新能源材料 投稿：杜咊咋.doc

新能源材料 投稿：杜咊咋 CatalysisToday131(2008)278–284 /locate/cattod CatalyticconversionofmethaneandCO2tosynthesisgasoveraLa2O3-modi?edSiO2supportedNicatalystin?uidized-bedreactor JingGaoa,ZhaoyinHoua,*,JianzhongGuoa,b, YinghongZhuc,XiaomingZhenga,* InstituteofCatalysis,DepartmentofChemistry,ZhejiangUniversity(XixiCampus),Hangzhou310028,China b DepartmentofChemistry,ZhejiangForestryUniversity,311300Lin’an,China c CollegeofChemicalEngineeringandMaterials,ZhejiangUniversityofTechnology,Hangzhou310012,China Availableonline26November2007 a Abstract Inthiscontribution,acommercialsphericalSiO2wasmodi?edwithdifferentamountsofLa2O3,andusedasthesupportofNicatalystsforautothermalreformingofmethaneina?uidized-bedreactor.Nitrogenadsorption,XRDandH2-TPRanalysisindicatedthatLa2O3-modi?edSiO2hadhighersurfacearea,strengthenedinteractionbetweenNiandsupport,andimproveddispersionofNi.CO2-TPDfoundthatLa2O3increasedthealkalescenceofSiO2andimprovedtheactivationofCO2.Cokingreaction(viabothtemperature-programmedsurfacereactionofCH4(CH4-TPSR)andpulsedecompositionofCH4)disclosedthatLa2O3reducedthedehydrogenationabilityofNi.CO2-TPO,O2-TPO(followedafterCH4-TPSR)con?rmedthatonlypartamountofcarbonspeciesderivedfrommethanedecompositioncouldberemovedbyCO2,andO2infeedplayedacrucialroleforthegasi?cationoftheinactivesurfacecarbons.Ni/xLa2O3-SiO2(x=10,15,30)possessedhighactivityandexcellentstabilityforautothermalreformingofmethaneina?uidized-bedreactor.#2007ElsevierB.V.Allrightsreserved. Keywords:Autothermalreformingofmethane;Ni/La2O3-SiO2catalysts;Synthesisgas;Fluidized-bedreactor 1.Introduction MethaneautothermalreformingwithCO2andoxygen(abbreviatedasMATR)hasbeenasubstantialinterestinrecentyearsinattractivealternativeroutesforconversionofnaturalgas(methane)tosynthesisgasforitslow-energyrequirementandawildrangeofH2/COratiobymanipulatingtherelativeconcentrationsofCO2andO2infeed[1–10].Atthesametime,RuckensteinandHurecommendedthatthiscombinedreactionscouldovercometheexplosionsth