Citation: HAO Teng, WANG Jun, YU Tie, WANG Jian-Qiang, SHEN Mei-Qing. Effect of NO₂ on the Selective Catalytic Reduction of NO with NH₃ over Cu/SAPO-34 Molecular Sieve Catalyst[J]. Acta Physico-Chimica Sinica, ;2014, 30(8): 1567-1574. doi: 10.3866/PKU.WHXB201405261 shu

Effect of NO₂ on the Selective Catalytic Reduction of NO with NH₃ over Cu/SAPO-34 Molecular Sieve Catalyst

HAO Teng ¹ ,
WANG Jun ¹ ,
YU Tie ¹ ,
WANG Jian-Qiang ^1, ,
SHEN Mei-Qing ^1,2,

1.
1. Key Laboratory for Green Chemical Technology, Ministry of Education of China, School of Chemical Engineering & Technology, Tianjin University, Tianjin 300072, P. R. China;
2. State Key Laboratory of Engines, Tianjin University, Tianjin 300072, P. R. China

Received Date: 17 March 2014
Available Online: 26 May 2014
Fund Project:

This study investigated the effects of NO₂ on the selective catalytic reduction (SCR) of NO by NH₃ over Cu/SAPO-34 catalyst at temperatures ranging from 100 to 500 ℃. The Cu/SAPO- 34 sample was hydrothermally treated at 750 ℃ for 4 h to obtain a de-greened sample and X-ray diffraction (XRD) and scanning electron microscopy (SEM) were used to characterize the structure of the catalyst. SCR activity test, kinetic analysis, and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ-DRIFTS) were all applied to evaluate the changes in catalytic activity in the presence of various NO/NO₂ ratios. The SCR results for different NO/NO₂ molar ratios demonstrated that NO₂ inhibited the NO_x removal efficiency over the Cu/SAPO- 34 catalyst at low temperatures (100-280 ℃), but enhanced the efficiency at high temperatures (above 280 ℃). The amount of N₂O was observed to increase with decreasing NO/NO₂ ratios, owing to the decomposition of NH₄NO₃. The kinetic results showed that the fast SCR reaction exhibited a higher apparent activation energy (E_a=64.02 kJ·mol^-1) than that of the standard SCR reaction (E_a=48.00 kJ·mol^-1) over Cu/SAPO-34 catalyst. The results of in situ-DRIFTS showed that NO₂ did not efficiently generate nitrate species on Cu2+ sites compared with NO, and that some nitrate species combined with NH₄₊ on Brønsted acid sites to generate NH₄NO₃. The inhibitory effect of NO₂ at low temperatures is evidently caused by deposited NH₄NO₃ covering the active sites of Cu/SAPO-34 catalyst, while these NH₄NO₃ species can be reduced by NO or thermally decomposed as the temperature increases.
- Ammonia selective catalytic reduction,
- NO_x (NO and NO₂),
- Cu/SAPO-34,
- Diffuse reflectance infrared Fourier transform spectrum,
- NH₄NO₃
1. [1]
  
