Citation: CHEN Feng, HUANG Bi-Chun, YANG Ying-Xin, LIU Xiao-Qing, YU Cheng-Long. Synthesis, Characterization and NH₃-SCR Activity of MnSAPO-34 Molecular Sieves[J]. Acta Physico-Chimica Sinica, ;2015, 31(12): 2375-2385. doi: 10.3866/PKU.WHXB201510201 shu

Synthesis, Characterization and NH₃-SCR Activity of MnSAPO-34 Molecular Sieves

1.
1 School 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: 28 April 2015
Available Online: 19 October 2015
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)

A series of MnSAPO-34 molecular sieves were synthesized by a hydrothermal method for selective catalytic reduction (SCR) of NO with NH₃ and characterized using X-ray photoelectron spectroscopy (XPS), temperature-programmed reduction (TPR), and temperature-programmed desorption (TPD). Three factors were studied, including Mn-loading, calcination temperature, and synthesis time. The MnSAPO-34, which was synthesized in 6 h and calcined at 550 ℃ with the Mn-loading (n_(MnO)/n_(P₂O₅)= 0.1), exhibits the highest activity among all the samples, with NO_x conversion of almost 100% and N₂ selectivity higher than 80%. The results show that the porous and crystalline structures of MnSAPO-34 are greatly affected by addition of manganese, and excessive Mn-loading could result in lower crystallinity and the generation of nonframework manganese oxides. Meanwhile, a decrease in specific surface area and pore volume are observed in MnSAPO-34 with higher Mn-loading; however, the opposite characteristics are observed with a decreasing calcination temperature and shorter synthesis time. Manganese species of high oxidation state, mostly Mn⁴⁺, are shown to be on the catalysts surface after high temperature calcination, and the increase ratio of Mn³⁺ could help to improve the catalytic activity. Under proper synthesis conditions, the incorporation of manganese could improve the adsorption of nitric oxide and ammonia, and the interaction between the strongly adsorbed NO and strongly adsorbed NH₃ might be the reason for the enhancement in their catalytic efficiency.
- Selective catalytic reduction,
- Nitrogen oxide,
- Manganese,
- SAPO-34 molecular sieve,
- X-ray photoelectron spectroscopy,
- Temperature-programmed reduction
1. [1]
  (1) Qi, G. S.; Yang, R. T. Appl. Catal. B-Environ. 2003, 44, 217. doi: 10.1016/S0926-3373(03)00100-0
2. [2]
  (2) Fang, C.; Zhang, D. S.; Cai, S. X.; Zhang, L.; Huang, L.; Li, H. R.; Maitarad, P.; Shi, L. Y.; Gao, R. H.; Zhang, J. P. Nanoscale 2013, 5, 9199. doi: 10.1039/c3nr02631k
3. [3]
  (3) Wang, L. S.; Huang, B. C.; Su, Y. X.; Zhou, G. Y.; Wang, K. L.; Luo, H. C.; Ye, D. Q. Chem. Eng. J. 2012, 192, 232. doi: 10.1016/j.cej.2012.04.012
4. [4]
  (4) Su, Y. X.; Fan, B. X.; Wang, L. S.; Liu, Y. F.; Huang, B. C.; Fu, M. L.; Chen, L. M.; Ye, D. Q. Catal. Today 2013, 201, 115. doi: 10.1016/j.cattod.2012.04.063
5. [5]
  (5) 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
6. [6]
  (6) 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
7. [7]
  (7) Yu, C. L.; Huang, B. C.; Yang, Y. X. Journal of South China University of Technology (Natural Science Edition) 2015, 3, 143. [喻成龙, 黄碧纯, 杨颖欣. 华南理工大学学报(自然科学版), 2015, 3, 143.]
8. [8]
  (8) 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
9. [9]
  (9) Wang, J.; Yu, T.; Wang, X. Q.; Qi, G. S.; Xue, J. J.; Shen, M. Q.; Li, W. Appl. Catal. B-Environ. 2012, 127, 137. doi: 10.1016/j.apcatb.2012.08.016
10. [10]
  (10) Ye, Q.; Wang, L. F.; Yang, R. T. Appl. Catal. A-Gen. 2012, 427-428, 24.
11. [11]
  (11) Martí nez-Franco, R.; Moliner, M.; Franch, C.; Kustov, A.; Corma, A. Appl. Catal. B-Environ. 2012, 127, 273. doi: 10.1016/j.apcatb.2012.08.034
12. [12]
  (12) Martí nez-Franco, R.; Moliner, M.; Concepcion, P.; Thogersen, J. R.; Corma, A. J. Catal. 2014, 314, 73. doi: 10.1016/j.jcat.2014.03.018
13. [13]
