SUZ4分子筛上二甲醚制备的研究.pdf

ABSTRACT ABSTRACT Overthepastfewdecadesmuchresearchhasbeenfocusedonsynthesis, characterization,andcatalysisonzeolites.Onlyfewofthesematerials,however,are usedcommerciallyasionexchangebuilders,adsorbents,orcatalysts.Thereis consequentlyasignificantincentive(i)toutilizeknownzeolitesinnovelapplications and(ii)toproducenewmaterialswithpotentiallyusefulproperties.Inthiscontext, synthesisofSUZ-4zeoliteanditsapplicationincatalysishavebeenstudiedinthis dissertation.ZeoliteSUZ-4isanewsyntheticaluminosilicatepatentedbyBritish PetroleumCo.(BPC)in1992.ZeoliteSUZ-4showshighactivity,selectivityand stabilityinmethanoldehydrationtodimethylether(DME),however,itwas deactivatedeasilyinsyngastoDME.Therefore,technologiesofXRD,SEM,MAS NMR,FTIR,TG-DTA,XPS,NH3-TPD,EDSandN2adsorptionareemployedfor catalystscharacterizations,and,basedontheresultsofcatalystscharacterizations, mechanismsofDMEformationandthereasonsforhighDMEselectivityinmethanol dehydrationoverHK-SUZ-4zeolitesareproposed.ThereasonforHK-SUZ-4 deactivationinsyngastoDMEisalsoreportedhere. Generally,ion-exchangeisemployedinmodifyingacidityofzeolites,andmany methodswereproposedinpreviouspapers.Itisproposedthatsomepotassiumionsin SUZ-4zeolitearelockedinasmallcage,asaresult,theirexchangewouldbedifficult. triedtoi ion-exchangedegreeofSUZ-4byperformingion Consequently,we exchange using multicycle of ion-exchange/calcination. Through three exchange/calcinationcyclesundergeneralhydrothermalcircumstance,theresulting protonexchangedzeolitewithion-exchangedegreeofonly76%wasobtained. HK-SUZ-4zeolitewithdifferention-exchangedegreepossessesvariouH+contents, and,consequently,theiraciditiesaredifferent.Asaresult,theypresentdistinct catalyticpropertiesinmethanoldehydrationtoDME. ItiswellknownthatDMEhasmanyadvantageouspropertiesasaproper ABSTRACT substitutefordieselorrefrigerantinfuture.Presently,DMEismadebycatalytic de