/CNTs,CWAO,2000mg/L200e0.69MPa,2h98%CWAO,,,2CWAO反应机理的研究进展CWAOWAO,WAO,WAO,,,3,Li[23]1991WAO,O#,HO#,HO2#,HO#HO2#Robert[24]WAO,5,5--1--N-(DMPO),(ESR)HO#H2O2,H2O2,CWAO(EDTA)O,C,NDelgado[25]CWAO,CWAO3,,,,,,WAO,Devlin[26]1984,,WAOCWAO,3CWAO动力学模型的研究进展,3.1CWAO,Harmsen[27]Pt/CCWAO,9,pH,Rivas[28]CWAO44,CWAO,,,O2pHH2O2,CWAOHO#PhOO#,HO2##297#ENVIRONMENTALPROTECTIONOFCHEMICALINDUSTRY2007273.2(1)CWAO-dc1dt=k0expEaRTcm1cn2(1):c1,(CODTOC);c2,DO;t,min;Ea,kJ/mo;lT,K;R,8.314J/(mol#K);m;n;k0,mn,[29,30],;,CWAO,3.3,Li[23]A,B,C3:A;B;C,CO2H2O311(2)cA+cBcA0+cB0=k2k1+k2-k3exp(-k3t)+k1-k3k1+k2-k3exp[-(k1+k2)t](2):cA,cBAB;cA0,cB0AB;k1,k2,k3,Belkacemi[31],,CWAOLarachi[32],Eftaxias[33]CuO/C-Al2O3,CWAO,CWAO,Langmuir-Hinshelwood,(3)~(5)ri=kap,iKici1+EjKjcj(3)kap=k0dexp-EaRTw8O2(4)Kj=K0jexp(-$HjRT(5):rii;kap,ii;Ki,Kjij;ci,cjij;kap;k0d,K0j;wO2;8;$Hj,kJ/molEftaxias(120~160e)(0.6~1.2MPa),Langmuir-Hinshelwood,,8%,,4结语CWAO,CWAO,;,,,CWAOCWAO,CWAO,,,,,CWAO#298#4.,1LuckF.Wetairoxidation:pas,tpresentandfuture.CatalToday,1999,53(1):81~912BarbierJrJ,Delano·F,JabouilleF,eta.lTotaloxidationofaceticacidinaqueoussolutionsovernoblemetalcata-lysts.JCata,l1998,177(2):378~3853FortunyA,BengoaC,FontJ,eta.lBimetalliccatalystsforcontinuouscatalyticwetairoxidationofpheno.lJHazardMater,1999,64(2):181~1934XuAihua,YangMin,DuHongzhang,eta.lInfluenceofpartialreplacementofCubyFeontheCWOofphenolintheCu0.5-xFexZn0.5Al2O4spinelcatalysts.CatalCommu,2006,7(8):513~5175DeLeitenburgC,GoiD,PrimaveraA,eta.lWetoxida-tionofaceticacidcatalyzedbydopedceria.ApplCatalB,1996,11(1):L29~L356BeziatJC.BessonM,GalletzotP,eta.lCatalyticwetairoxidationofcarboxylicacidsonTiO2-supportedrutheniumcatalysts.JCata,l1999,182(1):129~1357LinSS,ChenCL,ChangDJ,eta.lCatalyticwetairoxidationofphenolbyvariousCeO2catalysts.WaterRes,2002,36(12):3009~30148.:12.:,20079YangShaoxia,ZhuWanpeng,JiangZhanpeng,eta.lThesurfacepropertiesandtheactivitiesincatalyticwetairox-idationoverCeO2-TiO2catalysts,ApplSurfSc,i2006,252(24):8499~850510LeeDK.Catalyticwetairoxidationofcarboxylicacidsatatmosphericpressure.CatalToday,2000,63(2~4):249~25511ZhangQinglin,KarlTC.KineticsofwetoxidationofblackliquoroveraP-tPd-Ce/Al2O3catalys.tApplCatalB,1998,17(4):321~33212GallezotP,LaurainN,IsnardP.Catalyticwe-tairoxida-tionofcarboxylicacidsoncarbon-supportedplatinumcatalysts.ApplCatalB,1996,9(1~4):L11~L1713GallezotP,ChaumetS,PerrardA,eta.lCatalyticwetairoxidationofaceticacidoncarbon-supportedrutheniumcatalysts.JCata,l1997,168(1):104~10914AtwaterJE,AkseJR,McKinnisJA,eta.lLowtem-peratureaqueo