cuphenoih催化剂的合成及其羟基化催化性能研究word格式论文.docxVIP

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cuphenoih催化剂的合成及其羟基化催化性能研究word格式论文.docx

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cuphenoih催化剂的合成及其羟基化催化性能研究word格式论文

Withthedoublepropertiesoforganiccomponentandinorganiccomponent, organic-inorganichybridmaterials(OIH)exhibitgreatpotentialsascatalystsforbulky substratesinmanyreactions.OIH-supportedmetalcatalystshavetheadvantagesof homogeneousandheterogeneouscatalysts.Thisthesisdealswiththepreparation, characterizationandcatalyticreactivityinphenolhydroxylationofOIH-supportedcatalysts (Cu/Phen/OIH).Thecatalystwassynthesizedbyco-condensationproceduresandcharacterizedby FTIR、XRD、AAS、TG-DTA.AASgavetheresultthattheconcentrationofCuonthe catalystwas0.884mmol/g;TGA-DTAandFTIRdatashowedthatNH2-PhenwasgraftedtothesurfaceofOIHbycovalentbondandtherewascoordinationbondbetweenN-donor ligandandCu(Ⅱ);XRDresultshowedthatthecatalysthasthesamemesoporousstructurewithMCM-41.TG-DTAresultssuggestedthatCu/Phen/OIHwasstableunderreaction conditions.Thecatalystwasappliedintothereactionofphenolhydroxylation.Underthe optimizedconditions[m(phenol)︰m(30%H2O2)︰m(H2O)︰m(catalyst)=23.5︰28.5︰750︰1,50℃,2h],thecatalystshowedhighcatalyticactivityandselectivity,withtheconversionofphenolof30.6%andselectivityofdiphenolsof92.4%.Theconversionof phenol was increased by76.5% comparingwith homogeneous catalyst.Thephenol hydroxylation was a selectiveoxidative reaction.The·OHradical released byH2O2tendedtoattacktheo-andp-positionofphenol.Thebenzeneringwasactivated so that diphenolswereeasilyturned to phenolictars dueto deep oxidation. Then the surface ofthe catalyst was covered with phenolic tars. Sothe heterogeneous couldnot bereused.ThecatalystCu/Phen/OIHshowedhighcatalyticactivityandselectivityinphenol hydroxylation.Comparingwithothercatalysts,theefficiencyofCu/Phen/OIHwashigher because of low amount and short time needed forthereaction.Keywords:organic-inorganichybridmaterials;catalyst;Cu/Phen/OIH;phenol hydroxylation摘要...................................................................................................................................IAbstract...................................................................