Citation: GAO Peng, LI Feng, ZHAO Ning, WANG Hui, WEI Wei, SUN Yu-Han. Preparation of Cu/Zn/Al/(Zr)/(Y) Catalysts from Hydrotalcite-Like Precursors and Their Catalytic Performance for the Hydrogenation of CO₂ to Methanol[J]. Acta Physico-Chimica Sinica, ;2014, 30(6): 1155-1162. doi: 10.3866/PKU.WHXB201401252 shu

Preparation of Cu/Zn/Al/(Zr)/(Y) Catalysts from Hydrotalcite-Like Precursors and Their Catalytic Performance for the Hydrogenation of CO₂ to Methanol

GAO Peng ^1,2 ,
LI Feng ² ,
ZHAO Ning ^2, ,
WANG Hui ¹ ,
WEI Wei ^1, ,
SUN Yu-Han ^2,3

1.
1 Center for Greenhouse Gas and Environmental Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201203, P. R. China;
2 State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, P. R. China;
3 Chinese Academy of Sciences Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201203, P. R. China

Received Date: 10 February 2014
Available Online: 2 April 2014
Fund Project:

Cu/Zn/Al/(Zr)/(Y) hydrotalcite-like compounds with Cu:Zn:Al:Zr:Y atomic ratios of 2:1:1:0:0, 2:1: 0.8:0.2:0, 2:1:0.8:0:0.2, and 2:1:0.8:0.1:0.1 were prepared using the coprecipitation method. The mixed oxides were then obtained by the calcination of the precursors at 500 ℃ in air, and subsequently evaluated in terms of their catalytic performance for the synthesis of methanol from the hydrogenation of CO₂. The asprepared samples were characterized by X-ray diffraction (XRD), thermogravimetric (TG) analysis, N₂ adsorption, reactive N₂O adsorption, H₂ temperature-programmed reduction (H₂-TPR), and H₂/CO₂ temperature-programmed desorption (H₂/CO₂ TPD) techniques. The results of these analyses showed that the BET specific surface area increased significantly with the introduction of Zr and Y, which was related to the amount of H₂O and CO₂ evolved from the precursors during calcination. The Cu specific surface area and Cu dispersion properties increased in the order of Cu/Zn/Al2 revealed that the CO₂ conversion was dependent on the Cu specific surface area, and the CH₃OH selectivity increased linearly as the proportion of strongly basic sites increased. The introduction of Zr and Y therefore favored the production of methanol and the maximum CH₃OH yield was obtained over the Cu/Zn/Al/Zr/Y catalyst.
- Hydrotalcite-like precursor,
- Modifier,
- Cu/Zn/Al catalyst,
- CO₂ hydrogenation,
- Methanol
1. [1]
  
