Aromatization over nanosized Ga-containing ZSM-5 zeolites prepared by different methods: Effect of acidity of active Ga species on the catalytic performance

(整期优先)网络出版时间:2017-04-14
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NanosizedGa-containingZSM-5zeoliteswerepreparedviaisomorphoussubstitutionandimpregnationfollowedbycharacterizedusingvarioustechniques.Thecatalyticperformanceofthezeolitesforthearomatizationof1-hexenewasinvestigated.TheresultsindicatethatisomorphoussubstitutionpromotestheincorporationofGaheteroatomsintotheframeworkalongwiththeformationofextra-frameworkGaO+species([GaO+]a)thathavestrongerinteractionswiththenegativepotentialoftheframework.Inaddition,basedonthePy-IRresultsandcatalyticperformance,the[GaO+]aspecieswithstrongerLewisacidsitesproducedabettersynergismwithmoderateBr?nstedacidsitesandthusimprovedtheselectivitytoaromaticcompounds.However,theimpregnationresultsintheformationofGa2O3phaseandsmallamountsofGaO+speciesthataremainlylocatedontheexternalsurface([GaO+]b),whichcontributetoweakerLewisacidsitesduetoweakerinteractionswiththezeoliteframework.During1-hexenearomatization,thenanosizedGaisomorphouslysubstitutedZSM-5zeolitesamples(Gax-NZ5)exhibitedbettercatalyticperformancecomparedtotheimpregnatedsamples,andthehighestaromaticyield(i.e.,65.4wt%)wasachievedovertheGa4.2-NZ5sample,whichcontainedwiththehighestGacontent.