  (13) Deka, U.; Lezcano-Gonzalez, I.; Warrender, S. J.; Picone, A. L.; Wright, P. A.; Weckhuysen, B. M.; Beale, A. M. Microporous Mesoporous Mat. 2013, 166, 144. doi: 10.1016/j.micromeso.2012.04.056
14. [14]
  (14) Wei, Y. X.; He, Y. L.; Zhang, D. Z.; Xu, L.; Meng, S. H.; Liu, Z. M.; Su, B. L. Microporous Mesoporous Mat. 2006, 90, 188. doi: 10.1016/j.micromeso.2005.10.042
15. [15]
  (15) Tuš ar, N. N.; Mali, G.; Arć on, I.; Kauč ič , V.; Ghanbari-Siahkali, A.; Dwyer, J. Microporous Mesoporous Mat. 2002, 55, 203. doi: 10.1016/S1387-1811(02)00404-3
16. [16]
  (16) Rajić , N.; Stojaković , D.; Hoç evar, S.; Kauč ič , V. Zeolites 1993, 13, 384. doi: 10.1016/0144-2449(93)90154-U
17. [17]
  (17) Gu, J. F.; Agula, B.; Jia, M. L.; Liu, Y. P.; Zhaorigetu, B.; Yuan, Z. Y. Chin. J. Catal. 2010, 31, 322. [顾建峰, 阿古拉, 贾美林, 刘玉萍, 照日格图, 袁忠勇. 催化学报, 2010, 31, 322.]
18. [18]
  (18) Zhang, R. Z.; Zhao, L. F. Impurity Atoms of Phosphorus Aluminum Molecular Sieve and Its Application; Chemical Industry Press: Beijing, 2009; pp 56-57. [张瑞珍, 赵亮富. 杂原子磷铝分子筛及应用. 北京: 化学工业出版社, 2009: 56-57.]
19. [19]
  (19) Qi, G. S.; Yang, R. T. J. Phys. Chem. B 2004, 108, 15738. doi: 10.1021/jp048431h
20. [20]
  (20) Kapteijn, F.; Singoredjo, L.; Andreini, A.; Moulijn, J. A. Appl. Catal. B-Environ. 1994, 3, 173. doi: 10.1016/0926-3373(93)E0034-9
21. [21]
  (21) Tian, P.; Liu, Z. M.; Wu, Z. B.; Xu, L.; He, Y. L. Catal. Today 2004, 93-95, 735.
22. [22]
  (22) Thomas, J. M.; Greaves, G. N. Science 1994, 265, 1675.
23. [23]
  (23) Ramesh, K.; Chen, L. W.; Chen, F. X.; Liu, Y.; Wang, Z.; Han, Y. F. Catal. Today 2008, 131, 477. doi: 10.1016/j.cattod.2007.10.061
24. [24]
  (24) Wang, L. C.; Liu, Q.; Huang, X. S.; Liu, Y. M.; Cao, Y.; Fan, K. N. Appl. Catal. B-Environ. 2009, 88, 204. doi: 10.1016/j.apcatb.2008.09.031
25. [25]
  (25) Ristić , A.; Logar, N. Z.; Henninger, S. K.; Kauč ič , V. Adv. Funct. Mater. 2012, 22, 1952. doi: 10.1002/adfm.201102734
26. [26]
  (26) Ponce, S.; Peň a, M. A.; Fierro, J. L. G. Appl. Catal. B-Environ. 2000, 24, 193. doi: 10.1016/S0926-3373(99)00111-3
27. [27]
  (27) Kang, M.; Park, E. D.; Kim, J. M.; Yie, J. E. Appl. Catal. A-Gen. 2007, 327, 261. doi: 10.1016/j.apcata.2007.05.024
28. [28]
  (28) Akolekar, D. B.; Bhargava, S. K. Appl. Catal. A-Gen. 2001, 207, 355. doi: 10.1016/S0926-860X(00)00669-4
29. [29]
  (29) Lu, X.; Song, C.; Chang, C.; Teng, Y.; Tong, Z.; Tang, X. Ind. Eng. Chem. Res. 2014, 53, 11601. doi: 10.1021/ie5016969
30. [30]
  (30) Park, E.; Kim, M.; Jung, H.; Chin, S.; Jurng, J. ACS Catal. 2013, 3, 1518. doi: 10.1021/cs3007846
31. [31]
  (31) Vieira, A.; Tovar, M. A.; Pfaff, C.; Betancourt, P.; Méndez, B.; López, C. M.; Machado, F. J.; Goldwasser, J.; de Agudelo, M. M. R.; Houalla, M. J. Mol. Catal. A-Chem. 1999, 144, 101. doi: 10.1016/S1381-1169(98)00338-0
32. [32]
  (32) Wu, Z. B.; Jiang, B. Q.; Liu, Y.; Wang, H. Q.; Jin, R. B. Environ. Sci. Technol. 2007, 41, 5812. doi: 10.1021/es0700350
33. [33]
  (33) Liu, F. D.; He, H. Catal. Today 2010, 153, 70. doi: 10.1016/j.cattod.2010.02.043
34. [34]
  (34) Guan, B.; Lin, H.; Zhu, L.; Huang, Z. J. Phys. Chem. C 2011, 115, 12850. doi: 10.1021/jp112283g
35. [35]
  (35) Shu, Y.; Sun, H.; Quan, X.; Chen, S. J. Phys. Chem. C 2012, 116, 25319. doi: 10.1021/jp307038q
36. [36]
  (36) Yu, C. L.; Wang, L. S.; Huang, B. C. Aerosol Air Qual. Res. 2015, 15, 1017.
37. [37]
  (37) Vishwanathan, V.; Jun, K. W.; Kim, J. W.; Roh, H. S. Appl. Catal. A-Gen. 2004, 276, 251.
38. [38]
  (38) Jin, R. B.; Liu. Y.; Wu, Z. B.; Wang, H. Q.; Gu, T. T. Catal. Today 2010, 153, 84. doi: 10.1016/j.cattod.2010.01.039
39. [39]
  (39) Fang, C.; Zhang, D. S.; Shi, L. Y.; Gao, R. H.; Li, H. R.; Ye, L. P.; Zhang, J. P. Catal. Sci. Technol. 2013, 3, 803. doi: 10.1039/C2CY20670F
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Synthesis, Characterization and NH₃-SCR Activity of MnSAPO-34 Molecular Sieves