Citation: LIU Xiao-Qing, LI Shi-Hui, SUN Meng-Ting, YU Cheng-Long, HUANG Bi-Chun. Preparation, Characterization and Low-Temperature NH₃-SCR Activity of MnO_x/SAPO-11 Catalysts[J]. Acta Physico-Chimica Sinica, ;2016, 32(5): 1236-1246. doi: 10.3866/PKU.WHXB201602251 shu

Preparation, Characterization and Low-Temperature NH₃-SCR Activity of MnO_x/SAPO-11 Catalysts

1.
1 College of Environment and Energy, South China University of Technology, Guangzhou 510006, P. R. China;
2.
2 Key Laboratory of the Ministry of Education for Pollution Control and Ecosystem Restoration in Industry Clusters, South China University of Technology, Guangzhou 510006, P. R. China

Corresponding author: HUANG Bi-Chun,
Received Date: 23 November 2015
Available Online: 22 February 2016
Fund Project: 国家自然科学基金(51478191) (51478191)广东省省级科技计划项目(2014A020216003)资助 (2014A020216003)

MnO_x/SAPO-11 catalysts were prepared by impregnation, citric acid, and precipitation methods for low-temperature selective catalytic reduction (SCR) of NO with NH₃. The results indicated that the MnO_x/SAPO-11 catalyst with 20%(w) Mn loading prepared by the precipitation method showed the best SCR activity and N² selectivity. X-ray powder diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive spectrometry (EDS), atomic absorption spectrometry (AAS), N² adsorption-desorption, X-ray photoelectron spectroscopy (XPS), H₂ temperature-programmed reduction (H₂-TPR), NH₃ temperature-programmed desorption (NH₃-TPD), NO/O₂ temperature-programmed desorption, and mass spectrometry (NO/O₂-TPD-MS) were used to analyze the structural properties and catalytic performance of the catalysts. The results indicated that different manganese oxides were formed on the surface of SAPO-11 by the three different preparation methods. MnO_x loaded via the precipitation method existed as MnO₂ phase and amorphous MnO_x. The advantages of the catalyst prepared via this method were a large mesoporous and external surface area, the highest content of chemisorbed oxygen and Mn⁴⁺ as well as more favorable medium and strong acid sites. Thus, more NO₂ was produced on the catalyst during low-temperature SCR, which was a primary goal. MnO_x prepared by all three methods could be well-dispersed on the surface of SAPO-11. The dispersive action of SAPO-11 could affect the formation of MnO_x, which could affect the acidity of the catalysts. Thus, the temperature window was widened and N² selectivity was improved compared with pure MnO_x, with SAPO-11 acting as an excellent carrier.
