CeO2SiO2粒状除氟剂的制备及其对F的吸附性能宋宽秀

CeO2/SiO2F-宋宽秀＊　严玉清　颜秀茹　聂建明(　300072)　　CeO2,CeO2/SiO2。DTA-TG、XRD、IR,。,CeO2/SiO2F-,Freundlich。400℃CeO2/SiO2CeO2。　CeO2/SiO2,:O614;O647　　　　　:A　　　　　:1000-0518(2003)06-0586-042002-10-09,2002-12-29(953606811):,,1945,;E-mail:[e-mail];:,、、[1]。,CeO2·nH2O。Misak[2～4]CeO2·nH2O、,F-;Shushu[5]CeO2·nH2OF-。CeO2·nH2OF-,,,,,。,Ce(Ⅳ),,CeO2/SiO2,F-。1　1.1　CeO2/SiO2Ce(NO3)3·6H2O(,),H2O,Ce(Ⅲ)H2O2,Ce(Ⅲ)Ce(Ⅳ)。,,,30min,Ce(Ⅳ)(H3Cit),,,30min,0.025mol/LCe(Ⅵ)。0.45～0.28mm(897m2/g)400℃2h,,Ce(Ⅳ)()24h,,100℃H2O,CeO2/SiO2(1,700℃Ce(Ⅳ),,2)。,CeO2/SiO2。1.2　CeO2/SiO2F-DTA-TGWCT-1;BDX3300X;IRBIO-RADFTS3000;CeO2/SiO2CeO2,V(H2SO4)∶V(H2O)=1∶1H2O2,ⅢCe(Ⅳ)[6],CeO2。CeO2/SiO2F-,CeO2/SiO2,pHF-,WH-4,F-,CeO2/SiO2F-。F-[7]。206Vol.20No.620036　　　CHINESEJOURNALOFAPPLIEDCHEMISTRY　　　Jun.20032　2.1　CeO2/SiO22.1.1　DTA-TG分析　1CeO2/SiO2DTA-TG,1。1,101℃(DTA),3.74%(TG),HNO3;210281℃,H3Cit(2.87%),Ce(Ⅳ)(4.41%),400℃TG。1　CeO2/SiO2DTA-TGFig.1　DTA-TGcurvesofCeO2/SiO2precursor2　CeO2/SiO2XRDFig.2　XRDpatternsofCeO2/SiO2a.twoimpregnations(calcinatedat700℃);b.oneimpregnation(calcinatedat700℃);c.oneimpregnation(calcinatedat400℃)2.1.2　XRD分析　2b1CeO2/SiO2700℃XRD,2a1CeO2/SiO2,Ce(Ⅳ),700℃CeO2/SiO2XRD。2,2a4CeO2(JCPDSCeO2),2b,2CeO2/SiO2CeO2(5.45mg/g)1(4.15mg/g)。2c2bCeO2/SiO2,CeO2/SiO2400℃。2,CeO2/SiO2400℃,Ce(Ⅳ)CeO2,2.1.1TG-DTA。2a,Ce(Ⅳ)2CeO2/SiO2CeO2/SiO2,CeO2,,(111),Scherrer,SiO2CeO24nm。2.1.3　IR分析　31CeO2/SiO2(a)400℃CeO2/SiO2(b)IR。3bIR(),(3a)1358cm-11,(—COO-)[8],3a3b,400℃,1358cm-1,400℃—COO-,TG-DTA。2.2　CeO2/SiO2F-2.2.1　焙烧温度对CeO2/SiO2除氟性能的影响　41CeO2/SiO2,CeO2/SiO2F-(q)。,400℃500℃,CeO2/SiO2F-,,F-。CeO2/SiO2F-,CeO2F-[9],,CeO2587　6:CeO2/SiO2F-　　3　CeO2/SiO2IRFig.3　IRspectraof(a)CeO2/SiO2precursorand(b)thatcalcinatedat400℃4　CeO2/SiO2F-qFig.4　DependenceofF-adsorptioncapabilityonthecalcinationtemperatureofCeO2/SiO2pH=6.2;initialF-conc.:10mg/LH2O,F-。400℃500℃,F-,,CeO2。2.2.2　CeO2/SiO2除氟剂对F-的吸附等温线　5F-pH=4.81CeO2/SiO2F-。5a1,700℃F-,5b,、700℃CeO2/SiO2F-。Freundlichq=kc1/n,(a)q=0.1389c1.38(R=0.9793),(b)q=0.1885c1.39(R=0.9645)。,CeO2/SiO2F-Freundlich。2,k。[10],Freundlich,k=ans,ns,a。、,ak,ns1CeO2/SiO22CeO2,ns,k。