Citation: LIU Jian-Guo, DING Ming-Yue, WANG Tie-Jun, MA Long-Long. Structure and Performance of Cu-Fe Bimodal Support for Higher Alcohol Syntheses[J]. Acta Physico-Chimica Sinica, ;2012, 28(08): 1964-1970. doi: 10.3866/PKU.WHXB201205213 shu

Structure and Performance of Cu-Fe Bimodal Support for Higher Alcohol Syntheses

1.
1. Key Laboratory of Renewable Energy and Natural Gas Hydrate, Chinese Academy of Science, Guangzhou 510640,P.R. China;
2. Graduate School of Chinese Academy of Science, Beijing 100049, P.R.China

Received Date: 13 March 2012
Available Online: 21 May 2012
Fund Project: 国家自然科学基金国际(地区)合作项目(51161140331, 51036006) (地区)合作项目(51161140331, 51036006)国家科技支撑项目(2011BAD22B06)资助 (2011BAD22B06)

Copper-iron modified bimodal support (M) with different mass fractions of Cu and Fe elements were prepared by an ultrasonic impregnation method. The catalytic performance for higher alcohol syntheses (HAS) was investigated in a fixed-bed flow reactor. Several techniques, including N₂ physical adsorption, temperature-programmed reduction/desorption of hydrogen, (H₂-TPR/TPD) and X-ray diffraction (XRD) were used to characterize the catalysts. The results indicated that the bimodal pore support was formed by the addition of small-pore silica sol into the macroporous silica gel. Increased amounts of small pore silica sol caused a decrease in pore size in the bimodal carrier. An increase in the Fe/Cu molar ratio facilitated the dispersion of CuO, promoted the reduction of CuO and Fe₂O₃ on the surface layers, and enhanced the interaction between the copper and iron species as well as the bimodal support inside the large pores. The copper was well-dispersed on the catalyst and the amount of iron carbides formed was high in catalysts with a high Fe/Cu molar ratio. Increasing the Fe/Cu mass ratio promoted the catalytic activity and thus facilitated the synthesis of higher alcohols. When the Fe/Cu molar ratio was increased to 30/20, the CO conversion and the yield of higher alcohols increased to 46% and 0.21 g·mL^-1·h^-1, respectively. At the same time, the mass ratio of C₂₊OH/CH₃OH reached 1.96.
- Higher alcohols synthesis,
- Cu-Fe based catalyst,
- Bimodal pore support,
- Space-time yield,
- Selectivity of C₂+OH
1. [1]
  
  (1) Herman, R. G. Catal. Today 2000, 55, 233. doi: 10.1016/S0920-5861(99)00246-1
2. [2]
  (2) He, D. P.; Ding, Y. J.; Luo, H.Y.; Li, C. J. Mol.Catal. A:Chem.2004, 208, 267. doi: 10.1016/S1381-1169(03)00542-9
3. [3]
  (3) Tronconi, E.; Lietti, L.; Forzatti, P.; Pasquon, I. Appl. Catal.1989, 47, 317. doi: 10.1016/S0166-9834(00)83237-6
4. [4]
  (4) Mahdavi, V.; Peyrovi, M. H. Catal. Commun. 2006, 7, 542. doi: 10.1016/j.catcom.2006.01.012
5. [5]
  (5) Xiao, H. C.; Li, D. B.; Li,W. H.; Sun, Y. H. Fuel Process. Technol. 2010, 91, 383. doi: 10.1016/j.fuproc.2009.07.004
6. [6]
  (6) Courty, P.; Durand, D.; Freund, E.; Sugier, A. J. Mol. Catal.1982, 17, 241. doi: 10.1016/0304-5102(82)85035-9
7. [7]
  (7) Subramanian, N. D.; Balaji, G.; Kumar, C. S. S. R.; Spivey,J. J. Catal. Today 2009, 147, 100. doi: 10.1016/j.cattod.2009.02.027
8. [8]
  (8) Boz, I.; Sahibzada, M.; Metcalfe, I. S. Ind. Eng. Chem. Res.1994, 33, 2021. doi: 10.1021/ie00033a001
9. [9]
  (9) Pour, A. N.; Zamani, Y.; Tavasoli, A.; Shahri, S. M. K.; Taheri,S. A. Fuel 2008, 87, 2004. doi: 10.1016/j.fuel.2007.10.014
10. [10]
  (10) Bukur, D. B.; Lang, X. S. Ind. Eng. Chem. Res. 1999, 38, 3270.doi: 10.1021/ie990028n
11. [11]
  (11) Sibillia, J. A.; Dominguez, J. M.; Herman, R. G.; Klier, K.Prepr. Div. Fuel Chem. ACS 1984, 29, 261.
12. [12]
  (12) Xu, R.; Yang, C.;Wei,W.; Li,W. H.; Sun, Y. H.; Hu, T. D.J. Mol.Catal. A: Chem. 2004, 221, 51. doi: 10.1016/j.molcata.2004.07.003
13. [13]
  (13) Xu, R.; Ma, Z. Y.; Yang, C.;Wei,W.; Sun, Y. H. React. Kinet. Catal. Lett. 2004, 81, 91. doi: 10.1023/B:REAC.0000016521.91502.5f
14. [14]
  (14) Zhang, Y.; Yoneyama, Y.; Tsubaki, N. Chem. Commun. 2002,1216.
15. [15]
  (15) Zhang, Y.; Koike, M.; Yang, R. Q.; Hinchiranan, S.; Vitidsant,T.; Tsubaki, N. Appl. Catal. A 2005, 292, 252. doi: 10.1016/j.apcata.2005.06.004
16. [16]
  (16) Xu, B. L.; Fan, Y. N.; Zhang, Y.; Tsubaki, N. AIChE Journal2005, 51, 2068. doi: 10.1002/aic.10469
17. [17]
  (17) Inui, T.; Funabiki, M.; Suehiro, M.; Sezume, T. J. Chem. Soc. FaradayTrans. 1979, 75, 787.
18. [18]
  (18) Yang, Y.; Tao, Z. C.; Zhang, C. H.;Wang, H.; Tian, L.; Xu, Y.Y.; Xiang, H.W.; Li, Y.W. J. Fuel Chem. Technol. 2004, 32,717. [杨勇, 陶智超, 张成华, 王洪, 田磊, 徐元源,相宏伟, 李永旺. 燃料化学学报, 2004, 32, 717.]
19. [19]
  (19) Zhang, Y.; Zhang, C. M.; Lu, F.; Li, Y.W.; Sun, Y. H.; Zhong, B.J. Fuel Chem. Technol. 2000, 28, 244. [张业, 张池明, 陆凡, 李永旺, 孙予罕, 钟炳. 燃料化学学报, 2000, 28, 244.]
20. [20]
  (20) Burch, R.; Chappell, R. J. Appl. Catal. 1988, 45, 131. doi: 10.1016/S0166-9834(00)82398-2
21. [21]
  (21) Burch, R.; lunski, S. E.; Spencer, M. S. J. Chem. Soc. Faraday Trans. 1990, 86, 2683. doi: 10.1039/ft9908602683
22. [22]
  (22) Ding, M.Y.; Yang, Y.; Xu, J.; Tao, Z. C.;Wang, H. L.;Wang, H.;Xiang, H.W.; Li, Y.W. Appl. Catal. A 2008, 345, 176. doi: 10.1016/j.apcata.2008.04.036
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