Cu-Fe基双孔载体催化剂结构和低碳醇合成反应性能

doi:10.3866/PKU.WHXB201205213

Acta Phys. -Chim. Sin. ›› 2012, Vol. 28 ›› Issue (08): 1964-1970.doi: 10.3866/PKU.WHXB201205213

• CATALYSIS AND SURFACE SCIENCE • Previous Articles Next Articles

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

LIU Jian-Guo^1,2, DING Ming-Yue¹, WANG Tie-Jun¹, MA Long-Long¹

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:2012-03-13 Revised:2012-05-18 Published:2012-07-10
Contact: WANG Tie-Jun E-mail:wangtj@ms.giec.ac.cn
Supported by:
The project was supported by the National Natural Science Foundation of China (51161140331, 51036006) and Special Funds for Major State Basic Research Projects (2011BAD22B06).

Abstract

Abstract:

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.

Key words: Higher alcohols synthesis, Cu-Fe based catalyst, Bimodal pore support, Space-time yield, Selectivity of C₂+OH

MSC2000:

O643

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 Phys. -Chim. Sin., 2012, 28(08): 1964-1970.

References

(1) Herman, R. G. Catal. Today 2000, 55, 233. doi: 10.1016/S0920-5861(99)00246-1
(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) Tronconi, E.; Lietti, L.; Forzatti, P.; Pasquon, I. Appl. Catal.1989, 47, 317. doi: 10.1016/S0166-9834(00)83237-6
(4) Mahdavi, V.; Peyrovi, M. H. Catal. Commun. 2006, 7, 542. doi: 10.1016/j.catcom.2006.01.012
(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) Courty, P.; Durand, D.; Freund, E.; Sugier, A. J. Mol. Catal.1982, 17, 241. doi: 10.1016/0304-5102(82)85035-9
(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) Boz, I.; Sahibzada, M.; Metcalfe, I. S. Ind. Eng. Chem. Res.1994, 33, 2021. doi: 10.1021/ie00033a001
(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) Bukur, D. B.; Lang, X. S. Ind. Eng. Chem. Res. 1999, 38, 3270.doi: 10.1021/ie990028n
(11) Sibillia, J. A.; Dominguez, J. M.; Herman, R. G.; Klier, K.Prepr. Div. Fuel Chem. ACS 1984, 29, 261.
(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) 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) Zhang, Y.; Yoneyama, Y.; Tsubaki, N. Chem. Commun. 2002,1216.
(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) Xu, B. L.; Fan, Y. N.; Zhang, Y.; Tsubaki, N. AIChE Journal2005, 51, 2068. doi: 10.1002/aic.10469
(17) Inui, T.; Funabiki, M.; Suehiro, M.; Sezume, T. J. Chem. Soc. FaradayTrans. 1979, 75, 787.
(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) 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) Burch, R.; Chappell, R. J. Appl. Catal. 1988, 45, 131. doi: 10.1016/S0166-9834(00)82398-2
(21) Burch, R.; Golunski, S. E.; Spencer, M. S. J. Chem. Soc. Faraday Trans. 1990, 86, 2683. doi: 10.1039/ft9908602683
(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

[1]	Pei-Yi LIAO,Chen ZHANG,Li-Jun ZHANG,Yan-Zhang YANG,Liang-Shu ZHONG,Xiao-Ya GUO,Hui WANG,Yu-Han SUN. Influences of Cu Content on the Cu/Co/Mn/Al Catalysts Derived from Hydrotalcite-Like Precursors for Higher Alcohols Synthesis via Syngas [J]. Acta Phys. -Chim. Sin., 2017, 33(8): 1672-1680.
[2]	GUO Hai-Jun, XIONG Lian, LUO Cai-Rong, DING Fei, CHEN Xin-De, CHEN Yong. Effect of Fe/Co Mass Ratio on Catalytic Performances of Cu-Fe-Co Based Catalysts for Mixed Alcohols Synthesis [J]. Acta Phys. -Chim. Sin., 2011, 27(11): 2632-2638.
[3]	LI De-Bao;QI Hui-Jie;LI Wen-Huai;SUN Yu-Han;ZHONG Bing. Surficial Structure and Charge Effects of Ni Promoted K₂CO₃/MoS₂ Catalysts for Higher Alcohols Synthesis [J]. Acta Phys. -Chim. Sin., 2006, 22(09): 1132-1136.

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

PDF (PC)

Like

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 3

Metrics

Comments

Recommended 0