AgTiO2光催化氧化还原反应脱除水体中无机氮

研究论文Ag/TiO2柳丽芬1,2,李秀婷1,杨凤林1,余济美3(1.,116023;2.,116023;3.,):采用光催化还原法制备了高活性的载银二氧化钛光催化剂,并用XRFTEMXRD及XPSUV-Vis方法对催化剂进行了表征.考察了负载Ag的含量催化剂制备时间搅拌气体的种类以及Fe2+的添加等条件对该催化剂光催化水体脱氮活性的影响.结果表明:载银量1.0%时去除效果最佳;制备催化剂时光照时间不充分会使催化剂失去还原效力;氮气保护下催化剂反应活性更高;Fe2+的加入利于光催化反应;2h光催化含氨氮和亚硝基氮的水样,总脱氮率达到了63.9%.:Ag/TiO2;光催化反应;氨氮;亚硝酸氮:1000-3231(2006)04-0291-10:O64:A,[1],.(NH4+)N)(NO2-)N)(NO3-)N)4,[2].,.,,[3]..TiO2,[4].TiO2,,[5].TiO2.,TiO2AgPtCr:2006-04-03;:2006-04-25.:(20477006).:(1965-),,,,,,E-mail:[e-mail].291244Vol.24No.420067PhotographicScienceandPhotochemistryJuly,2006[6].PtCr,Ag,,Ag[7],.AgTiO2.AgTiO2,Anammox,N2,,AgFe2+,.11.1TiO2(Degussa,P-25,75%,25%,50m3/g),(Ag-NO3,0.01357mol/L),EDTA(0.01mol/L).722E(),752(),TOC-VCPH-TNM-1(SHI-MADZU),SX2(),101-1A(),(LG10-2.4A,),SRS3400X(XRF),JSM-100CXÒ(TEM),D/MAX-2400X(XRD),JASCOUV-550(UV-Vis),Kratos-am-icusXPS(KratosAralyficalLtd.UK).1.211-(20W,K=253.7nm);2-;3-;4-Double-deckringedquartzreactiontube1-ultravioletlamp(20W,K=253.7nm),2-quartzreactor,3-aerationequipment,4-reactionfluid1.31gP-25TiO2(1),,EDTA,150mL.2922420min,20W1.5h.,4,105e,.0.5%1.0%1.5%.1.4()(1)..1g/L,TN()50mg/L(,pHU10.0)10.4),(,;400mL/min,800mL/min),2h,0.5h,(0.22Lm).,,N-(1-)-,.22.1(TEM)(2)(1.5h,Ag(1.0%)/TiO2)(1)2nm),.X(XRD),XRD(3)Ag(38.2b44.2b64.6b),X(XRF).AgTiO2,TEM.21.5hTEM(Ag(1.0%)/TiO2)TEMphotosofphotocatalystsamplepreparedwith1.5hirradiation2.22.2.1Ag/TiO2N2,4:Ag/TiO229331.5hXRD(Ag(1.0%)/TiO2)XRDpatternsofphotocatalystsamplepreparedwith1.5hirradiation.4)6,,,,,;4(Ag(1.0%)/TiO2)Influenceoflightontransformationoftotalnitrogen5(Ag(1.0%)/TiO2)Influenceoflightontransformationofammonianitrogen6(Ag(1.0%)/TiO2)Influenceoflightontransformationofnitritenitrogen,,.N2.294242.2.27,Ag/TiO2.Ag(),1.0%70.5%1.0%1.5%(pH=10.1,400mL/min)ConversionrateoftotalnitrogenasafunctionoftimewithdifferentAgloading:0.5%,1.0%,1.5%Ag/TiO2,50.97%(1),21117%,29.80%,.TiO2TiO2.-,;,,,TiO2,,TiO2,.,TiO2.Ag1.0%,1.0%TiO2.10.5%1.0%1.5%(pH=10.1,400mL/min)ChangesofnitrogenspeciesasafunctionofAgloadinginphotocatalyst:0.5%,1.0%,1.5%Ag/%0.51.01.5TN/%41.0150.9736.15NH4-N/TN0/%14.9121.1712.93NO2-N/TN0/%26.1129.8023.232.2.3,().8,,,,,.,,.,,,.9,1.5h,4:Ag/TiO2295,,.,1.5h0.5h.80.5h,(Ag(1.0%)/TiO2,pH=10.1)Changesofnitrogenspeciesafterreactionusingphotocatalystpreparedwith0.5hirradiation91.5h,(Ag(1.0%)/TiO2,pH=10.1)Changesofnitrogenspeciesafterreactionusingphotocatalystpreparedwith1.5hirradiationX(XPS)(10):368.51eV374.53eV,Ag+[8,9].0.5h1.5h,TiBAg:16.2B0.4115.4B0.37.1.5hAuger,0.5hAuger.XPS,,1eV.