  (1) Busca, G.; Lietti, L.; Ramis, G.; Berti, F. Appl. Catal. B: Environ. 1998, 18, 1. doi: 10.1016/S0926-3373(98)00040-X
2. [2]
  (2) Qi, G. S.; Yang, R. T.; Chang, R. Appl. Catal. B: Environ. 2004, 51, 93. doi: 10.1016/j.apcatb.2004.01.023
3. [3]
  (3) Liu, C. C.; Teng, H. Appl. Catal. B: Environ. 2005, 58, 69. doi: 10.1016/j.apcatb.2004.12.002
4. [4]
  (4) Yan, J. Y.; Sachtler,W. M. H.; Kung, H. H. Catal. Today 1997, 33, 279. doi: 10.1016/S0920-5861(96)00100-9
5. [5]
  (5) Sjövall, H.; Olsson, L.; Fridell, E.; Blint, R. J. Appl. Catal. B: Environ. 2006, 64, 180. doi: 10.1016/j.apcatb.2005.12.003
6. [6]
  (6) Kwak, J. H.; Tonkyn, R. G.; Kim, D. H.; Szanyi, J.; Peden, C. H. F. J. Catal. 2010, 275, 187. doi: 10.1016/j.jcat.2010.07.031
7. [7]
  (7) Fickel, D.W.; D′Addio, E.; Lauterbacha, J. A.; Lobo, R. F. Appl. Catal. B: Environ. 2011, 102, 441. doi: 10.1016/j.apcatb.2010.12.022
8. [8]
  (8) Bull, I.; Xue,W. M.; Burk, P.; Boorse, S. R.; Jaglowski,W. M.; Koermer, G. S.; Moini, A.; Patchett, J. A.; Dettling, J. C. Caudle, M. T. Copper CHA Zeolite Catalysts. US Patent 7601662, 2009.
9. [9]
  (9) Kwak, J. H.; Tran, D.; Burton, S. D.; Szanyi, J.; Lee, J. H.; Peden, C. H. F. J. Catal. 2012, 287, 203. doi: 10.1016/j.jcat.2011.12.025
10. [10]
  (10) Schmieg, S. J.; Oh, S. H.; Kim, C. H. Catal. Today 2012, 184, 252. doi: 10.1016/j.cattod.2011.10.034
11. [11]
  (11) Fickel, D.W.; Lobo, R. F. J. Phys. Chem. C 2010, 114, 1633.
12. [12]
  (12) Korhonen, S. T.; Fickel, D.W.; Lobo, R. F.;Weckhuysen, B. M.; Beale, A. M. Chem. Commun. 2010, 47, 800.
13. [13]
  (13) Xue, J. J.;Wang, X. Q.; Qi, G. S.;Wang, J.; Shen, M. Q.; Li,W. J. Catal. 2013, 297, 56. doi: 10.1016/j.jcat.2012.09.020
14. [14]
  (14) Fan, S. K.; Xue, J. J.; Yu, T.; Fan, D. Q. Catal. Sci. Technol. 2013, 3, 2357. doi: 10.1039/c3cy00267e
15. [15]
  (15) Brandenberger, S.; Kröcher, O.; Tissler, A.; Althoff, R. Catal. Rev. -Sci. Eng. 2008, 50, 492. doi: 10.1080/01614940802480122
16. [16]
  (16) Rahkamaa-Tolonen, K.; Maunula, T.; Lomma, M.; Huuhtanen, M.; Keiski, R. L. Catal. Today 2005, 100, 217. doi: 10.1016/j.cattod.2004.09.056
17. [17]
  (17) Devadas, M.; Kröcher, O.; Elsener, M.;Wokaun, A.; Söger, N.; Pfeifer, M.; Demel, Y.; Mussmann, L. Appl. Catal. B: Environ. 2006, 67, 187. doi: 10.1016/j.apcatb.2006.04.015
18. [18]
  (18) Grossale, A.; Nova, I.; Tronconi, E. Catal. Today 2008, 136, 18. doi: 10.1016/j.cattod.2007.10.117
19. [19]
  (19) Grossale, A.; Nova, I.; Tronconi, E.; Chatterjee, D.;Weibel, M. J. Catal. 2008, 256, 312. doi: 10.1016/j.jcat.2008.03.027
20. [20]
  (20) Grossale, A.; Nova, I.; Tronconi, E. J. Catal. 2009, 265, 141. doi: 10.1016/j.jcat.2009.04.014
21. [21]
  (21) Iwasaki, M.; Shinjoh, H. Appl. Catal. A: Gen. 2010, 390, 71. doi: 10.1016/j.apcata.2010.09.034
22. [22]
  (22) Shi, X. Y.; Liu, F. D.; Xie, L. J.; Shan,W. P.; He, H. Environ. Sci. Technol. 2013, 47, 3293
23. [23]
  (23) Sjovall, H.; Olsson, L.; Fridell, E.; Blint, R. J. Appl. Catal. B: Environ. 2006, 64, 180. doi: 10.1016/j.apcatb.2005.12.003
24. [24]
