简介:ThecatalyticactivityofFe/ZSM-5fortheselectivereductionofNOtoN2withmethaneinthepresenceofexcessO2wasstudied.Fe/ZSM-5catalystswithvariousFeloadingswerepreparedbyimpregnationmethod.ItiswellknownthatmethaneisinactivewhenFe/ZSM-5asthecatalystfortheselectivecatalyticreduction(SCR)ofNOwithmethane.However,thispapershowsthatwhenthecontentofFewasabout0.5%,Fe/ZSM-5showedhighercatalyticactivityandselectivityofmethane,andputforwardmeasurableactivationforCH4isanimportantfactorforthereactionofremovalofNOxwithCH4.
简介:TheinfluenceofmischmetaladditiononphysicochemicalpropertiesofPtSnNa/ZSM-5catalystwasstudiedbymeansofXRF,H2chemisorption,XRD,TPR,NH3-TPDandTPOtechniques.TheresultsshowedthatthepresenceofmischmetalhadanobviousimpactonthecatalyticperformanceofthePtSnNa/ZSM-5catalyst.AsuitablecontentofmischmetalnotonlycouldenhancetheinteractionsbetweenPtspeciesandthesupport,butalsoinhibittheformationofcokeduringthereaction,thusimprovingthecatalyticactivityandstability.Inourexperiments,whenthecontentofmischmetalwas3m%,thecatalystexhibitedbestcatalyticperformance.However,thecontinuousadditionofmischmetalcouldpromotethereductionofSnspeciestometallictin,whichwasdisadvantageoustothereaction.
简介:AseriesofZSM-5zeolites,withthemorphologiesofsphere,spherewithcubicparticlesonthesurface,andcubicparticles,weresynthesizedbyhydrothermalmethodusingn-butylamineasthetemplate,assistedbytheadditionofNaClandcrystalseed.X-raydiffraction(XRD),scanningelectronmicroscope(SEM),X-rayfluorescence(XRF)andtemperature-programmeddesorptionofammonia(NH3-TPD)wereusedtocharacterizethesesamples.Thesamplesweretestedwithtoluenemethylationreaction.Themodifiedsamplecomposedofsphericalparticleswith3μmcrystalparticlesonthesurfacehadapara-xyleneselectivityof95%andmaintained79%oftheinitialconversionafterrunningthereactionfor50h.Thismodifiedsampleshowedthebeststabilityamongthetestedthreemodifiedsamples.
简介:CarbondepositionduringmethanoltohydrocarbonsleadstothequickdeactivationofZSM-5catalystanditisoneofthemajorproblemsforthistechnology.DecreasingthecrystalsizeorintroducingmesoporesintoZSM-5zeolitescanimproveitsdiffusionpropertyanddecreasethecokeformation.Inthispaper,nano-sizedZSM-5zeolitewithintercrystallinemesoporescombiningthemesoporousandnanosizedstructurewasfabricated.Forcomparison,themesoporousZSM-5andnano-sizedZSM-5werealsoprepared.ThesecatalystsampleswerecharacterizedbyXRD,BET,NH3-TPD,TEM,Py-IRandTGtechniquesandusedontheconversionofmethanoltogasolineinafixed-bedreactoratT=405°C,WHSV=4.74h-1andP=1.0MPa.Itwasfoundthattheexternalsurfaceareaofthenano-sizedZSM-5zeolitewithintercrystallinemesoporesreached104m2/g,largerthanthatofmesoporousZSM-5(66m2/g)andnanosizedZSM-5(76m2/g).Catalyticlifetimeofthenano-sizedZSM-5zeolitewithintercrystallinemesoporeswas93h,whichwasonlylongerthanthatofmesoporousZSM-5(86h),butshorterthanthatofnanosizedZSM-5(104h).Strongaciditypromotedthecokeformationandthusdecreasedthecatalyticlifetimeofthenano-sizedZSM-5zeolitewithintercrystallinemesoporesthoughitpresentedlargeexternalsurfacethatcouldimprovethediffusionproperty.Thespecialzeolitecatalystwasfurtherdealuminatedtodecreasethestrongacidity.Afterthis,itscokeformationratewasslowedandcatalyticlifetimewasprolongedto106hbecauseofthelargeexternalsurfaceareaanddecreasedweakacidity.Thisspecialstructuralzeoliteisapotentialcatalystformethanoltogasolinereaction.
