简介:Thecrackingandaromatizationofn-hexaneoverH-ZSM-5modifiedbyvariousrareearthswereinvestigatedbymeansofcontinuousflowmicro-reactor.ThesurfacepropertiesofmodifiedH-ZSM-5catalystswereobtainedfromIR,XRDandXPS.Theresultsshowthattherareearthsenhancethearomatizingpropertiesofthecatalystswhicharepreparedbymechanicalmixturemethod.Theresultsofn-hexanecrackingandaromatizationarecorrelatedwiththeacidity.TheBrnstedacidicsitesaretheactivesitesofn-hexanearomatization,whileLewisacidsiteplaysanimportantroleinn-hexanecracking.
简介:TheexternalsurfaceofHZSM-5zeolitewaspassivatedbyliquidsiliceousdepositionandbyacidicsitespoisoningwithlepidine,respectively.Thenmethanol-to-hydrocarbons(MTH)reactionwasinvestigatedovertheaboveas-preparedcatalystsandthedissolublecokeontheseusedcatalystswasanalyzedbyGC-MS,tostudytheroleoftheexternalsurfaceofHZSM-5inthecatalyticreaction.ComparisonwiththeexperimentalresultsbasedonparentZSM-5showedthattheproductdistributionofMTHreactionwasobviouslyinfluencedbytheexternalsurface.Evidenceswerelistedasfollows:(1)thefinalproductonparentHZSM-5showedhigheraromaticselectivity,lowerolefinselectivity,lowerratioofC2/C3+aliphaticsandhigherratioofC3/C4+aliphaticsthanthereactionmixtureproducedbythesolecatalysisofacidicsitesinHZSM-5channel;(2)alittleofpentamethylbenzeneandhexamethylbenzeneintheproductonparentHZSM-5,wasproducedviamulti-methylationofmethylbenzeneontheexternalsurface.TheaboveconclusionmayalsobesuitableforMTHreactionoverotherzeoliteswith10-ringchannel.
简介:ThecokedepositiononHZSM-5/SAPO-34compositecatalystshasbeenstudiedintheconversionofethanoltopropylene.TheHZSM-5/SAPO-34compositecatalystsweresynthesizedbyhydrothermalmethod(ZS-HS)andfullyblending(ZS-MM).TheusedcatalystswerecharacterizedbyXRD,N2adsorption–desorption,TGA,TPO,elementalanalysis,FTIRandXPS.ThecokingkineticsonbothZS-HSandZS-MMhasbeeninvestigatedandtheircokingrateequationswereobtained.TheusedZS-MMcatalysthadhigheramountofcokeandlowernC:nHthantheusedZS-HS.90%ofthecokewasdepositedinthemicroporesofZS-HS,whilealmost45%ofthecokelocatedinthemicroporesofZS-MM.ThecokedepositedonZS-HScatalystwasmainlygraphite-likecarbonspecies,whereasdehydrogenatedcokespecieswasthemajoronZS-MM.ThecokingactivationenergyofZS-MMwaslowerthanthatofZS-HS,andthecokingrateonZS-MMwasfasterthanonZS-HS.Inaddition,theregenerationofZS-MMcatalystshowedthatithadagoodhydrothermalstability.Thedifferencesoncokingbehaviorsonthetwocatalystswereduetotheirdifferentacidicpropertiesandtextures.
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:Fractionalpyrolysisandone-steppyrolysisofnaturalalgaeCyanobacteriafromTaihuLakewerecomparativelystudiedfrom200to500°C.One-steppyrolysisproducedbio-oilwithcomplexcompositionandlowhighheatingvalue(HHV30.9MJ/kg).FractionalpyrolysisseparatedthedegradationofdifferentcomponentsinCyanobacteriaandimprovedtheselectivitytoproductsinbio-oil.Thatis,acidsat200°C,amidesandacidsat300°C,phenolsandnitrilesat400°C,andphenolsat500°C,weregotasmainproducts,respectively.HZSM-5couldpromotethedehydration,crackingandaromatizationofpyrolyticintermediatesinfractionalpyrolysis.AtoptimalHZSM-5catalystdosageof1.0g,theselectivitytoproductsandthequalityofbio-oilwereimprovedobviously.Themainproductsinbio-oilchangedtonitriles(47.2%)at300°C,indoles(51.3%)andphenols(36.3%)at400°C.Theoxygencontentwasreducedto7.2wt%and9.4wt%,andtheHHVwasraisedto38.1and37.3MJ/kgat300and400°C,respectively.Fractionalcatalyticpyrolysiswasproposedtobeanefficientmethodnotonlytoprovideapotentialsolutionforalleviatingenvironmentalpressurefromwaterblooms,butalsotoimprovetheselectivitytoproductsandobtainhighqualitybio-oil.
简介:采用BET、FT-IR、XRD、29Si-NMR、27Al-NMR等分析手段,研究了不同硅铝比的HZSM-5分子筛微观结构及其在醛氨缩合中的催化性能.结果表明,不同硅铝比的HZSM-5分子筛,在FT-IR谱图约1219,1102,950,799,447cm-1处有差异;在29Si-NMR谱中存在2个峰,A峰(-113.4)往高化学位移方向移动,B峰(-109.7)逐渐减弱直至消失;在27Al-NMR谱中存在1个峰,此峰(55.3)往低化学位移方向移动.醛氨缩合反应用HZSM-5分子筛催化剂的最适宜硅铝比范围在90~170之间,在此催化剂上合成烷基吡啶,收率可达89.8%.
简介:将SO4^2-/TiO2-HZSM-5负载镧制备了新型催化剂SO4^2-/La2O3-TiO2-HZSM-5,以对羟基苯甲酸和丙醇的酯化反应为探针,考察了不同制备条件对催化剂性能的影响。结果表明:la^3+浸渍浓度为0.07mol/L,经110℃烘干后于500℃焙烧3h所得催化剂活性最好。对影响酯化反应的因素进行考察,最佳实验条件为n(醇)∶n(酸)=5∶1,反应时间4h,催化剂用量3.0%(总物料),酯化率可达96.0%。且该催化剂具有良好的重复使用和再生能力,适宜合成对羟基苯甲酸酯。