简介: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.
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:Unlikeorganic–inorganichybridperovskites,all-inorganiccesiumleadhalideperovskitesholdgreatpromisefordevelopinghigh-performanceoptoelectronicdevices,owingtotheirimprovedstability.Herein,weinvestigatetheperovskite-relatedCsPb2Br5nanoplatelets(NPLs)withtunableemissionwavelengthsviachangingthereactiontemperaturesto100°C,120°C,and140°C.ReactiontemperatureplaysakeyroleindeterminingtheshapesandthicknessesoftheresultingCsPb2Br5NPLs.AhighertemperatureisinfavoroftheformationofsmallerandthickerNPLs.Todeveloptheirpotentialapplicationsinoptoelectronicdevices,greenlightemittingdiodes(LEDs)andphotodetectorsbasedonCsPb2Br5NPLsarefabricated.ThegreenLEDsbasedonCsPb2Br5NPLssynthesizedat140°Cexhibitanexcellentpuregreenemission(fullwidthathalf-maximumof<20nm)anddisplayaluminousefficiencyof34.49lm∕Wunderanoperationcurrentof10mA.Moreover,thephotodetectorbasedonCsPb2Br5NPLssynthesizedat100°Chasbetterperformancewitharisetimeof0.426s,adecaytimeof0.422s,andaratioofthecurrent(withandwithoutirradiation)of364%.
简介:Aserialofprotonatedandlayeredtransitionmetaloxides,includinglayeredHTaWO6,HNbMoO6aswellasHNbWO6,weresynthesizedbysolid-statereactionandion-exchange.ThelayeredHTaWO6hasbeensystematicallystudiedasasolidacidtorealizethedehydrationoffructoseto5-hydroxymethylfurfural(HMF).ThetransitionmetaloxidesampleswerecharacterizedwithICP-OES,EDS,XRD,XPS,SEM,TGA,FT-IR,N2adsorption–desorptionandNH3-TPD.Theinfluentialfactorssuchasreactiontemperature,reactiontime,solvent,catalystamountandsubstrateconcentrationweredeeplyinvestigated.Theoptimizedfructoseconversionrateof99%withHMFyieldof67%wereachievedafter30minat140°Cindimethylsulfoxide.
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:建立了一种电感耦合等离子体质谱(ICP-MS)法测定环境水样中Cu、Zn、Mn、Pb、Cd5种重金属元素含量的方法。经过仪器条件优化和干扰校正后,方法中5种元素的工作曲线的相关系数均大于0.999,检出限为0.014-0.22μg/L。对加入国家标准物质作为质控样15个批次的环境水样进行统计分析并绘制质控图。同时与原子吸收光谱法测定结果进行对比分析,测定值与标准值基本一致,质控样的测定值基本都在控制线范围之内。结果表明,方法精密度和准确度均能满足环境水样的分析,ICPMS法更适用于大批量、多样化环境水样的监测分析。
简介:Theneworganic-inorganiccompound,[C_6H_7N_2O_2]_3TeCl_5·2Clwassynthesizedanditsstructurewasdeterminedatroomtemperatureinthetriclinicsystem(P~-1)withthefollowingparameters:a=10.5330(11)?,b=10.6663(11)?,c=15.9751(16)?,α=82.090(2)°,β=71.193(2)°,γ=68.284(2)°andZ=2.ThefinalcycleofrefinementledtoR=0.057andRw=0.149.ThecrystalstructurewasstabilizedbyanextensivenetworkofN--H···Clandnon-classicalC--H···Clhydrogenbondsbetweenthecationandtheanionicgroup.Severalthermalanalysistechniquessuchasthermogravimetricanalysis,differentialscanningcalorimetricanalysisandevolvedgasanalysiswereused.Weusedisoconversionalkineticsmethodstodeterminethekineticsparameters.Weobservethatthedecompositionof[C_6H_7N_2O_2]_3TeCl_5·2Clentailstheformationhydrochloricacidofnitroanilineasvolatiles.Theinfraredspectrawererecordedinthe4000–400cm~(-1)frequencyregion.TheRamanspectrawererecordedintheexternalregionoftheanionicsublatticevibration50–1500cm~(-1).TheopticalbandgapwascalculatedfromtheUV-VisabsorbancespectrausingclassicalTaucrelationwhichwasfoundtobe3.12and3.67eV.