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1、物理化学学报(WuliHuaxueXuebao)MayActaPhys.鄄Chim.Sin.,2008,24(5)：833-838833[Article]www.whxb.pku.edu.cnZn、Mn助剂对CuFe合成低碳醇催化剂的影响1,2111,鄢林明桂房克功李德宝孙予罕(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,太原030001;2中国科学院研究生院,北京100049)摘要：研究了锌、锰助剂对CuFe合成低碳醇催化剂结构及性能的影响.低温N2吸附、X射线衍射(XRD)和H2鄄程序升温还原(H2鄄TPR)结果表明,锌的添加导致催化剂比
2、表面下降,不利于活性相的分散;而锰则促进铜铁的分散,增加了铜铁的接触面积,有利于二者之间的相互作用.CO吸附的漫反射红外光谱(DRIFT)表明,锌增强了铁对CO的吸附能力,这种效应与ZnFe2O4的形成有直接关系;而锰助剂由于稀释效应,减弱了铁对CO吸附能力和链增长能力.催化剂的反应性能测试表明,与CuFe催化剂相比,CuZnFe催化剂的活性大幅度提高,但C2+醇选择性下降;CuFeMn催化剂的活性却有所下降,C2+醇选择性也降低,但总醇的选择性提高.双助剂修饰的催化剂表现出明显的协同效应,改变了催化剂的织构,降低了Cu的还原温度,修饰了Fe的还原性
3、能.更重要的是,Zn和Mn的添加显著增强了CO在催化剂表面的吸附量.催化剂催化性能总体上优于CuZnFe和CuFeMn催化剂.关键词：低碳醇合成;CuFe催化剂;锌助剂;锰助剂;协同效应中图分类号：O643EffectofZnandMnPromotersonCopper鄄IronBasedCatalystsforHigherAlcoholSynthesis1,2111,鄢LINMing鄄GuiFANGKe鄄GongLIDe鄄BaoSUNYu鄄Han(1StateKeyLaboratoryofCoalConversion,InstituteofCoal
4、Chemistry,ChineseAcademyofSciences,Taiyuan030001,P.R.China;2GraduateSchooloftheChineseAcademyofSciences,Beijing100049,P.R.China)Abstract：TheinfluencesofzincandmanganesepromotersonthestructureandreactionbehaviorofCuFecatalystforhigheralcoholsynthesiswereinvestigatedbyN2adsorptio
5、n,X鄄raydiffraction(XRD),H2temperature鄄programmedreduction(H2鄄TPR),insitudiffusereflectanceinfraredspectroscopy(DRIFT)andCO+H2reaction.ItwasfoundthatthezincadditivesuppressedthedispersionofactivephasesbutimprovedtheiractivationabilitytowardsCOmoleculeduetotheformationofanewspine
6、lphase,ZnFe2O4.ThepresenceofmanganeseshowedamorefavorableeffectonthedispersionofactivephasesandthenpromotedthesynergisticeffectbetweencopperandironalthoughtheadsorptiontendencytowardsCOdeclinedduetothedilutioneffectofmanganese.ComparedwithbinaryCuFecatalyst,CuZnFecatalysthadahi
7、gheractivitywiththedecreasingofC2+OHselectivity,andCuFeMncatalystshowedimprovedtotalalcoholselectivityalthoughbothCOconversionandC2+OHselectivitydecreased.TheresultsofthedoublypromotedCuFecatalystevidentlyindicatedtheexistenceofsynergisticeffectbetweenzincandmanganese,whichmodi
8、fiedthetextureparameters,decreasedthereductiontemperat
