超声光催化降解苯胺及其衍生物研究顾浩飞

:0253-2468(2003)05-0593-05　　　:X703.1　　　:A顾浩飞1,安太成1,2＊,文　晟2,陈卫国1,朱锡海1,傅家谟2,盛国英2　(1.,　510275;2.,,　510640):,,TiO2-.,,,.:;;;;SonophotocatalyticdegradationofanilineanditsderivativesGUHaofei1,ANTaicheng1,2,WENSheng2,CHENWeiguo1,ZHUXihai1,FUJiamo2,SHENGGuoying2　(1.SchoolofChemistryandChemicalEngineering,ZhongshanUniversity,Guangzhou　510275,China;2.StateKeyLaboratoryofOrganicGeochemistry,GuangdongKeyLaboratoryofEnvironmentalResourcesUtilizationandProtection,GuangzhouInstituteofGeochemistry,Chi-neseAcademyofSciences,Guangzhou　510640,China)Abstract:Theeffectsofcompoundswithdifferentstructuresontheirsonophotocatalyticdegradationwereinvestigatedindetail,usinganilineanditsderivativesasmodelpollutant,andanewAdvancedOxidationProcesses(AOPs),sonophotocatalysiswhichcombinedthephotocatalysiswithultrasonictechnology,waspioneeredfordegradingorganicpollutants.Theexperimentalresultshowedthatthesynergeticeffectwasnotassignificantasexpected,butthesonophotocatalytictechnologyhavegoodCODremovalefficiencies,furthermore,thecompoundswithdifferentstructuresalsoplayedanimportantroleinthesonophotocatalyticreaction.Keywords:sonophotocatalysis;photocatalysis;ultrasonic;compoundstructure;structurereactivity:2002-07-26;:2002-10-14:(29977030);(A3030502);(OGL-200210):(1978—),,.　＊,,、、、,.,TiO2-,,(·OH)[1],-.,,[2—5],.2080,O·、OH·、HO2·,,,,[6,7],.KR[7];Stock23520039　　　　　ACTASCIENTIAECIRCUMSTANTIAEVol.23,No.5Sep.,2003DOI:10.13671/j.hjkxxb.2003.05.006N.L.ChundeW.,[8,9].8,,.1　1.1　1　Fig.1　Sonophotocatalyticreactor1.1.2　:P-25TiO2;,,,,,,,,.1.0×10-3molL.:500W();Branson1200(47kHz,30W,Branson,USA);COD();(CARY100VARIAN)1.3　1.0×10-3molL700mL,1.4g,,、、,,;,15min;2h,,COD.2　2　Fig.2　ChangeofU-visiblespectraofaniline2.1　,2,,90min,.,[7].SF:SF=Rspc-(Rpc+Rus);Rspc,RpcRus、COD.SF0,,SF,;,SF≤0,.3,,,SF=0.0100-(0.0059+0.0028)=0.00130;SF=0.0073-(0.0045+0.0019)=0.00090;SF=0.0100-(0.0077+0.0024)=-0.00010,,,,.594　　　　　　　　　　233　Fig.3　KineticofCODremovalforanilinederivatives(a:aniline;b:p-nitr-oaniline;c:p-toluidine).,,.,3(a—c):,.2.2　、、、[10].D'Oliveira[11],TiO2-(Kow)Hammett(σ):k1=-10σ+5.2lgKow-7.5.　　.-(Kow),(Hammettσ),(,).4　CODFig.4　CODremovalvsreactiontimecurves2.2.1　　,,,≈.σ4.σ,,.,(·OH),,,,·OH.-(Kow).logKow[12],logKow(1.40)(1.39)(1.29).COD,COD.5955:5　CODFig.5　CODremovalvsreactiontimecurves,p-toluidineofanilineandchloroaniline,、,;,,、,-(Kow),Kow,,,Kow.,,,.[12]logKow,logKow(1.90)(1.88)(1.83),,5COD.[13],TiO2:2、4、6-2、4-,.,—Cl,logKow(0.90),,,.6　CODFig.6　CODremovalvsreactiontimecurvesofpara-substitutedanilinederivatives2.2.2　、、、、,COD6.,、、90minCOD,、.:—CH3,δ—π,;—OCH3p—π,p—π,p—π,,—OCH3—CH3;logKow1.39,logKow0.95,COD.—Cl、—SO3H、—NO2,,,—SO3H—NO2—Cl,COD6,.logKow1.88,,COD.596　　　　　　　　　　233　(1),,.(2),-logKow,,logKow,,.(3)—CH3,;—Cl,.(4),:≈≈.:[1]　HoffmanM,MartinS,ChoiW,etal.Environmentalapplicationofsemi-conductorphotocatalysis[J].ChemRev,1995,95:69[2]　AlbericiRM,JardimWF.PhotocatalyticdegradationofphenolandchlorinatedphenolsusingAg-TiO2inaslurryreactor[J].Wa-terRes,1994,28:1845[3]　AnTC,ZhuXH,XiongY.SynergicdegradationofreactivebrilliantredX-3Busingthreedimensionelectrode-photocatalyticreac-tor.J.Envion.Sci.Health[J].2001,36A(10):2069[4]　NavioJA,TestaJJ,DjedjeianP,etal.Iron-dopedtitaniapowdersbyasol-gelmethods.PartⅡ:photocatalyticproperties[J].Appl.Catal.A:General,1999,178:191[5]　AnTC,ZhuXH,XiongY.Feasibilitystudyofphotoelectrochemicaldegradationofmethylenebluewiththreedimensionalelectro-des-photocatalyticreactor[J].Chemosphere,2002,46(6):897[6]　KadoY,AtobeM,NonakaT.Ulyrasoniceffectonelectroorganicprocess-part20.PhotocatalyticoxidationofaliphaticalcoholinaqueoussuspensionofTiO2powder[J].UltrasonSonochem,2001,8:69[7]　AnTC,GuHF,ZhuXH,etal.DecolorizationandCODremovalfromreactivedye-containingwastewaterusingsonophotocatalytictechnology[J].JChemTechnolBiotechnolAccepted,2003(inpress)[8]　StockNL,PellerJ,VinodgopalK,etal.Combinativesonolysisandphotocatalysisfortextiledyedegradation[J].EnironSciTechnol,2000,34:1747[9]　WuCD,LiuXH,WeiDB,etal.Photosonochemicaldegradationofphenolinwater[J].WatRes,2001,35(16):3927[10]　,.[J].,1998,17(11):43[11]　Jean-Chrstophe,D'Oliveira,ClaudioMinero,etal.PhotodegradationofdichlorophenolsandtrichlorophenolsinTiO2aqueoussus-pensions[J].JPhotochemPhotobiolA:Chem,1993,72(3):261[12]　KarelV.HandbookofEnvironmentaldataonorganicchemicals(2ndEd.)[M].NewYork,VanNostrandReinholdCompanyInc.,1983.356,1110[13]　,,.TiO2[J].,1990,9(6):1305975: