Fenton法氧化处理水中土霉素的研究

27Vol.2,No.720087ChineseJournalofEnvironmentalEngineeringJul.2008Fenton3(,100085)Fenton,Fenton(Fe2+2H2O2)H2O2Fe2+pH,,H2O2Fe2+51,pH3.04.0,H2O20.9mmol/L,100mg/L10minTOC40%,(BOD5/COD),FentonX70311A167329108(2008)0720865204StudyonFentonreagentdegradationofoxytetracyclineinaqueoussolutionLiKuixiaoCaoNanZhangYuYangMinYiQizhen(StateKeyLaboratoryofEnvironmentalAquaticChemistry,ResearchCenterforEco2EnvironmentalSciences,ChineseAcademyofSciences,Beijing100085)AbstractDegradationofoxytetracyclinebyFentonreactionwasstudiedinthispaper.Theinfluencesonthedegradationrateofreactionconditionswerediscussed.Moreover,theeffectofoxalicacidonoxytetracyclinedegradationwasstudied.Theresultsshowedthattheoptimumratioofhydrogenperoxideandferrousis5to1,andtheoptimumpHoccurredat3.04.0.UndertheoptimalconditionsofthatinitialpH=3,[H2O2]=0.9mmol/L,theratioofH2O2/Fe2+=5,andreactiontime=30min,100mg/Loxytetracyclinewascompletelydegradedwithin10min,correspondingly40%TOCremovalandsignificantimprovementofbiodegradabilitywereobserved.Oxalicacidpresentinsolutionssuppressedtheoxidationefficiencywhileitsinhibitioninfluencecouldbeeliminatedbytheexcessiveaddofferrous.Keywordsoxytetracycline;Fentonreagent;oxalicacid:(50525824);(06FZZDSH00900);(20477057):2008-01-05;:2008-03-15:(1978),,,E2mail:[e-mail]3,E2mail:[e-mail](oxytetracycline),[13],,[4],,,(ad2vanceoxidationprocesses,AOPs)AOPs,Fenton,,[58]Fenton,H2O2Fe2+,Fenton211.1(Agilent1100,Agilent),(TOC25050,Shi2madzu,),pH(WTW2pH2MeterMultilineP4,)(CAS.no.205824620)Sigma2aldrich,FeSO47H2O,H2O2(30%),,NaOH,Milli2Q(Millipore,Watford,)1.2,100mg/L,,,NaOHH2SO4pH,FeSO47H2O,H2O2,NaOH,pH7.58.0,Fenton,1.3COD(CTL212,,)BODBOD5(WTWOxiTop212,)0.45m,20L(Agilent1100,Agilent),,HPLC::ZoRbaxC18(250mm416mm,5m);A:0.01mol/L,B:=11();:26;1mL/min;:355nm;:20L(TOC25050)22.1H2O2Fe2+H2O2Fe2+Fenton[9,10]H2O2Fe2+,Fe2+H2O2,pH=3H2O2(0.5mmol/L),Fe2+(0.0250.2mmol/L)1Fe2+,;Fe2+0.1mmol/L,15min92135%;Fe2+1(0.2mmol/L),15min92186%,Fe2+,,Fe2+0.1mmol/L,H2O2Fe2+511Fe2+[H2O2]0=0.5mmol/LFig.1EffectofFe2+concentrationonoxytetracyclineremoval2.2H2O2Fe2+H2O2Fe2+,FentonH2O2Fe2+=51,Fenton,2,0.9mmol/L,Fenton2.3pHFenton,pHOH,Fe2+[11,12],pH3,H+,Fe3+Fe2+,,pHFe2+Fe3+,FentonpH,Fenton6687:Fenton2Fe2+H2O2Fig.2EffectofFe2+andH2O2amountondegradationofoxytetracycline3H2O20.5mmol/L,Fe2+0.1mmol/L,100mg/L,30min,pH3,Fenton,pH3.04.0,99%[13,14]3pHFig13EffectofinitialpHofthesolutiononefficiencyofoxytetracyclinedegradation2.4(13mmol/L),Fenton4H2O20.9mmol/L,Fe2+0.18mmol/L,100mg/L,30min,(0.253mmol/L),2mmol/L,,Fe2+,5,Fe2+,Fe2+[15]Fenton,,Fenton2.5Fenton,Fen2tonTOCBOD5/COD6,TOC10min40%,BOD5/COD5min,0.030.26,30min0.29Fenton,5min,BOD5/COD,76826TOCBOD5/CODFig.6RemovalofTOCandvariationofBOD5/CODduringFentonoxidationprocess3(1)Fenton,TOC(2):51;pH3.0,0.90.18(mmol/L)100mg/L,10min(3),,(4),Fenton,,,[1]ZhuJ.,SnowD.D.,CassadaD.A.,etal.Analysisofoxytetracycline,tetracycline,andchlortetracyclineinwaterusingsolid2phaseextractionandliquidchromatography2tan2demmassspectrometry.J.Chromatogr.A,2001,928:177186[2]KimS.,EichhornP.,JensenJ.N.,etal.Removalofan2tibioticsinwastewater:Effectofhydraulicandsolidreten2tiontimesonthefateoftetracyclineintheactivatedsludgeprocess.Environ.Sci.Technol.,2005,39:58165823[3]SarmahA.K.,MeyerM.T.,BoxallA.B.A.Aglobalper2spectiveontheuse,sales,exposurepathways,occur2rence,fateandeffectsofveterinaryantibiotics(VAs)intheenvironment.Chemosphere,2006,65:725759[4]BoxallA.B.A.,KolpinD.W.,Halling2S«rensenB.,etal.Areveterinarymedicinescausingenvironmentalrisks?Environ.Sci.Technol.,2003,37:286A294A[5]MaJ.H.,SongW.J.,ChenC.C.,etal.Fentondegrada2tionoforganiccompoundspromotedbydyesundervisibleirradiation.Environ.Sci.Technol.,2005,39:58105815[6]KuoK.W.DecolorizingdyewastewaterwithFentonsrea2gent.Wat.Res.,1992,26:881886[7]RivasF.J.,BeltranF.J.,GimenoO.,etal.OptimisationofFentonsreagentusageasapretreatmentforfermenta2tionbrines.J.HazardMater,2003,96:277290[8]DeMoraisJ.L.,ZamoraP.P.Useofadvancedoxidationprocessestoimprovethebiodegradabilityofmaturelandfillleachate.J.HazardMater,2005,123:181186[9]NeyensE.,BaeyensJ.AreviewofclassicFentonsperoxi2dationasanadvancedoxidationtechnique.J.HazardMa2ter,2003,98:3350[10]YoonJ.,LeeY.,KimS.InvestigationofthereactionpathwayofOHradicalsproducedbyFentonoxidationintheconditionsofwastewatertreatment.Wat.Sci.Techn2ol.,2001,44(5):1521[11]KwonB.G.,LeeD.S.,KangN.,etal.Characteristicsofp2chlorophenoloxidationbyFentonsreagent.Wat.Res.,1999,33:21102118[12]LuM.C.,LinC.J.,LiaoC.H.,etal.InfluenceofpHonthedewateringofactivatedsludgebyFentonsrea2gent.Wat.Sci.Technol.,2001,44:327332[13]SedlakD.L.,AndrenA.W.OxidationofchlorobenzenewithFentonsreagent.Environ.Sci.Technol.,1991,25:777782[14]BigdaR.J.ConsiderFentonschemistryforwastewatertreatment.Chem.Eng.Prog.,1995,91:6266[15],,.FentonFenton2,42D.,2005,24:365369868