活性组分浸渍顺序对ni_sn_cr_活性炭催化乙酸甲酯气相羰基化合成醋酐性能的影

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1、石油化工2010年第39卷第4期PETROCHEMICALTECHNOLOGY·377·活性组分浸渍顺序对Ni-Sn-Cr/活性炭催化乙酸甲酯气相羰基化合成醋酐性能的影响1,211贾庆龙,谭猗生,韩怡卓(1.中国科学院山西煤炭化学研究所煤转化国家重点实验室,山西太原030001;2.中国科学院研究生院,北京100049)[摘要]以活性炭(AC)为载体,采用等体积浸渍法,按照活性组分浸渍顺序的不同制备了一系列Ni-Sn-Cr/AC催化剂;在连续流动固定床反应器上考察了Ni-Sn-Cr/AC催化剂催化乙酸甲酯气相羰基化合成醋酐的性能,并采用XRD和N2物理吸附法对催化剂的物相和织

2、构性质进行了表征。实验结果表明,在催化剂制备过程中3种活性组分Ni,Sn,Cr的加入顺序对Ni-Sn-Cr/AC催化剂的活性有较大影响;先浸渍Ni组分然后同时浸渍Sn和Cr组分的Ni/Sn-Cr/AC催化剂的活性最高,在n(CO)∶n(H)=8、n(乙酸甲酯)∶n(CHI)=7、n(CO)∶n(乙酸甲酯)=4、反应温度205℃、反应压力5.5MPa、气态空速1200h-1的条23件下,Ni/Sn-Cr/AC催化剂上乙酸甲酯的转化率为38.5%,醋酐的选择性为80.3%。不同浸渍顺序制备的Ni-Sn-Cr/AC催化剂的织构性质并不是催化剂活性的决定因素。[关键词]活性组分;浸渍

3、顺序;镍-锡-铬催化剂;羰基化;乙酸甲酯;醋酐;活性炭[文章编号]1000-8144(2010)04-0377-05[中图分类号]TQ426.8[文献标识码]AEffectsofActiveComponentImpregnationSequenceonActivitiesofNi-Sn-Cr/ActivatedCarbonCatalystsinGasPhaseCarbonylationofMethylAcetatetoAceticAnhydride1,211JiaQinglong,TanYisheng,HanYizhuo(1.StateKeyLabofCoalConversi

4、on,InstituteofCoalChemistry,ChineseAcademyofSciences,TaiyuanShanxi030001,China;2.GraduateSchoolofChineseAcademyofSciences,Beijing100049,China)[Abstract]Withdifferentimpregnationsequencesofactivecomponents,aseriesofNi-Sn-Crcatalystssupportedonactivatedcarbon(AC)werepreparedthroughimpregnatio

5、n.Catalyticperformancesofthepreparedcatalystsingasphasecarbonylationofmethylacetate(MeOAc)toaceticanhydride(AcOAC)wereevaluatedinacontinuousflowfixed-bedreactor.PhasestatesandtexturalpropertiesofthecatalystswereanalyzedbymeansofXRDandN2physicaladsorption.Experimentalresultsindicatedthatimpr

6、egnationsequencesofNi,SnandCrplayedanimportantpartforperformancesofNi-Sn-Cr/ACcatalystsinthecarbonylation.Ni/Sn-Cr/ACcatalyst(firstimpregnationwithNiandthenco-impregnationwithSnandCr)wasthehighestinthecatalyticactivityunderreactionconditionsofn(CO)∶n(H2)8,n(MeOAc)∶n(CH3I)7,n(CO)∶n(MeOAc)4,2

7、05℃,-15.5MPaandGHSV1200h.MeOAcconversionandAcOAcselectivityreached38.5%and80.3%,respectively.TexturalpropertiesofNi-Sn-Cr/ACcatalystswithdifferentimpregnationsequencesofactivecomponentswerenotdeterminantfactorfortheiractivities.[Keywords]activecomponent;