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K改性β-Mo2C催化剂CO加氢合成低碳混合醇的研究

Mixed alcohols synthesis from CO hydrogenation over potassium-promoted β-Mo2C catalysts

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【作者】 向明林李德宝肖海成齐会杰李文怀孙予罕钟炳

【Author】 XIANG Ming-lin~(1,2),LI De-bao~1,XIAO Hai-cheng~(1,2),QI Hui-jie~1,LI Wen-huai~1,SUN Yu-han~1,ZHONG Bing~1(1.State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China;2.Graduate University of the Chinese Academy of Sciences,Beijing 100039,China)

【机构】 中国科学院山西煤炭化学研究所煤转化国家重点实验室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中国科学院研究生院北京100039山西太原030001

【摘要】 制备系列K改性的β-Mo2C催化剂并对其CO加氢合成低碳混合醇性能进行了考察。结果表明,K改性使β-Mo2C催化剂的CO加氢选择性发生显著变化。β-Mo2C催化剂CO加氢的产物主要为C1~C4烷烃,经K改性后β-Mo2C催化剂上产物主要为C1~C5低碳醇,其中高级醇(C2+OH)选择性可达到33.78%。通过对碱金属质量分数的考察发现,当K/Mo(原子比)为0.2时,总醇选择性达到最大值,低碳醇的时空收率达到0.12 g/(mL.h-1)。β-Mo2C催化剂上醇烃产物均符合线性An-derson-Schu ltz-F lory(A-S-F)分布曲线,而K改性β-Mo2C催化剂上醇产物为独特的甲醇负偏离A-S-F分布。可见,K助剂的加入有效促进了低碳醇的形成,尤其是促进了C1OH到C2OH的链增长步骤。

【Abstract】 The modification effects of K2CO3 on β-Mo2C catalysts for mixed alcohols synthesis from CO hydrogenation were studied.Un-prompted β-Mo2C produced mainly hydrocarbons of C1-C4 under the reaction conditions of 573K,8.0MPa,H2/CO=1.0,GHSV=2000h-1.Addition of K2CO3 to β-Mo2C resulted in remarkable selectivity shift from hydrocarbons to alcohols.Moreover,the promoter of potassium enhanced the ability of chain propagation of β-Mo2C with the higher selectivity of C2+ alcohols.The investigations of the loadings of K2CO3 in β-Mo2C revealed that the maximum of alcohol yield obtained at K/Mo(molar ratio) =0.2.On K/β-Mo2C catalysts,the distribution of hydrocarbons obeyed the traditional linear Anderson-Schultz-Flory equation,while the distribution of alcohols gave a unique linear Anderson-Schultz-Flory with remarkable deviation of methanol.Thus,potassium promoter exerted a prominent function on the whole chain propagation to produce alcohols especially for the stage of methanol to ethanol.

  • 【文献出处】 燃料化学学报 ,Journal of Fuel Chemistry and Technology , 编辑部邮箱 ,2006年02期
  • 【分类号】TQ223
  • 【被引频次】30
  • 【下载频次】341
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