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

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: 5 June 2014
Available Online: 12 September 2014
Fund Project: 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)

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.
- Ce,
- CuCo/CNTs catalyst,
- Syngas,
- Higher alcohol,
- Ethanol
1. [1]
  
  (1) Li, D. B.; Ma, Y. G.; Qi, H. J.; Li,W. H.; Sun, Y. H.; Zhong, B. Prog. Chem. 2004, 16, 584. [李德宝, 马玉刚, 齐会杰, 李文怀, 孙予罕, 钟炳. 化学进展, 2004, 16, 584.]
2. [2]
  (2) Ran, H. F.; Fang, K. G.; Lin, M. G.; Sun, Y. H. Nat. Gas Chem. Ind. 2010, 35, 1. [冉宏峰, 房克功, 林明桂, 孙予罕. 天然气化工, 2010, 35, 1.]
3. [3]
  (3) Xiao, K.; Bao, Z. H.; Qi, X. Z.;Wang, X. X.; Zhong, L. S.; Fang, K. G.; Lin, M. G.; Sun, Y. H. Chin. J. Catal. 2013, 34, 116.
4. [4]
  (4) Zheng,W.;Yao, X. G.; Hu, D. Z.;Wen, L. Q.;Wang, X. Q. Sci. Technol. Inf. 2009, 10. [郑伟, 姚喜贵, 胡大志, 文良起, 王小倩. 科技资讯, 2009, 10.]
5. [5]
  (5) Shi, L. M.; Chu,W. J. Mol. Catal. (China) 2011, 25, 316. [士丽敏, 储伟. 分子催化, 2011, 25, 316.]
6. [6]
  (6) Lin, M. G.; Fang, K. G.; Li, D. B.; Sun, Y. H.; Chin. J. Catal. 2008, 29, 559. [林明桂, 房克功, 李德宝, 孙予罕. 催化学报, 2008, 29, 559.]
7. [7]
  (7) Wang, N.; Fang, K. G.; Lin, M. G.; Jiang, D.; Li, D. B.; Sun, Y. H. Nat. Gas Chem. Ind. 2010, 35, 6. [王宁, 房克功, 林明桂, 姜东, 李德宝, 孙予罕. 天然气化工, 2010, 35, 6.]
8. [8]
  (8) Chen, X. P.; Zhao, N.; Sun, Y. H.; Ren, J.;Wang, X. Z.; Zhong, B. Coal Convers. 1998, 21, 22. [陈小平, 赵宁, 孙予罕,任杰, 王秀芝, 钟炳. 煤炭转化, 1998, 21, 22.]
9. [9]
  (9) Shi, L. M.; Chu,W.; Deng, S. Y. J. Fuel Chem. Technol. 2012, 40, 436. [士丽敏, 储伟, 邓思玉. 燃料化学学报, 2012, 40, 436.]
10. [10]
  (10) Pan, H.; Bai, F. H.; Su, H. Q. Chem. Ind. Eng. Prog. 2010, 29, 157. [潘慧, 白凤华, 苏海全. 化工进展, 2010, 29, 157.]
11. [11]
  (11) Mao, D. S.; Guo, S. Q.; Yu, J.; Han, L. P.; Lu, G. Z. Acta. Phys. -Chim. Sin. 2011, 27, 2639. [毛东森, 郭胜强, 俞俊,韩璐蓬, 卢冠忠. 物理化学学报, 2011, 27, 2639.] doi: 10.3866/PKU.WHXB20111125
12. [12]
  (12) Huang, L. H.; Chu,W.; Hong, J. P.; Luo, S. Z. Chin. J. Catal. 2006, 27, 596. [黄利宏, 储伟, 洪景萍, 罗仕忠. 催化学报, 2006, 27, 596.] doi: 10.1016/S1872-2067(06)60033-8
13. [13]
  (13) Dong, X.; Liang, X. L.; Li, H. Y.; Lin, G. D.; Zhang, P.; Zhang, H. B. Catal. Today 2009, 147, 158. doi: 10.1016/j.cattod.2008.11.025
14. [14]