简介:FreshZSM-5zeolitecatalystswerepretreatedat460℃and500℃withvariouscumulativeamountofwaterfeed(CAWF)inafixedbedreactor.Thecatalyticprocesswascarriedoutunderthefollowingconditions:atemperatureof480℃;amethanolWHSVof3h-1;amethanolpartialpressureof30kPa;andatimeonstreamof12h,24hand48h,respectively.TheBETparametersofcatalystsanddiffusioncoefficientsoftolueneshowedthatthereweretwotypesofmesoporesgeneratedunderdifferenthydrothermalconditions.MildtemperatureandmoderateCAWFconditionsledtoexternalopenmesoporeswhichcouldbeenteredfromtheexternalsurfaceofthezeolite,whileahightemperatureorahighCAWFconditionresultedinthegenerationofmacroporesorinternalisolatedmesopores,whichwereoccludedinthemicroporousmatrix.TheTGAresultsshowedthatcatalystwithexternalopenmesoporeshadgoodabilitytoresistcokeaccumulationandgoodperformanceonpropyleneselectivity,whiletheinternalisolatedmesoporesdidnocontributetotheincreaseddiffusivityofreactantsandproducts.
简介:<正>ZSM-5/MCM-41compositemolecularsievewaspreparedbythenano-assemblingmethod.TheZSM-5molecularsieve,theMCM-41molecularsieve,theZSM-5/MCM-41mechanicalmixtureandtheZSM-5/MCM-41compositemolecularsievewerecharacterizedbyX-raypowderdiffractometry,N2adsorptionisotherms,temperatureprogrammeddesorptionofammoniaandscanningelectronmicroscopyandtheirpropertieswereanalyzed.UsingFCCgasolineasthefeed,activitiesofdifferentmolecularsievesforreducingolefincontentwereinvestigatedinacontinuoushigh-pressuremicro-reactorunitunderthefollowingconditions:areactiontemperatureof400℃,areactiontimeof2h,aweighthourlyspacevelocityof3h-1,andareactionpressureof2.0MPa.TheresultsshowedthattheHMCM-41molecularsievehadlowreactionperformance,andtheHZSM-5molecularsievedemonstratedhigharomatizationactivity,whiletheZSM-5/MCM-41compositemolecularsieveexhibitedabestolefin-reducingperformancebecauseofitshighisomerizationactivityandmoderatearomatizationactivity.Withalargestolefin-reducmgcapabilityandareasonabledistributionofproducts,thecompositemolecularsievewasmoresuitableforFCCgasolineupgradingcomparedtootherthreecatalysts.
简介: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.
简介:Micro-mesoporouscompositemolecularsievesH-ZSM-5/MCM-41werepreparedbythehydrothermaltechniquewithalkali-treatedH-ZSM-5zeoliteasthesourceandcharacterizedbyscanningelectronmicroscopy,transmissionelectronmicroscopy,energydispersivespectroscopy,X-raydiffraction,N2adsorption-desorptionmeasurementandNH3temperature-programmeddesorption.ThecatalyticperformancesforthemethanoldehydrationtodimethyletheroverH-ZSM-5/MCM-41wereevaluated.Amongthesecatalysts,H-ZSM-5/MCM-41preparedwithNaOHdosage(nNa/nSi)varyingfrom0.4to0.47presentedexcellentcatalyticactivitywithmorethan80%methanolconversionand100%dimethyletherselectivityinawidetemperaturerangeof170—300℃,andH-ZSM-5/MCM-41preparedwithnNa/nSi=0.47showedconstantmethanolconversionofabout88.7%,100%dimethyletherselectivityandexcellentlifetimeat220℃.Theexcellentcatalyticperformanceswereduetothehighlyactiveanduniformacidicsitesandthehierarchicalporosityinthemicro-mesoporouscompositemolecularsieves.ThecatalyticmechanismofH-ZSM-5/MCM-41forthemethanoldehydrationtodimethyletherprocesswasalsodiscussed.
