Ce-Cu-Co/CNTs催化剂催化合成气制低碳醇及乙醇的研究

采用共浸渍法制备了不同Ce含量的Ce-Cu-Co/CNTs催化剂,考察了其在合成气制低碳醇反应中的催化性能,借助X射线衍射(XRD)、程序升温还原(H2-TPR)、N2吸脱附实验(BET)、透射电镜(TEM)和CO程序升温脱附(CO-TPD)对这些催化剂进行了表征.结果表明,当Ce的质量分数为3%时,低碳醇的时空收率和选择性达到最高,分别为696.4 mg?g-1?h-1和59.7%,其中乙醇占总醇的46.8%,适量Ce的添加能提高Cu物种在催化剂上的分散度和催化剂的还原性能,能显著地增加催化剂吸附CO的能力,促进合成醇活性位的形成,进而明显提高催化剂的活性和总醇的选择性.研究表明,将具有高活...

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Published in物理化学学报 Vol. 30; no. 11; pp. 2127 - 2133
Main Author 韩涛 黄伟 王晓东 唐钰 刘双强 游向轩
Format Journal Article
LanguageChinese
Published 太原理工大学煤科学与技术教育部和山西省重点实验室,太原,030024%太原理工大学煤科学与技术教育部和山西省重点实验室,太原030024 2014
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
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ISSN1000-6818
DOI10.3866/PKU.WHXB201409121

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Summary:采用共浸渍法制备了不同Ce含量的Ce-Cu-Co/CNTs催化剂,考察了其在合成气制低碳醇反应中的催化性能,借助X射线衍射(XRD)、程序升温还原(H2-TPR)、N2吸脱附实验(BET)、透射电镜(TEM)和CO程序升温脱附(CO-TPD)对这些催化剂进行了表征.结果表明,当Ce的质量分数为3%时,低碳醇的时空收率和选择性达到最高,分别为696.4 mg?g-1?h-1和59.7%,其中乙醇占总醇的46.8%,适量Ce的添加能提高Cu物种在催化剂上的分散度和催化剂的还原性能,能显著地增加催化剂吸附CO的能力,促进合成醇活性位的形成,进而明显提高催化剂的活性和总醇的选择性.研究表明,将具有高活性和高碳链增长能力的CuCo基催化剂与碳纳米管的限域效应结合,可实现缩窄产物分布、大幅度提高乙醇选择性的目的.
Bibliography:11-1892/06
HAN Tao, HUANG Wei, WANG Xiao-Dong, TANG Yu, LIU Shuang-Qiang, YOU Xiang-Xuan (1.Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, P R. China; 2.State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, P R. China)
A series of Ce-Cu-Co/carbon nanotubes (CNTs) catalysts with different Ce contents were prepared by co-impregnation, and the catalytic performance was investigated for the synthesis of higher alcohols from syngas. The catalysts were characterized by X-ray diffraction (XRD), temperature-programmed reduction of H2 (H2-TPR), N2 adsorption-desorption isotherms (BET), transmission electron microscopy (TEM), and temperature-programmed desorption of CO (CO-TPD). The results showed that at a Ce content of 3% the catalyst had the highest catalytic activity. The formation rate and selectivity of alcohol reached 696.4 mg .g-'. h-1 and 59.7%, where the mas
ISSN:1000-6818
DOI:10.3866/PKU.WHXB201409121