Promoted effect of zinc–nickel bimetallic oxides supported on HZSM-5 catalysts in aromatization of methanol

(整期优先)网络出版时间:2017-03-13
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Zn/ZSM-5(NZ2)andZn/Ni/ZSM-5(NZ3)asthecatalystsformethanoltoaromatics(MTA)weresynthesizedbyasimpleultrasonicimpregnation.ThetexturalandacidpropertiesofallcatalystswerecharacterizedusingXRD,HRTEM,NH3-TPD,Py-IR,XPS,XRFandTGtechniques.TheXRDandHRTEMresultsshowedthatthebasiczeolitestructureswerenotaffectedmuchwiththeincorporationofZnandNispecies.However,greatchangeshavetakenplaceinacidproperties.ThePy-IRandXPSresultsindicatedthattheZn-Lewisacidsites(ZnOH+species),whichhavestrongerinteractionwiththezeoliteframeworkcomparedwithZnOspecies,weregeneratedattheexpenseofBacidsiteswiththeincorporationofzincspecies.Moreover,theproductanalysisresultsshowedthattheincorporationofzincspeciespromotedtheprimaryaromatizationbyenhancingthedehydroaromatizationandsuppressingthecrackingandsubsequentH-transferreaction.Furthermore,theadditionofNispecieswellinhibitedthelossofzincspeciesbyconvertingpartialZnOspeciestoZnOH+species,andthusimprovedthearomatizationactivityandcatalyststability.ThecatalyticperformanceresultsshowedthattheNZ3possesshigherconversionofmethanolinalongertimeandloweraveragerateofcokeformationcomparedwithNZ2.Inaddition,theNZ3alsoexhibitedthehighestyieldofBTXasthereactionproceeds.