Ce-Cu-Co/CNTs催化剂催化合成气制低碳醇及乙醇的研究

引用本文: 韩涛, 黄伟, 王晓东, 唐钰, 刘双强, 游向轩. Ce-Cu-Co/CNTs催化剂催化合成气制低碳醇及乙醇的研究[J]. 物理化学学报, 2014, 30(11): 2127-2133. doi: 10.3866/PKU.WHXB201409121 shu

Citation: HAN Tao, HUANG Wei, WANG Xiao-Dong, TANG Yu, LIU Shuang-Qiang, YOU Xiang-Xuan. Study of Ce-Cu-Co/CNTs Catalysts for the Synthesis of Higher Alcohols and Ethanol from Syngas[J]. Acta Physico-Chimica Sinica, 2014, 30(11): 2127-2133. doi: 10.3866/PKU.WHXB201409121 shu

Ce-Cu-Co/CNTs催化剂催化合成气制低碳醇及乙醇的研究

韩涛 ^1, ,
黄伟 ^1, ,
王晓东 ^1,2, ,
唐钰 ^1, ,
刘双强 ^1, ,
游向轩 ^1,

基金项目:
国家自然科学基金重点项目(21336006) (21336006)

国家自然科学基金面上项目(21176176) (21176176)

高等学校博士学科点专项(优先发展领域) (20111402130002) (优先发展领域) (20111402130002)

煤转化国家重点实验室开放课题基金项目(J14-15-603)资助 (J14-15-603)

摘要:

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.

关键词:

Ce
/ CuCo/CNTs 催化剂
/ 合成气
/ 低碳醇
/ 乙醇

English

Study of Ce-Cu-Co/CNTs Catalysts for the Synthesis of Higher Alcohols and Ethanol from Syngas

1.
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
Received Date: 05 June 2014
Available Online: 30 October 2014
Fund Project:
国家自然科学基金重点项目(21336006)

国家自然科学基金面上项目(21176176)

高等学校博士学科点专项(优先发展领域) (20111402130002)

煤转化国家重点实验室开放课题基金项目(J14-15-603)资助

Abstract:

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^-1· h^-1 and 59.7%, where the mass fraction of ethanol was 46.8% of the total amount of alcohols. The addition of an appropriate amount of Ce facilitated the dispersion of Cu and promoted reduction of the catalysts. It also markedly increased the adsorption capacity for CO, and significantly improved the formation of active sites for alcohols, which is favorable for the catalytic activity and to improve the selectivity of alcohols. Research showed that combining the CuCo-based catalyst, which has high activity and a high ability of carbon chain growth, with the confinement effect of CNTs can result in a narrow distribution of alcohols and significantly improve the selectivity of ethanol.

Key words:

Ce
/ CuCo/CNTs catalyst
/ Syngas
/ Higher alcohol
/ Ethanol

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沈阳化工大学材料科学与工程学院沈阳 110142

Ce-Cu-Co/CNTs催化剂催化合成气制低碳醇及乙醇的研究

English

Study of Ce-Cu-Co/CNTs Catalysts for the Synthesis of Higher Alcohols and Ethanol from Syngas

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Ce-Cu-Co/CNTs催化剂催化合成气制低碳醇及乙醇的研究

English

Study of Ce-Cu-Co/CNTs Catalysts for the Synthesis of Higher Alcohols and Ethanol from Syngas

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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