- Selective catalytic reduction,
- Nitrogen oxide,
- SAPO-11 molecular sieve,
- Precipitation method,
- Manganese oxide
1. [1]
  (1) Yang, C.; Liu, X. Q.; Huang, B. C.; Wu, Y. M. Acta Phys.-Chim. Sin. 2014, 30, 1895. [杨超, 刘小青, 黄碧纯, 吴友明. 物理化学学报, 2014, 30, 1895.] doi: 10.3866/PKU.WHXB201407162
2. [2]
  (2) Yao, X. J.; Gong, Y. T.; Li, H. L.; Yang, F. M. Acta Phys. -Chim. Sin. 2015, 31, 817. [姚小江, 贡营涛, 李红丽, 杨复沫, 物理化学学报, 2015, 31, 817.] doi: 10.3866/PKU.WHXB201503253
3. [3]
  (3) Chen, J. H.; Cao, F. F.; Qu, R. Y.; Gao, X.; Cen, K. F. J. Colloid Interface Sci. 2015, 456, 66. doi: 10.1016/j.jcis.2015.06.001
4. [4]
  (4) Lian, Z. H.; Liu, F. D.; He, H.; Shi, X. Y.; Mo, J. S.; Wu, Z. B. Chem. Eng. J. 2014, 250, 390. doi: 10.1016/j.cej.2014.03.065
5. [5]
  (5) Wan, Y. P.; Zhao, W. R.; Tang, Y.; Li, L.; Wang, H. J.; Cui, Y. L.; Gu, J. L.; Li, Y. S.; Shi, J. L. Appl. Catal. B-Environ. 2014, 148, 114. doi: 10.1016/j.apcatb.2013:10.049
6. [6]
  (6) Andreoli, S.; Deorsola, F. A.; Galletti, C.; Pirone, R. Chem. Eng. J. 2015, 278, 174. doi: 10.1016/j.cej.2014.11.023
7. [7]
  (7) Dai, Y.; Li, J. H.; Peng, Y.; Tang, X. F. Acta Phys. -Chim. Sin. 2012, 28, 1771. [戴韵, 李俊华, 彭悦, 唐幸福, 物理化学学报, 2012, 28, 1771.] doi: 10.3866/PKU.WHXB201205113
8. [8]
  (8) Huang, P.; Pan, S.W.; Huang, B. C.; Cheng, H.; Ye, D. Q.; Wu, J. L.; Fu, M. L.; Lu, S. L. Acta Phys. -Chim. Sin. 2013, 29, 176. [黄萍, 盘思伟, 黄碧纯, 程华, 叶代启, 吴军良, 付名利, 卢圣良. 物理化学学报, 2013, 29, 176.] doi: 10.3866/PKU.WHXB201210094
9. [9]
  (9) Jiao, J. Z.; Li, S. H.; Huang, B. C. Acta Phys. -Chim. Sin. 2015, 31, 1383. [焦金珍, 李时卉, 黄碧纯. 物理化学学报, 2015, 31, 1383.] doi: 10.3866/PKU.WHXB201504292
10. [10]
  (10) Venkatathri, N.; Srivastava, R. Stud. Surf. Sci. Catal. 2004, 154, 978. doi: 10.1016/S0167-2991(04)80913-3
11. [11]
  (11) Meriaudeau, P.; Tuan, V. A.; Nghiem, V. T.; Lai, S. Y.; Hung, L. N.; Naccache, C. J. Catal. 1997, 169, 55. doi: 10.1006/jcat.1997.1647
12. [12]
  (12) Yang, X. M.; Xu, Z. S.; Tian, Z. J.; Ma, H. J.; Xu, Y. P.; Qu, W.; Lin, L.W. Catal. Lett. 2006, 109, 139. doi: 10.1007/s10562-006-0070-6
13. [13]
  (13) Wang, Z. M.; Tian, Z. J.; Teng, F.; Wen, G. D.; Xu, Y. P.; Xu, Z. S.; Lin, L.W. Catal. Lett. 2005, 103, 109. doi: 10.1007/s10562-005-6510-x
14. [14]
  (14) Wang, Z. M.; Tian, Z. J.; Teng, F.; Xu, Y. P.; Hu, S.; Tan, M. W.; Xu, Z. S.; Lin, L.W. Chin. J. Catal. 2005, 26, 819. [汪哲明, 田志坚, 滕飞, 徐云鹏, 胡胜, 谭明伟, 徐竹生, 林励吾. 催化学报, 2005, 26, 819.]