  (24) Colombo, M.; Nova, I.; Tronconi, E. Catal. Today 2010, 151, 223. doi: 10.1016/j.cattod.2010.01.010
25. [25]
  (25) Xie, L. J.; Liu, F. D.; Liu, K.; Shi, X. Y.; He, H. Catal. Sci. Technol. 2014, 4, 1104. doi: 10.1039/c3cy00924f
26. [26]
  (26) Buchholz, A.;Wang,W.; Xu, M.; Arnold, A.; Hunger, M. Microporous Mesoporous Mat. 2002, 56, 267. doi: 10.1016/S1387-1811(02)00491-2
27. [27]
  (27) Xu, L.; Du, A.;Wei, Y.;Wang, Y.; Yu, Z.; He, Y.; Zhang, X.; Liu, Z. Microporous Mesoporous Mat. 2008, 115, 332. doi: 10.1016/j.micromeso.2008.02.001
28. [28]
  (28) Tan, J.; Liu, Z.; Bao, X.; Liu, X.; Han, X. Microporous Mesoporous Mat. 2002, 53, 97. doi: 10.1016/S1387-1811(02)00329-3
29. [29]
  (29) Martins, G. V. A.; Berlier, G.; Bisio, C.; Coluccia, S.; Pastore, H. O.; Marchese, L. J. Phys. Chem. C 2008, 112, 7193. doi: 10.1021/jp710613q
30. [30]
  (30) Ma, L.; Cheng, Y.; Cavataio, G.; McCabe, R.W.; Fu, L.; Li, J. Chem. Eng. J. 2013, 225, 323 doi: 10.1016/j.cej.2013.03.078
31. [31]
  (31) Onida, B.; Gabelica, Z.; Lourencüo, J.; Garrone, E. J. Phys. Chem. 1996, 100, 11072. doi: 10.1021/jp9600874
32. [32]
  (32) Centi, G.; Perathoner, S. Catal. Today 1996, 29, 117. doi: 10.1016/0920-5861(95)00289-8
33. [33]
  (33) Hadjiivanov, K.; Klissurski, D.; Ramis, G.; Busca, G. Appl. Catal. B: Environ. 1996, 7, 251. doi: 10.1016/0926-3373(95)00034-8
34. [34]
  (34) Adelman, B. J.; Beutel, T.; Lei, G. D.; Sachtler,W. M. H. J. Catal. 1996, 158, 327. doi: 10.1006/jcat.1996.0031
35. [35]
  (35) Wang, D.; Zhang, L.; Kamasamudram, K.; Epling,W. S. ACS Catal. 2013, 3, 871. doi: 10.1021/cs300843k
36. [36]
  (36) Sjövall, H.; Fridell, E.; Blint, R. J.; Olsson, L. Top Catal. 2007, 42, 113.
37. [37]
  (37) Qi, G. S.; Yang, R. T. J. Phys. Chem. B 2004, 108, 15738. doi: 10.1021/jp048431h
38. [38]
  (38) Trovarelli, A. Catal. Rev. -Sci. Eng. 1996, 38, 439. doi: 10.1080/01614949608006464
39. [39]
  (39) Centi, G.; Perathoner, S. Catal. Today 1996, 29, 117. doi: 10.1016/0920-5861(95)00289-8
40. [40]
  (40) Konduru, M. V.; Chuang, S. S. C. J. Catal. 2000, 196, 271. doi: 10.1006/jcat.2000.3046
41. [41]
  (41) Fanning, P. E.; Vannice, M. A. J. Catal. 2002, 207, 166. doi: 10.1006/jcat.2002.3518
42. [42]
  (42) Lei, G. D.; Adelman, B. J.; Sárkány, J.; Sachtler,W. M. H. Appl. Catal. B: Environ. 1995, 5, 245. doi: 10.1016/0926-3373(94)00043-3
43. [43]
  (43) Hadjiivanov, K. I. Catal. Rev. -Sci. Eng. 2000, 42, 71. doi: 10.1081/CR-100100260
44. [44]
  (44) Ivanova, E.; Hadjiivanov, K.; Klissurski, D.; Bevilacqua, M.; Armaroli, T.; Busca, G. Microporous Mesoporous Mat. 2001, 46, 299. doi: 10.1016/S1387-1811(01)00311-0
45. [45]
  (45) 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
46. [46]
  (46) Liu, Y.; Gao, Z. Acta Petrol Sin. Pet. Process Section 1996, 12, 35. [刘毅, 高滋. 石油学报: 石油加工, 1996, 12, 35.]
47. [47]
  (47) Lok, B. M.; Messina, C. A.; Patton, R. L.; Gajek, R. T.; Cannon, T. R.; Flanigen, E. M. Crystalline Silicoaluminophosphates. US Patent 4440871, 1984.
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Effect of NO₂ on the Selective Catalytic Reduction of NO with NH₃ over Cu/SAPO-34 Molecular Sieve Catalyst