活性艳红X_3B水溶液的光催化脱色及矿化过程研究_李昱昊

研究简报X-3B李昱昊,毛立群,张顺利,金振声,张治军(,475001)　:对染料活性艳红X-3B水溶液的光催化反应过程进行了初步研究.首先,利用紫外-可见吸收光谱、高效液相色谱和质谱对反应过程中溶液组成的变化进行了测试,并用重铬酸盐法测定了各反应时刻溶液的COD值;其次,使用红外吸收光谱对反应过程中催化剂表面的吸附物种进行了考察.研究结果表明,在本实验条件下,活性艳红X-3B水溶液的光催化脱色和矿化过程是同时进行的,脱色反应完成后,溶液中生成了难以降解的中间产物,致使矿化过程难以继续进行.:光催化;活性艳红X-3B;脱色反应;矿化过程:1000-3231(2004)05-0383-08　　:O64　　:A,.,,15%(150/),[1].、、、,[2,3].,TiO2.Blake300[4],,114,.[5-7]、[8-11]、[12-15],,.:2004-06-04;:2004-07-05.:(20071010).:(1977-),,;(1969-),,,,Tel:[phone],E-mail:[e-mail].383　22　5Vol.22　No.5　　20049PhotographicScienceandPhotochemistrySept.,2004　,,,.TiO2,X-3B.,X-3B,,X-3B.1　1.1　TiO2(,,20—30nm),X-3B(,1),.1　X-3BStructuremodelofreactivebrilliantredX-3B1.2　X-3B、(Υ=6cm),(18±2℃).250W,,1.14mW/cm2(,365nm),10min.100mL50mg/LX-3B(a),100mgTiO2,10min,.,,,12h.t=0h、0.5h、1h、2h、4h、8h,b、c、d、e、f、g;4h,(100mg)4h(h).1.3　-(UV-Vis,HEλIOSαUV-Vis,UNICAM)、(MS,ESQUIRE-LC,BRUKER)、(HPLC,Agilent1100,Agilent),(GB11914-89)(ChemicalOxygenDemand,COD),COD(COD0-CODt)/COD0;(FT-IR,AVATAR360FT-IR,Nicolet).0.5μm,,:ZORBAXSB-C18;UV,　384　　　　　　　　　22　220nm;:,20%5min,60min100%,10min,5min.ESI.2　2.1　X-3B2　X-3BPhotolysisdecolorationratecurveofreactivebrilliantredX-3BaqueoussolutionX-3B,.2,,X-3Bλ=536nm.X-3B[16],X-3B,,X-3B,,X-3B.2.1.1　UV-Vis3UV-Vis,,3　X-3BUV-VisUV-VisabsorbencyspectraofreactivebrilliantredX-3BaqueoussolutionatdifferentreactiontimeX-3B6,190nm、235nm、280nm、330nm,:370nmX-3B-;430—570nmX-3B,X-3B[17].,,430—570nm,4h(f),,X-3B.　5:X-3B385　　　X-3B-,、,,N2,X-3B[16].4h,,190—350nm.UV-Vis,4h,,,X-3B,,190nm、220nm、255nm3.4h8h(h)190—350nm,.,X-3B4h.4h,X-3B,4h(f)4h,(h)UV-Vis,8h(g),.,X-3B4—8h,.4　X-3BCODCODremovalofreactivebrilliantredX-3Baqueoussolutionatdifferentreactiontime2.1.2　COD4COD,COD.,2h,COD;2h,COD,4h,COD,80%.UV-Vis,X-3B,,,4h,.4h,4h(h),COD80%(),8h(g)COD,,.2.1.3　FT-IR5FT-IR,1TiO2,2,3—70.5h、1h、2h、4h、8h　386　　　　　　　　　22　　　　5　FT-IRFT-IRabsorbencyspectraofphotocatalystsinthesolutionatdifferentreactiontime6　X-3BHighperformanceliquidchromatographyofreactivebrilliantredX-3BaqueoussolutionⅠf,Ⅱh　5:X-3B387　　　,84h4h.5,TiO23,3500—3000cm-1OH[18];1630cm-1H—O—H;800—500cm-1TiO2Ti—O—Ti.TiO2,1580—1300cm-1.-[19],().UV-Vis,,X-3B().2.2　X-3B64h(f)4h(h)HPLC.,4h(5Ⅰ),4h(5Ⅱ),,,4h4h.74h(f)4h(h)7　X-3BThemassspectraofreactivebrilliantredX-3BaqueoussolutionⅠf,ⅡhMS.7Ⅰ、Ⅱ,fhMS,m/z=230—3605—7,m/z=480—6508—10.X-3B615,X-3B,X-3B-,,314,m/z=230—360X-3B,m/z=480—650X-3B.　388　　　　　　　　　22　HPLCMS,:,X-3B,..3　1.,X-3B.2.X-3B,.:[1]　LucarelliL,NadtochenkoV,KiwiJ.Environmentalphotochemistry:quantitativeadsorptionandFTIRstudiesduringtheTiO2-photocatalyzeddegradationoforangeⅡ[J].Langmuir,2000,16:1102-1108.