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1、物理化學(xué)學(xué)報(WuliHuaxueXuebao)ActaPhys.一Chim.Sin.2014,3D(11),2127—21332127November【Article】doi:10.3866/PKU.WHXB201409121www.whxb.pku.edu.caCe.Cu.Co/CNTs催化劑催化合成氣制低碳醇及乙醇的研究韓濤,,黃偉,王曉東唐鈺’劉雙強’游向軒’(‘太原理工大學(xué)煤科學(xué)與技術(shù)教育部和山西省重點實驗室,太原030024;z中國科學(xué)院山西煤炭化學(xué)研究所煤轉(zhuǎn)化國家重點實驗室,太原030001)摘要
2、:采用共浸漬法制備了不同Ce含量的Ce.Cu.Co,CNTs催化劑,考察了其在合成氣制低碳醇反應(yīng)中的催化性能,借助X射線衍射(XRD)、程序升溫還原(H.TPR)、Nz吸脫附實驗(BET)、透射電鏡(TEM)和CO程序升溫脫附(CO.TPD)對這些催化劑進行了表征.結(jié)果表明,當(dāng)Ce的質(zhì)量分?jǐn)?shù)為3%時,低碳醇的時空收率和選擇性達到最高,分別為696.4mg·g·h和59.7%,其中乙醇占總醇的46.8%,適量Ce的添加能提高Cu物種在催化劑上的分散度和催化劑的還原性能,能顯著地增加催化劑吸附CO的能力,促進合成醇
3、活性位的形成,進而明顯提高催化劑的活性和總醇的選擇性.研究表明,將具有高活性和高碳鏈增長能力的CuCo基催化劑與碳納米管的限域效應(yīng)結(jié)合,可實現(xiàn)縮窄產(chǎn)物分布、大幅度提高乙醇選擇性的目的.關(guān)鍵詞:Ce;CuCo/CNTs催化劑:合成氣:低碳醇:乙醇中圖分類號:0643StudyofCe--Cu--Co/CNTsCatalystsfortheSynthesisofHigherAlcoholsandEthanolfromSyngasHANTao’HUANGWei’。WANGXiao—Dong’_TANGYu’LIUSh
4、uang·QiangYOUXiang—Xuan’('KeyLaboratoryofCoalScienceandTechnologyofMinistryofEducationandShanxiProvince,TaiyuanUniversityofTechnology,Taiyuan030024,R.China;StateKeyLaboratoryofCoalConversion.InstituteofCoalChemistry,ChineseAcademyofSciences,Taiyuan030001,PR.
5、China)Abstract:AseriesofCe-Cu—Co/carbonnanotubesfCNTS)catalystswithdiferentCecontentswerepreparedbycO-impregnation,andthecatalyticperformancewasinvestigatedforthesynthesisofhigheralcoholsfrOmsyngas.ThecatalystswerecharacterizedbyX—raydi仟ractionfXRD),temperat
6、ure—programmedreductionofH2(H2-TPR),N2adsorption—desorptionisotherms(BET),transmissionelectronmicroscopy(TEM),andtemperature-programmeddesorptionofCO(CO—TPD).TheresultsshowedthatataCecontentof3%thecatalysthadthehighestcatalyticactivity.Theformationrateandsel
7、ectivityofalcohoIreached696.4mq·a·h~and59-7%.wherethemassfractionofethanolwas46.8%ofthetotaIamountofalcohols.TheadditionofanappropriateamountofCefacilitatedthedispersionofCuandpromotedreductionofthecatalysts.1talsomarkedlyincreasedtheadsorptioncapacityforCO.
8、andsignificantlyimprovedtheformationofactivesitesforalcohols.whichjsfavorableforthecatalyticactivityandtoimprovetheselectivityofalcohols.ResearchshowedthatcombiningtheCuCo-basedcatalyst,whichhas