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1、JournalofMolecularCatalysisA:Chemical273(2007)7380DeactivationandregenerationoftitaniumsilicalitecatalystforepoxidationofpropyleneQingfaWang∗,LiWang,JunxiaChen,YulongWu,ZhentaoMiKeyLaboratoryforGreenChemicalTechnologyoftheMinistryofEducation,SchoolofChemicalEngineering&Technology,TianjinUniver
2、sity,Tianjin300072,PRChinaReceived2October2006;receivedinrevisedform22March2007;accepted23March2007Availableonline30March2007AbstractContinuousepoxidationofpropylenewith30-wt%hydrogenperoxideinisopropylalcoholsolventovertitaniumsilicalite(TS-1)zeolitewascarriedoutandthegoodselectivitytopropyle
3、neoxideandstabilityofTS-1wereobtained.Afterthereactionof263h,thedeactivationoftheTS-1catalystoccurred.Thespentcatalystswereregeneratedbycalcinationsat550◦Cfor5h,washingwithisopropylalcoholsolventorwashingwithdilutehydrogenperoxide,andtheactivityevaluationoftheregeneratedcatalystswerestudied.Th
4、edeactivatedandregeneratedcatalystswerecharacterizedbyscanningelectronmicroscopy,X-raydiffraction,Fourier-transforminfraredspectroscopy,29Simagicanglespinningnuclearmagneticresonance,thermogravimetricanalysisandBrunauerEmmettTellermethod.Thecompositionsdepositedonthesurfaceofthecatalystswereco
5、llectedbysolventextractionandwereanalyzedbygaschromatographymassspectrometry(GCMS).TheresultsshowedthatcalcinationandwashingwithdilutehydrogenperoxidewerehighlyeffectiveregenerationmethodsandthecatalyticactivityofTS-1catalystscanbemostlyrecoveredafterthesetreatments.Washingwithisopropylalcohol
6、hadasubtleeffectinrecoveringthecatalyticactivityoftheTS-1catalyst.ThemajorcauseofthedeactivationoftheTS-1catalystforepoxidationisblockingmicroporesinducedbybulkyorganicby-productsformedbyconsecutivereactionsoftargetreaction,suchasdimerizationoroligomerizationofpropyleneoxide,etherificationofpro
7、pyleneoxidewithisopropylalcohol.Inaddition,leachingofframeworktitaniumalsocontributestothedeactivationofthecatalyst.©2007ElsevierB.V.Allrightsreserved.Keywords:Propyleneepoxidation;Titaniumsilicalite;Deactivationandregeneration;Blocking