Citation: SUN Meng-Meng, CAO Yi, LAN Li, ZOU Sha, FANG Zhi-Tao, CHEN Yao-Qiang. Selective Catalytic Oxidation of Ammonia to Nitrogen over Iron and Copper Bimetallic Catalysts[J]. Acta Physico-Chimica Sinica, ;2014, 30(12): 2300-2306. doi: 10.3866/PKU.WHXB201409291 shu

Selective Catalytic Oxidation of Ammonia to Nitrogen over Iron and Copper Bimetallic Catalysts

1.
Key Laboratory of Green Chemistry & Technology of the Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, P. R. China

Received Date: 16 June 2014
Available Online: 29 September 2014
Fund Project: 国家自然科学基金(21173153) (21173153) 国家高技术研究发展计划项目(863) (2013AA065304) (863) (2013AA065304)四川省科技厅科技支撑项目(2011GZ0035, 2012FZ0008)资助 (2011GZ0035, 2012FZ0008)

Iron and copper bimetallic catalysts with fixed total contents of copper and iron were prepared by a co-impregnation method, and then used for selective catalytic oxidation of ammonia to nitrogen. The properties of the catalysts were characterized by N₂ adsorption-desorption, H₂ temperature-programmed reduction (H₂- TPR), NH₃ temperature-programmed desorption (NH₃-TPD), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The iron and copper bimetallic catalysts exhibited od activity and high selectivity of N₂ at the gas hourly space velocity (GHSV) of 100000 h^-1. The activity and N₂ selectivity in the low temperature range increased with increasing Cu loading, whereas in the high temperature range (above 400 ℃) the selectivity of N₂ was directly related to the content of iron. The highest NH₃ conversion was achieved at about 350℃ for Fe_0.25Cu_0.75/ZSM-5, and the N₂ selectivity was up to 97% at 300 ℃. On the other hand, the extremely high N₂ selectivity about 98% was obtained over Fe_0.75Cu_0.25/ZSM-5 at 500 ℃. In addition, N₂O as the by-product and greenhouse gas was obtained in very low amounts for all the catalysts. The characterization results showed that the activity was influenced by the acid content and the amounts of copper species. Moreover, the highly reducing capacity could improve the N₂ selectivity.
- Iron,
- Copper,
- Molecular sieve,
- Ammonia oxidation reaction,
- N₂ selectivity,
- Catalyst
1. [1]
  