15. [15]
  (15) Campelo, J. M.; Lafont, F.; Marinas, J. M. Appl. Catal. A-Gen. 1998, 170, 139. doi: 10.1016/S0926-860X(98)00036-2
16. [16]
  (16) Tian, S. S.; Chen, J. X. Fuel Process. Technol. 2014, 122, 120. doi: 10.1016/j.fuproc.2014.01.031
17. [17]
  (17) Mathisen, K.; Stockenhuber, M.; Nicholson, D. G. Phys. Chem. Chem. Phys. 2009, 11, 5476. doi: 10.1039/b902491c
18. [18]
  (18) Worch, D.; Suprun, W.; Glaeser, R. Catal. Today 2011, 176, 309. doi: 10.1016/j.cattod.2010.12.008
19. [19]
  (19) Jiang, B. Q.; Liu, Y.; Wu, Z. B. J. Hazard. Mater. 2009, 162, 1249. doi: 10.1016/j.jhazmat.2008.06.013
20. [20]
  (20) Ning, P.; Song, Z. X.; Li, H.; Zhang, Q. L.; Liu, X.; Zhang, J. H.; Tang, X. S.; Huang, Z. Z. Appl. Surf. Sci. 2015, 332, 130. doi: 10.1016/j.apsusc.2015.01.118
21. [21]
  (21) Guo, R. T.; Zhen, W. L.; Pan, W. G.; Hong, J. N.; Jin, Q.; Ding, C. G.; Guo, S. Y. Environ. Technol. 2014, 35, 1766. doi: 10.1080/09593330.2014.881424
22. [22]
  (22) Mao, D. S.; Tao, L. H.; Guo, Y. L.; Lu, G. Z. Industrial Catalysis 2008, 16, 21. [毛东森, 陶丽华, 郭杨龙, 卢冠忠. 工业催化, 2008, 16, 21.]
23. [23]
  (23) Wang, L. S. Low-temperature Selective Catalytic Reduction of M_xO_y/MWCNTs Catalysts and Reaction Mechanism Study. Master Dissertation, South China University of Technology, Guangzhou, 2012. [王丽珊. M_xO_y/MWCNTs 催化剂的低温SCR性能与反应机理研究. 广州华南理工大学, 2012.]
24. [24]
  (24) Myeong-Heon, U.; Kang, M. J. Ind. Eng. Chem. 2005, 11, 540.
25. [25]
  (25) Xu, X. T.; Zhai, J. P.; Li, I. L.; Ruan, S. C. Appl. Mech. Mate. 2013, 275-277, 1737. doi: 10.4028/www.scientific.net/AMM.275-277.1737
26. [26]
  (26) Zhang, Y.W.; Shen, M. Q.; Wu, X. D.; Weng, D.; Zhang, Z. H.; Tian, R.; Chi, K. B. Acta Phys. -Chim. Sin. 2006, 22, 1495. [张钺伟, 沈美庆, 吴晓东, 翁端, 张志华, 田然, 迟克彬. 物理化学学报, 2006, 22, 1495.] doi: 10.1016/S1872-1508(06)60077-6
27. [27]
  (27) Liu, Q. Y.; Zuo, H. L.; Wang, T. J.; Ma, L. L.; Zhang, Q. Appl. Catal. A-Gen. 2013, 468, 68. doi: 10.1016/j.apcata.2013.08.009
28. [28]
  (28) Wang, L.; Huang, B.; Su, Y.; Zhou, G.; Wang, K.; Luo, H.; Ye, D. Chem. Eng. J. 2012, 192, 232. doi: 10.1016/j.cej.2012.04.012
29. [29]
  (29) Yu, C. L.; Wang, L. S.; Huang, B. C. Aerosol Air Qual. Res. 2015, 15, 1017. doi: 10.4209/acqr.2014.08.0162
30. [30]
  (30) Wang, D.; Jangjou, Y.; Liu, Y.; Sharma, M. K.; Luo, J.; Li, J.; Kamasamudram, K.; Epling, W. S. Appl. Catal. B-Environ. 2015, 165, 438. doi: 10.1016/j.apcatb.2014.10.020
31. [31]
  (31) Greenhalgh, B.; Fee, M.; Dobri, A.; Moir, J.; Burich, R.; Charland, J. P.; Stanciulescu, M. J. Mol. Catal. A-Chem. 2010, 333, 121. doi: 10.1016/j.molcata.2010.10.008
32. [32]
  (32) Stobbe, E. R.; Boer, B. A.; Geus, J.W. Catal. Today 1999, 47, 161. doi: 10.1016/S0920-5861(98)00296-X
33. [33]
  (33) Trawczyński, J.; Bielak, B.; Miśta, W. Appl. Catal. B-Environ. 2005, 55, 277. doi: 10.1016/j.apcatb.2004.09.005
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Preparation, Characterization and Low-Temperature NH₃-SCR Activity of MnO_x/SAPO-11 Catalysts