[2]　,,.[J].,2001,21(12):1-4.ZhangYB,YuYM,LiuQJ.Progressinmultiphasesphotocatalyticdegradationofdye-containingwastewater[J].In-dustrialWaterTreatment,2001,21(12):1-4.[3]　,.[J].,2000,20(1):14-18.ZhangLS,JiangLL.Methodsfordecolorizationofdyewastewater[J].EnvironmentalProtectionofChemicalIn-dustry,2000,20(1):14-18.[4]　GoswamiDY.Areviewofengineeringdevelopmentsofaqueousphasesolarphotocatalyticdetoxificationanddisinfec-tionprocesses[J].JournalofSolarEngineering,1997,119(3),101-107.[5]　LinsebiglerAL,LuGQ,YatesJT,etal.PhotocatalysisonTiO2surface:principles,mechanisms,andselectedresults[J].Chem.Rev.,1995,95:735-758.[6]　GrzechulskaJ,MorawskiJW.Photocatalyticdecompositionofazo-dyeacidblack1inwaterovermodifiedtitaniumdioxide[J].AppliedCatalysisB:Environmental,2002,36:45-51.[7]　SakthivelS,ShankarMV,PalanichamyM,etal.PhotocatalyticdecompositionofleatherdyecomparativestudyofTiO2supporteronaluminaandglassbeads[J].JournalofPhotochemistryandPhotobiologyA:Chemistry,2002,148:153-159.[8]　StathatosE,PetrovaT,LianosP.Studyoftheefficiencyofvisible-lightphotocatalyticdegradationofbasicbluead-sorbedonpureanddopedmesoporoustitaniafilms[J].Langmuir,2001,17:5025-5030.[9]　AsahiR,MorikawaT,LhwakiT,etal.Visible-lightphotocatlysisinnitrogen-dopedtitaniumoxides[J].Science,2001,293(13):269-271.[10]　YuJC,YuJG,ZhaoJC.EnhancedphotocatalyticactivityofmesoporousandordinaryTiO2thinfilmsbysulfuricacidtreatment[J].AppliedCatalysisB:Environmental,2002,36:31-43.[11]　,,,.X-3B[J].,2000,21(1):100-105.ShiLY,LiCZ,FangDY,etal.PhotocatalyticdecolorizationofactiveredX-3BbyultrafineTiO2particlessynthe-sizedinhightemperatureaerosolreactor[J].ActaEnergiaeSolarisSinica,2000,21(1):100-105.[12]　WuTX,LiuGM,ZhaoJC.EvidenceforH2O2generationduringtheTiO2-assistedphotodegradationofdyesinaqueousdispersionsundervisiblelightillumination[J].J.Phys.Chem.,1999,103:4862-4867.[13]　ChenCC,ZhaoW,LiJY,etal.Formationandidentificationofintermediatesinthevisible-light-assistedpho-todegradationofsulforhodamine-BdyeinaqueousTiO2dispersion[J].Environ.Sci.Technol.,2002,36:3604-3611.[14]　,　,.TiO2[J].,2002,14(3):192-199.TangYC,HuC,WangYZ.RecentadvancesinmechanismsandkineticsofTiO2photocatalysis[J].Progressin　5:X-3B389　　　Chemistry,2002,14(3):192-199.[15]　,,,.[J].,1999,20(3):359-361.LiuGM,ZhangTY,WuTX,etal.Mechanismofphotocatalyticdegradationofdyepollutant-alizarinredundervisi-blelightradiation[J].ChineseJournalofCatalysis,1999,20(3):359-361.[16]　,,,.X-3B[J].,2001,22(2):181-184.MaoLQ,YangJJ,Guo