  (1) Krupa, S. V. Environ. Pollut. 2003, 124, 179. doi: 10.1016/S0269-7491(02)00434-7
2. [2]
  (2) Hung, C. M. Powder Technol. 2009, 196, 56. doi: 10.1016/j.powtec.2009.07.001
3. [3]
  (3) Akah, A.; Cundy, C.; Garforth, A. Appl. Catal. B: Environ. 2005, 59, 221. doi: 10.1016/j.apcatb.2004.10.020
4. [4]
  (4) Sobczyk, D. P.; Hensen, E. J. M.; Jong, A. M. D.; Santen, R. A. V. Top. Catal. 2003, 23, 1. doi: 10.1023/A:1024834800948
5. [5]
  (5) Hung, C. M. Powder Technol. 2010, 200, 78. doi: 10.1016/j.powtec.2010.02.014
6. [6]
  (6) Broek, A. C. M. V. D.; Grondelle, J. V.; Santen, R. A. V. J. Catal.1999, 185, 297. doi: 10.1006/jcat.1999.2506
7. [7]
  (7) Gang, L.; Anderson, B. G.; Grondelle, J. V.; Santen, R. A. V. Appl. Catal. B: Environ. 2003, 40, 101. doi: 10.1016/S0926-3373(02)00129-7
8. [8]
  (8) Zhang, L.; Zhang, C. B.; He, H. J. Catal. 2009, 261, 101. doi: 10.1016/j.jcat.2008.11.004
9. [9]
  (9) Zhang, L.; He, H. J. Catal. 2009, 268, 18. doi: 10.1016/j.jcat.2009.08.011
10. [10]
  (10) Long, R. Q.; Yang, R. T. J. Catal. 2002, 207, 158. doi: 10.1006/jcat.2002.3545
11. [11]
  (11) Cui, X. Z.; Zhou, J.; Ye, Z. Q.; Chen, H. R.; Li, L.; Ruan, M. L.; Shi, J. L. J. Catal. 2010, 270, 310. doi: 10.1016/j.jcat.2010.01.005
12. [12]
  (12) Qi, G. S.; Yang, R. T. Appl. Catal. A: Gen. 2005, 287, 25. doi: 10.1016/j.apcata.2005.03.006
13. [13]
  (13) Qi, G. S.; Gatt, J. E.; Yang, R. T. J. Catal. 2004, 226, 120. doi: 10.1016/j.jcat.2004.05.023
14. [14]
  (14) Long, R. Q.; Yang, R. T. J. Catal. 2001, 201, 145. doi: 10.1006/jcat.2001.3234
15. [15]
  (15) Gang, L.; Grondelle, J. V.; Anderson, B. G.; Santen, R. A. V. J. Catal. 1999, 186, 100. doi: 10.1006/jcat.1999.2524
16. [16]
  (16) Metkar, P. S.; Harold, M. P.; Balakotaiah, V. Appl. Catal. B: Environ. 2012, 111, 67.
17. [17]
  (17) Song, S. Q.; Jiang, S. J. Appl. Catal. B: Environ. 2012, 117, 346.
18. [18]
  (18) Liang, C. X.; Li, X. Y.; Qu, Z. P.; Tade, M.; Liu, S. M. Appl. Surf. Sci. 2012, 258, 3738. doi: 10.1016/j.apsusc.2011.12.017
19. [19]
  (19) Shi, L.; Yu, T.;Wang, X. Q.;Wang, J.; Shen, M. Q. Acta Phys. -Chim. Sin. 2013, 29, 1550. [石琳, 于铁, 王欣全, 王军, 沈美庆. 物理化学学报, 2013, 29, 1550.] doi: 10.3866/PKU.WHXB201304283
20. [20]
  (20) Rauscher, M.; Kesore, K.; Mönnig, R.; Schwieger,W.; Tißler, A.; Turek, T. Appl. Catal. A: Gen. 1999, 184, 249. doi: 10.1016/S0926-860X(99)00088-5
21. [21]
  (21) Zhang, T.; Liu, J.;Wang, D. X.; Zhao, Z.;Wei, Y. C.; Cheng, K.; Jiang, G. Y.; Duan, A. J. Appl. Catal. B: Environ. 2014, 148, 520.
22. [22]
  (22) Wang, J.; Huang, Y.; Yu, T.; Zhu, S. C.; Shen, M. Q.; Li,W.; Wang, J. Q. Catal. Sci. Technol. 2014, 4, 3004. doi: 10.1039/c4cy00451e
23. [23]
  (23) Brüggemann, T. C.; Keil, F. J. J. Phys. Chem. C 2009, 113, 13860.
24. [24]
  (24) Wagner, C. D.; Riggs,W. M.; Davis, L. E.; Moulder, J. F. Handbook of X-ray Photoelectron Spectroscopy, 1st ed.; Muilenberg, G. E. Ed. Perkin-Elmer Corporation: Eden Prairie, Minnesota, USA, 1979.
25. [25]
  (25) Gurgul, J.; ??tka, K.; Hnat, I.; Rynkowski, J.; Dzwigaj, S. Microporous Mesoporous Mat. 2013, 168, 1. doi: 10.1016/j.micromeso.2012.09.015
26. [26]
  (26) Lisi, L.; Pirone, R.; Russo, G.; Stanzione, V. Chem. Eng. J. 2009, 154, 341. doi: 10.1016/j.cej.2009.04.025
27. [27]
  (27) Long, R. Q.; Yang, R. T. J. Catal. 2001, 198, 20. doi: 10.1006/jcat.2000.3118
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