5　CeO2/SiO2F-Fig.5　IsothermaladsorptionofF-onCeO2/SiO2pH=4.81;a.CeO2/SiO2sampleobtainedfromoneimpregnation;b.CeO2/SiO2samplewithtwoimpregnationscalcinationtemperature700℃6　qtFig.6　Plotsofadsorptioncapacityofsilicagelvstimea.d=0.90～0.45mm(specificasea303m2/g);b.d=0.45～0.28mm(specificasea897m2/g)588　　　　　　　　　　　　　　　　　　　20　2.2.3　CeO2/SiO2对F-的吸附速率　6Ce(Ⅳ)0.025mol/L1,(500℃)F-(c(F-)=10mg/L,pH=6.2)(q)(t)。6,CeO2/SiO2F-。БРЫΚИНА[11]-ln(1-F)=kt(,Ft,k),6-ln(1-F)t,k(a)=0.0214(R=0.9721),k(b)=0.0345(R=0.9613)。,0.45～0.28mmF-0.90～0.45mm1.61。　　　　1　RuvaracA.GroupⅣHydrousOxides———SyntheicInorganicIonExchangers.InorganicIonExchangeMaterials[M].BocaRaton,Florida,CRCPress,1982:152　2　MisakNZ,MikhailEM.JApplChemBiotech[J],1978,28:499　3　MisakNZ,MikhailEM.JInorgNuclChem[J],1981,43:1903　4　MisakNZ,El-naggarIM.JColloidandInterfaceSci[J],1990,135(1):6　5　ShushuI,ZyunjiN,TokuzoK,etal.ChemSocJapan[J],1987,(5):807　6　SONGEn-Lie(),ZHANGQuan-Ming(),Trans().PracticalInorganicLuminosityAnalysis()[M].Shenyang():LiaoningPeoplePress(),1983:183　7　WEIFu-Sheng().MonitorandAnalysisMethodsofWasteWater(),3rdEdn(3)[M].Beijing():ChineseEnvironmentSciencePress(),1989:297　8　JINGXu-Ying(),CHENShi-Li(),MEEn-Yi().IRSpectrumApplicationIntroduction()[M].Tianjin():TianjinScienceandTechnologyPress(),1992:92　9　SONGKuan-Xiu(),YANXiu-Ru(),HULiu-Chang(),etal.ChinJApplChem(应用化学)[J],1998,15(4):92　10　AdamsonAWAuth().GUTi-Ren()Tran().SurfacePhysicalChemistry()[M].Beijing():SciencePress(),1984:402　11　БрыкинаТВ,МарчакЛС,БелявскаяКА.ЖАналитическоиХимии,1980,35(12):2294PreparationofGranularCeO2/SiO2andItsAdsorptivityTowardsF-SONGKuan-Xiu＊,YANYu-Qing,YANXiu-Ru,NIEJian-Ming(DepartmentofChemistry,TianjinUniveisity,Tianjin300072)Abstract　GranularCeO2/SiO2capableofabsorbingfluorineregentshasbeenpreparedbyimpregnationmethodfollowedbycalcination.ThesamplesarecharacterizedbyDTA-TG,XRDandIRandtheF-ad-sorbi-litymeasurements.TheadsorptivityofCeO2/SiO2towardsF-isdecreasedwithincreaseincalcinationtemperatureintherangeof400to800℃.TheisothermaladsorptionofF-onCeO2/SiO2conformstoFre-undlichequation.CeO2inCeO2/SiO2sampleobtainedfromcalcinationat400℃appearedtobeacrys-talline.Keywords　CeO2/SiO2,fluorineadsorbingreagent589　6:CeO2/SiO2F-