简介:综述了近年来ZSM-5沸石分子筛的合成及表面改性研究进展.合成方面重点介绍了有机胺合成、无机胺合成及负载合成方法;表面改性方面重点介绍了水蒸气改性、离子交换改性及化学气相沉积改性方法.
简介:Inthisworktypicalmechanicalpropertiesforacatalystsupportmaterial,ZSM5(aspray-driedgranularzeolite),havebeenmeasuredinordertorelatethebulkbehaviourofthepowdermaterialtothesingleparticlemechanicalproperties.Particleshapeandsizedistributionofthepowders,determinedbylaserdiffractionandscanningelectronmicroscopy(SEM),confirmedthesphericalshapeofthespray-driedparticles.TheexcellentflowabilityofthematerialwasassessedbytypicalmethodssuchastheHausnerratioandtheCarrindex.Thiswasconfirmedbybulkmeasurementsoftheparticle-particleinternalfrictionparameterandflowfunctionusingaSchulzeshearcell,whichalsoillustratedthelowcompressibilityofthematerial.SingleparticlecompressionwasusedtocharacterizesingleparticlemechanicalpropertiessuchasreducedelasticmodulusandstrengthfromHertzcontactmechanicstheory.Comparisonwithsurfacepropertiesobtainedfromnanoindentationsuggestsheterogeneity,thesurfacebeingharderthanthecore.Inordertoevaluatetherelationshipbetweensingleparticlemechanicalpropertiesandbulkcompressionbehaviour,uniaxialconfinedcompressionwascarriedout.ItwasdeterminedthattheAdamsmodelwassuitablefordescribingthebulkcompressionandfurthermorethattheAdamsmodelparameter,apparentstrengthofsingleparticles,wasingoodagreementwiththesingleparticlestrengthdeterminedfromsingleparticlecompressiontest.
简介:TheepoxidationofallylchloridewithH2O2onTi-ZSM-5preparedbyisomorphoussubstitutionofHZSM-5withTiCl4gaswasstudied.TheresultsshowthatTi-ZSM-5hasahighcatalyticefficiencyfortheepoxidationofallylchloride.TheH2O2utilizationreaches99.50%whentheallylchloride/H2O2molarratiois>1.Theeffectofsolventspecies,catalystconcentration,H2O2andallylchlorideconcentrationandreactiontemperatureontheepoxidationwasinvestigatedsimultaneously.Itisfoundthatmethanolisthebestsolventforthereaction.Thereactionrateequationwithv=k[Cat.][H2O2]1/2-[C3H5Cl]andtheapparentactivationenergywithEa=63.462kJ/molareobtainedaccordingtothekineticsstudy.
简介:碱性体系中以水玻璃和硅溶胶为双硅源,硫酸铝为铝源,在硅铝酸盐凝胶形成过程中加入氧氯化锆,用水热晶化法成功合成了Zr-ZSM-5分子筛。通过XRD、Raman、UV-VIS、BET、SEM、NH3-TPD、Py-IR等手段对其进行表征。研究结果表明:Zr成功进入ZSM-5分子筛骨架,且随着锆摩尔含量的增加,分子筛的比表面积减小,孔径和孔体积增大,势必会影响到分子筛的择形催化性能;此外,分子筛的酸类型重新分布,L酸比例增大,总酸量和酸强度有所减小,势必会影响其酸催化性能;同时分子筛的生长方式也发生了改变,晶体结构由三维棺状变为二维层片状,相对结晶度有所降低,但其骨架结构依然保持完整。
简介:试验制备了Pd/CeO2-ZSM-5/CC催化剂,测定了其对低中温尾气CO的催化净化活性。试验表明,Pd/CeO2-ZSM-5/CC催化剂具有良好的催化活性,Pd负载量大的催化剂活性越好。CO初始浓度为100ppm,O2浓度为21%,空速为100000h-1时,0.4%Pd催化剂的T100为192℃。