  (1) Choudhury, J. ChemCatChem 2012, 4 (5), 609. doi: 10.1002/cctc.201100495
2. [2]
  (2) Olah, G. A.; Geoppert, A.; Prakash, G. K. S. Beyond Oil and Gas: the Methanol Economy, 1st ed.;Wiley-VCH:Weinheim, 2006; pp 173-187, 239-245.
3. [3]
  (3) Pontzen, F.; Liebner,W.; Gronemann, V.; Rothaemel, M.; Ahlers, B. Catal. Today 2011, 171 (1), 242. doi: 10.1016/j.cattod.2011.04.049
4. [4]
  (4) Yang, R. Q.; Yu, X. C.; Zhang, Y.; Li,W. Z.; Tsubaki, N. Fuel 2008, 87 (4-5), 443. doi: 10.1016/j.fuel.2007.06.020
5. [5]
  (5) Jun, K.W.; Shen,W. J.; Rao, K. S. R.; Lee, K.W. Appl. Catal. A: Gen. 1998, 174, 231. doi: 10.1016/S0926-860X(98)00195-1
6. [6]
  (6) Hong, Z. S.; Cao, Y.; Deng, J. F.; Fan, K. N. Catal. Lett. 2002, 82 (1-2), 37.
7. [7]
  (7) Gao, P.; Li, F.; Zhang, L. N.; Zhao, N.; Xiao, F. K.;Wei,W.; Zhong, L. S.; Sun, Y. H. Journal of CO 2 Utilization 2013, 2, 16. doi: 10.1016/j.jcou.2013.06.003
8. [8]
  (8) Wang, J.; Chen, H. B.; Yun, H.; Lin, J. D.; Yi, J.; Zhang, H. B.; Liao, D.W. Acta Phys. -Chim. Sin. 2003, 19 (1), 65. [王进, 陈鸿博, 云虹, 林敬东, 易军, 张鸿斌, 廖代伟. 物理化学学报, 2003, 19 (1), 65.] doi: 10.3866/PKU.WHXB20030115
9. [9]
  (9) Gao, P.; Li, F.; Zhan, H. J.; Zhao, N.; Xiao, F. K.;Wei,W.; Zhong, L. S.;Wang, H.; Sun, Y. H. J. Catal. 2013, 298, 51. doi: 10.1016/j.jcat.2012.10.030
10. [10]
  (10) An, X.; Li, J. L.; Zuo, Y. Z.; Zhang, Q.;Wang, D. Z.;Wang, J. F. Catal. Lett. 2007, 118 (3-4), 264. doi: 10.1007/s10562-007-9182-x
11. [11]
  (11) Fernandez, J. M.; Barriga, C.; Ulibarri, M. A.; Labajos, F. M.; Rives, V. Chem. Mater. 1997, 9 (1), 312. doi: 10.1021/cm9603720
12. [12]
  (12) Zhang, L. H.; Li, F.; Evans, D. G.; Duan, X. Mater. Chem. Phys. 2004, 87 (2-3), 402. doi: 10.1016/j.matchemphys.2004.06.010
13. [13]
  (13) Alejandre, A.; Medina, F.; Salagre, P.; Correig, X.; Sueiras, J. E. Chem. Mater. 1999, 11 (4), 939. doi: 10.1021/cm980500f
14. [14]
  (14) Zhang, L. H.; Zheng, C.; Li, F.; Evans, D. G.; Duan, X. J. Mater. Sci. 2008, 43 (1), 237. doi: 10.1007/s10853-007-2167-8
15. [15]
  (15) Gao, P.; Li, F.; Zhao, N.; Xiao, F. K.;Wei,W.; Zhong, L. S.; Sun, Y. H. Appl. Catal. A: Gen. 2013, 468, 442. doi: 10.1016/j.apcata.2013.09.026
16. [16]
  (16) Shannon, R. D. Acta Crystallogr. A 1976, 32, 751. doi: 10.1107/S0567739476001551
17. [17]
  (17) Wu, G. D.;Wang, X. L.; Chen, B.; Li, J. P.; Zhao, N.;Wei,W.; Sun, Y. H. Appl. Catal. A: Gen. 2007, 329, 106. doi: 10.1016/j.apcata.2007.06.031
18. [18]
  (18) Velu, S.; Sabde, D. P.; Shah, N.; Sivasanker, S. Chem. Mater. 1998, 10 (11), 3451. doi: 10.1021/cm980185x
19. [19]
  (19) Zhang, L. H.; Li, F.; Evans, D. G.; Duan, X. Ind. Eng. Chem. Res. 2010, 49 (13), 5959. doi: 10.1021/ie9019193
20. [20]