-UV-Vis(11):,SPA(SurfacePlasmonAbsorption).10Ag/TiO2(0.5h1.5h)XPSAg3dXPSspectrumofAg/TiO2(0.5hand1.5h)11Ag/TiO2(0.5h1.5h)UV-VisUV-VisspectraofAg/TiO2(0.5hand1.5h).Yu[10]:,TiO2;,.[11]29624.SPA[12],[10].,[13],,,,.115h015h,..,.2.2.4,,,.12,,,2h62.38%(2),,2.,,,,12TN(Ag(1.0%)/TiO2,pH=10.32)Influenceofstirringgasonphotocatalyticremovalrateoftotalnitrogen(Ag(1.0%)/TiO2,pH=10.32),12.12%.,N2Ar,;N2,.2(Ag(1.0%)/TiO2,pH=10.32)Influenceofstirringgasonconversionrateofnitrogenspeciesinphotocatalyticreaction(Ag(1.0%)/TiO2,pH=10.32)N2ArTN/%62.3825.87NH4-N/%62.6839.55NO2-N/%61.9812.122.2.5Fe2+TiO2FeSO4(Fe2+19.34mg/L),Fe2+.13(),Fe2+,TN,63.91%(3),Fe2+2.(1415),4:Ag/TiO2297.Fe2+,,,Fe2+Ag/TiO2.Fe3+19.34mg/L()(3),Fe2+,,,23.10%,Fe2+.3Fe2+(Ag(1.0%)/TiO2,pH=10.21)InfluenceofFe2+onconversionrateofnitrogenspeciesFe2+Fe3+Fe2+Fe3+TN/%38.0463.9131.86NH4-N/TN0/%24.2044.6022.27NO2-N/TN0/%13.8321.6732.69NO3-N/TN0/%02.3623.1013Fe2+InfluenceofFe2+onremovalrateofTN(Ag(1.0%)/TiO2,pH=10.21)14Fe2+InfluenceofFe2+onconversionrateofammonianitrogen(Ag(1.0%)/TiO2,pH=10.21)15Fe2+InfluenceofFe2+onconversionrateofnitritenitrogen(Ag(1.0%)/TiO2,pH=10.21):,.[14]ESR,.29824Fe2+,Fe2+,Fe2+Fe3+,,.Fe2+,..Fe3+,,Fe3+.,,Fe3+[15].3TiO2,N2;,,1.0%;,0.5h,,1.5h)));,;Fe2+,.2h,63.9%.:[1],.[J].,2001,21(1):9-12.ZhangY,WanJQ.Newdevelopmentoftheindustrialwastewaterpollutioncontrol[J].IndustrialWaterTreat-ment,2001,21(1):9-12.[2],.)))[M].:,1999,195-197.ShenYL,WangBZ.NewTechnologiesforBiologicalWastewaterTreatmentTheoryandApplication[M].Be-ijing:ChinaEnvironmentSciencePress,1999.195-197.[3],.[J].,2004,15(5):174-176.WuJ,CuiJG.Photocatalysisdegradationofinorganicnitrogeninwater[J].SCI/TECHInformationDevelopment&Economy,2004,15(5):174-176.[4],,.Ag[J].,2002,16(2):222-226.CuiP,XuNP,ShiJ.EffectsofpreparationconditionsonphotocatalyticactivityofAg/TiO2membranephotocatalystpreparedbythephoto-reductiontechnology[J].JournalofChemicalEngineeringofChineseUniversities,2002,16(2):222-226.[5],,,.Ag-TiO2[J].,2004,62(12):1110-1114.XinBF,JingLQ,RenZY,etal.PreparationandactivityofAg-TiO2photocatalystwithmult-ivalencystate[J].ActaChimicaSinica,2004,62(12):1110-1114.[6],,,.TiO2[J].,1998,10(4):349-361.ShengWR,ZhaoWK,HeF,etal.TiO2basedphotocatalysisanditsapplicationsforwastewatertreatment[J].ProgressinChemistry,1998,10(4):349-361.[7]SuC,YehJC,LinJL,etal.ThegrowthofAgfilmsonaTiO2(110)-(1x1)surface[J].Appl.Surf.Sci.,4:Ag/TiO22992001,169-170:366-370.[8]KatoS,HiranoY,IwataM,etal.Photocatalyticdegradationofgaseoussulfurcompoundsbysilver-depositedtitan-iumdioxide[J].AppliedCatalysisB:Environment