  (14) Wang, M.W.; Li, F. Y.; Peng, N. C. New Carbon Mater. 2002, 17, 75. [王敏炜, 李凤仪, 彭年才. 新型碳材料, 2002, 17, 75.](15) Pan, X. L.; Fan, Z. L.; Chen,W.; Ding, Y. J.; Luo, H. Y.; Bao, X. H. Nat. Mater. 2007, 6, 507.
15. [15]
  (16) Shi, L. M.; Chu,W.; Xu, H. Y.; Deng, S. Y. Rare Metal Mater. Eng. 2009, 38, 1382. [士丽敏, 储伟, 徐慧远, 邓思玉. 稀有金属材料与工程. 2009, 38, 1382.]
16. [16]
  (17) Wang, J. J.; Chernavskii, P. A.;Wang, Y.; Khodakov, A. Y. Fuel 2013, 103, 1111. doi: 10.1016/j.fuel.2012.07.055
17. [17]
  (18) Shi, L. M.; Chu,W.; Deng, S. Y. J. Nat. Gas Chem. 2011, 20, 48. doi: 10.1016/S1003-9953(10)60145-4
18. [18]
  (19) Cai, Q. R.; Peng, S. Y. The Catalysis Action in C1 Chemistry. Chemical Industry Press: Beijing, 1995; p137. [蔡启瑞, 彭少逸. 碳-化学中的催化作用. 北京: 化学工业出版社, 1995: 137.]
19. [19]
  (20) Xiao, D. X.; Doesburg, E. S. J. Catal. Today 1987, 2, 123.
20. [20]
  (21) Nachal, D. S.; G. B.; Challa, S. S. R. K.; James, J. S. Catal. Today 2009, 147, 100. doi: 10.1016/j.cattod.2009.02.027
21. [21]
  (22) Jae, Y. K.; Jose, A. R.; Jonathan, C. H.; Anatoly, I. F.; Peter, L. L. J. Am. Chem. Soc. 2003, 125, 10684. doi: 10.1021/ja0301673
22. [22]
  (23) Christpher, S. P.; Hari, N.; Chelsey, D. B. J. Catal. 2009, 266, 308. doi: 10.1016/j.jcat.2009.06.021
23. [23]
  (24) Jing, G.; Jian, Z. G.; Dan, L.; Zhao, Y. H; Jin, H. F.; Xiao, M. Z. Int. J. Hydrog. Energy 2008, 33, 5493. doi: 10.1016/j.ijhydene.2008.07.040
24. [24]
  (25) Damyanva, S.; Bueno, J. M. C. Appl. Catal. A 2003, 253, 135. doi: 10.1016/S0926-860X(03)00500-3
25. [25]
  (26) Shu, J. J.; Shao, Q. S. Appl. Catal. B 2013, 140 -141, 1.
26. [26]
  (27) Fang, Y. Z.; Liu, Y.; Zhang, L. H. Appl. Catal. A 2011, 397, 183. doi: 10.1016/j.apcata.2011.02.032
27. [27]
  (28) Li, H. Y.; Ren, X. B.; Guo, X. Y. Chem. Phys. Lett. 2007, 437, 108. doi: 10.1016/j.cplett.2007.02.015
28. [28]
  (29) Shu, J. C.; Xiu, L. P.; Liang, Y.; Xin, H. B. Mater. Lett. 2011, 65, 1522. doi: 10.1016/j.matlet.2011.02.070
29. [29]
  (30) Santiso, E. E.; Kostov, M. K.; George, A. M.; Nardelli, M. B.; Gubbins, K. E. Appl. Surf. Sci. 2007, 253, 5570. doi: 10.1016/j.apsusc.2006.12.121
30. [30]
  (31) Guo, S. Q.; Mao, D. S.; Yu, J.; Han, P. L. J. Fuel Chem. Technol. 2012, 40, 1103. [郭强胜, 毛东森, 俞俊, 韩璐蓬. 燃料化学学报, 2012, 40, 1103.]
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