  (20) Gao, P.; Li, F.; Xiao, F. K.; Zhao, N.; Sun, N. N.;Wei,W.; Zhong, L. S.; Sun, Y. H. Catal. Sci. Technol. 2012, 2 (7), 1447. doi: 10.1039/c2cy00481j
21. [21]
  (21) Cheng, J.; Yu, J. J.;Wang, X. P.; Li, L. D.; Li, J. J.; Hao, Z. P. Energy Fuels 2008, 22 (4), 2131. doi: 10.1021/ef8000168
22. [22]
  (22) Xu, Z. P.; Zeng, H. C. J. Phys. Chem. B 2000, 104 (44), 10206. doi: 10.1021/jp001963n
23. [23]
  (23) Trujillano, R.; Holgado, M. J.; Pigazo, F.; Rives, V. Physica B 2006, 373 (2), 267. doi: 10.1016/j.physb.2005.11.154
24. [24]
  (24) Behrens, M.; Kasatkin, I.; Kuhl, S.;Weinberg, G. Chem. Mater. 2010, 22 (2), 386. doi: 10.1021/cm9029165
25. [25]
  (25) Gao, P.; Li, F.; Xiao, F.; Zhao, N.;Wei,W.; Zhong, L. S.; Sun, Y. H. Catal. Today 2012, 194 (1), 9. doi: 10.1016/j.cattod.2012.06.012
26. [26]
  (26) Guo, X. M.; Mao, D. S.; Lu, G. Z.;Wang, S.;Wu, G. S. J. Catal. 2010, 271, 178. doi: 10.1016/j.jcat.2010.01.009
27. [27]
  (27) Guo, X. M.; Mao, D. S.; Lu, G. Z.;Wang, S. Acta Phys. -Chim. Sin. 2012, 28 (1), 170. [郭晓明, 毛东森, 卢冠忠, 王嵩. 物理化学学报, 2012, 28 (1), 170.] doi: 10.3866/PKU.WHXB201228170
28. [28]
  (28) Arena, F.; Italiano, G.; Barbera, K.; Bordiga, S.; Bonura, G.; Spadaro, L.; Frusteri, F. Appl. Catal. A: Gen. 2008, 350, 16. doi: 10.1016/j.apcata.2008.07.028
29. [29]
  (29) Guo, X.; Mao, D.; Lu, G.;Wang, S.;Wu, G. J. Mol. Catal. A: Chem. 2011, 345 (1-2), 60. doi: 10.1016/j.molcata.2011.05.019
30. [30]
  (30) Wilmer, H.; Genger, T.; Hinrichsen, O. J. Catal. 2003, 215, 188. doi: 10.1016/S0021-9517(03)00003-4
31. [31]
  (31) Waugh, K. C. Solid State Ionics 2004, 168 (3-4), 327. doi: 10.1016/j.ssi.2003.05.001
32. [32]
  (32) Wu, G. D.;Wang, X. L.;Wei,W.; Sun, Y. H. Appl. Catal. A: Gen. 2010, 377, 107. doi: 10.1016/j.apcata.2010.01.023
33. [33]
  (33) Liu, Y. X.; Sun, K. P.; Ma, H.W.; Xu, X. L.;Wang, X. L. Catal. Commun. 2010, 11 (10), 880. doi: 10.1016/j.catcom.2010.03.014
34. [34]
  (34) Liu, X. M.; Lu, G. Q.; Yan, Z. F.; Beltramini, J. Ind. Eng. Chem. Res. 2003, 42 (25), 6518. doi: 10.1021/ie020979s
35. [35]
  (35) Arena, F.; Barbera, K.; Italiano, G.; Bonura, G.; Spadaro, L.; Frusteri, F. J. Catal. 2007, 249, 185. doi: 10.1016/j.jcat.2007.04.003
36. [36]
  (36) Gao, L. Z.; Au, C. T. J. Catal. 2000, 189, 1. doi: 10.1006/jcat.1999.2682
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Preparation of Cu/Zn/Al/(Zr)/(Y) Catalysts from Hydrotalcite-Like Precursors and Their Catalytic Performance for the Hydrogenation of CO2 to Methanol

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通讯作者: 陈斌, bchen63@163.com

Preparation of Cu/Zn/Al/(Zr)/(Y) Catalysts from Hydrotalcite-Like Precursors and Their Catalytic Performance for the Hydrogenation of CO₂ to Methanol