One-Pot Synthesis of Hierarchically Nanoporous SSZ-13 for Conversion of Methanol to Olefins

(整期优先)网络出版时间:2017-03-13
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ThemaindisadvantageofmicroporousSSZ-13catalystusedinthemethanoltoolefins(MTO)processisitsrapiddeactivationduetoitsrelativelylowcokeresistance.Meanwhile,thehierarchicalzeolitesusuallyexhibitimprovedcatalyticstabilitythankstotheirbettermasstransferability.Herein,thehierarchicallynanoporousSSZ-13zeoliteswereone-potsynthesizedbyusingN,N,N-trimethyl-1-adamantanammoniumhydroxideasamicroporousstructuredirectingagentandC18H37N+(CH3)2C6H12N+(CH3)2C6H13(Br-)2(hereinafterabbreviatedasC18-6-6Br2)asamesoporogen.ThehierarchicallynanoporousSSZ-13catalystwascharacterizedbyXRD,N2physisorption,SEM,TEM,TG-DTG,27Aland29SiNMRspectroscopyandNH3-TPDtechniques.TheresultsshowedthatthehierarchicalSSZ-13zeolitesynthesizedinthepresenceoftheC18-6-6Br2surfactantexhibitsaggregatesofprimarynanocrystalsandcontainsthewell-developedmesoporesandexcellentacidity.Comparedtoitsconventionalcounterpart,thehierarchicalSSZ-13zeolitehaslongercatalyticlifetimeandhigherselectivityforethyleneandpropyleneintheMTOreaction,whichcanbeattributedtothesynergisticeffectoftheirgoodacidityandimproveddiffusionpropertiesresultedfromthehierarchicalporestructure.