SiO_2催化合成气制低碳醇性能的影响.pdf

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1、物理化学学~(WuliHuaxueXuebao1NovemberActa尸．一Chim．Sin．2011，27(11)，2639-26452639[Article】www．whxb．pku．edu．cnCe添加对Cu．Fe，SiO2催化合成气制低碳醇性能的影响毛东森郭强胜俞俊韩璐蓬卢冠忠(上海应用技术学院化学与环境工程学院应用催化研究所，上海200235)摘要：采用共浸渍法制备了添加不同Ce含量(相对于SiO的摩尔分数为0-20％)的Ce-Cu-Fe／SiO催化剂，在连续流动微型固定床反应器中考察了其催化CO加氢合成低碳醇反应的性能，并采用X

2、射线衍射(XRD)、低温N吸附、程序升温还原(H．TPR)、CO吸附傅里叶变换红外光谱(CO-FTIR)~ICO程序升温脱附(co-TPD)技术对催化剂进行了表征．结果表明：添加适量的Ce，一方面降低了Cu的晶粒大小，提高了Cu的分散度，进而提高了对CO的吸附能力：另一方面掺入的Ce和Cu之间存在相互作用，提高了CO解离和非解离吸附的能力，从而有利于CH的生成和CO的插入反应．上述两方面的共同作用同时提高了Cu．Fe／SiO：催化剂的活性和醇的选择性．当Ce含量为1O％时，在压力为3．0MPa，温度为250。C，空速为6000mL·g～·和H

3、，CO摩尔比为2的反应条件下，Ce．Cu．Fe／SiO催化剂上醇的时空产率达到121．0g·kg～·，比未添加Ce的Cu—Fe／SiO催化剂的时空产率(58．0g·kg～·h1)提高了一倍以上．关键词：铈助剂：Cu—Fe／SiO催化剂：合成气：催化加氢：低碳醇中图分类号：O643EfectofCeriumAdditionontheCatalyticPerformanceofCu·Fe／Si02fortheSynthesisofLowerAlcoholsfrOmSyngasMAODong—SenGUOQiang-ShengYUJunHANLu-

4、PengLUGuan—Zhong(ResearchInstituteofAppliedCatalysi5SchoolofChemicalandEnvironmentalEngineering,ShanghaiInstituteofTechnology,Shanghai20023LR．China)Abstract：AseriesofCe．Cu．Fe／SiO2catalystswithdifferentCecontents(molefractionrelativetoSiO2，0-20％1werepreparedbyco-impregnation

5、andtheircatalyticperformancesforCOhydrogenationtoloweralcoholswereinvestigatedusingacontinuousflowfixedbedmicro．reactor．ThesecatalystswerecharacterizedbyX-raydiffraction(XRD)，N2-adsorption，temperature—programmedreductionofH2(H2一TPR)，FouriertransforminfraredofCOadsorption(CO

6、-FTIR)，andtemperature-programmeddesorptionofCOfCO．TPD)．TheresultsshowedthattheadditionofanappropriateamountofCedecreasedtheCucrystalsizeandpromotedthedispersionofCu．whichgreatlyincreasedtheamountofadsorbedCO．Additionally．theinteractionofdopedCewithCuincreasedtheassociativea

7、nddissociateadsorptioncapacityofCO．whichisfavorablefortheformationofCHandtheinsertionreactionofadsorbedCOtoCHBoththeactivityandalcohoIselectivityoftheCu．Fe／SiO2catalystjncreasedunderthecombinedefectoftheabove．mentionedtwoaspects．AtaCecontentof10％．thespacetimeyieldofloweralc

8、oholsimprovedfrOm58．0g·kg～·h～overtheCu-Fe／SiO2catalystto121．0g·kg～·hovertheCe—Cu—F