Skip to main content
Log in

Reversibility of Mn Valence State in MnOx/TiO2 Catalysts for Low-temperature Selective Catalytic Reduction for NO with NH3

  • Published:
Catalysis Letters Aims and scope Submit manuscript

Abstract

Selective catalytic reduction (SCR) of NO with NH3 was investigated using TiO2-supported Mn oxide catalysts prepared by wet impregnation at different MnO x loadings and reduction temperatures. The structures, valence states, and physicochemical properties were characterized using Brunauer–Emmett–Teller, X-ray diffraction, Raman, and X-ray photoelectron methods. The 20 wt% MnO x /TiO2 catalyst, which was rich in Mn4+ species, showed the best SCR activity and N2 selectivity at low temperatures. As the reduction temperature increased, the Mn valence states gradually changed from Mn4+ to Mn2+. When the valence state was lowered (Mn4+ to Mn2+), the SCR activity decreased significantly at low temperatures. H2 shut-off tests confirmed that the activity of the reduced catalyst was not fully recovered. For superior SCR activity at low temperatures, the MnO x species on the MnO x /TiO2 catalyst surface should be kept as Mn4+.

Graphical Abstract

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9
Fig. 10
Fig. 11

Similar content being viewed by others

References

  1. Fritz A, Pitchon V (1997) Appl Catal B 13:1

    Article  CAS  Google Scholar 

  2. Bosch H, Janssen F (1988) Catal Today 2:369

    Article  CAS  Google Scholar 

  3. Forzatti P, Lietti L (1996) Heterogen Chem Rev 3:33

    Article  CAS  Google Scholar 

  4. Alemany LJ, Berti F, Busca G, Ramisa G, Robbac D, Toledob GP, Trombetta M (1996) Appl Catal B 10:299

    Article  CAS  Google Scholar 

  5. Cho SM (1994) Chem Eng Prog 90:39

    CAS  Google Scholar 

  6. Wood SC (1994) Chem Eng Prog 90:32

    CAS  Google Scholar 

  7. Li J, Chang H, Ma L, Hao J, Yang RT (2011) Catal Today 175:147

    Article  CAS  Google Scholar 

  8. Kapteijn F, Singoredjo L, Andreini A, Moulijn J (1994) Appl Catal B 3:173

    Article  CAS  Google Scholar 

  9. Tang X, Hao J, Xu W, Li J (2007) Catal Commun 8:329

    Article  CAS  Google Scholar 

  10. Park TS, Jeong SK, Hong SH, Hong SC (2001) Ind Eng Chem Res 40:4491

    Article  CAS  Google Scholar 

  11. Kang M, Park ED, Kim JM, Yie JE (2006) Catal Today 111:236

    Article  CAS  Google Scholar 

  12. Qi G, Yang RT, Chang R (2004) Appl Catal B 51:93

    Article  CAS  Google Scholar 

  13. Qi G, Yang RT (2003) J Catal 217:434

    CAS  Google Scholar 

  14. Kang M, Park ED, Kim JM, Yie JE (2007) Appl Catal A 327:261

    Article  CAS  Google Scholar 

  15. Kijlstra WS, Daamen JCML, Van De Graaf JM, Van Der Linden B, Poels EK, Bliek A (1996) Appl Catal B 7:337

    Article  CAS  Google Scholar 

  16. Sjoerd Kijlstra W, Biervliet M, Poels EK, Bliek A (1998) Appl Catal B 16:327

    Article  CAS  Google Scholar 

  17. Singoredjo L, Korver R, Kapteijn F, Moulijn J (1992) Appl Catal B 1:297

    Article  CAS  Google Scholar 

  18. Qi G, Yang RT (2005) Appl Catal B 60:13

    Article  CAS  Google Scholar 

  19. Ma AZ, Grunert W (1999) Chem Commun 1:71

    Article  Google Scholar 

  20. Wu Z, Jin R, Liu Y, Wang H (2008) Catal Commun 9:2217

    Article  CAS  Google Scholar 

  21. Wu Z, Jiang B, Liu Y, Zhao W, Guan B (2007) J Hazard Mater 145:488

    Article  CAS  Google Scholar 

  22. Jiang B, Liu Y, Wu Z (2009) J Hazard Mater 162:1249

    Article  CAS  Google Scholar 

  23. Bi-Jun W, Xiao-Qin L, Shu-Gang W, Lin Z, Lin-Yan C (2008) J Combust Sci Technol 14:221

    Google Scholar 

  24. Marban G, Valdes-Solis T, Fuertes AB (2004) J Catal 226:138

    Article  CAS  Google Scholar 

  25. Valdes-Solis T, Marban G, Fuertes AB (2003) Appl Catal B 46:261

    Article  CAS  Google Scholar 

  26. Thirupathi B, Smirniotis PG (2012) Catal Lett 141:1404

    Google Scholar 

  27. Ettireddy PR, Ettireddy N, Mamedov S, Boolchand P, Smirniotis PG (2007) Appl Catal B 76:123

    Article  CAS  Google Scholar 

  28. Pena DA, Uphade BS, Smirniotis PG (2004) J Catal 221:421

    Article  CAS  Google Scholar 

  29. Thirupathi B, Smirniotis PG (2011) Appl Catal B 110:195

    Article  CAS  Google Scholar 

  30. Thirupathi B, Smirniotis PG (2012) J Catal 288:74

    Article  CAS  Google Scholar 

  31. Giakoumelou I, Fountzoula C, Kordulis C, Boghosian A (2006) J Catal 239:1

    Article  CAS  Google Scholar 

  32. Djaoued Y, Badilescu S, Ashrit PV, Bersani D, Lottici PP, Robichaud J (2001) J Sol-Gel Sci Technol 24:255

    Article  Google Scholar 

  33. Orendorz A, Brodyanski A, Losch J, Bai L, Chen Z, Le Y, Ziegler C, Gnaser H (2007) Surf Sci 601:4390

    Article  CAS  Google Scholar 

  34. Bernard MC, Hugot Le Goff A, Thi BV, De Torresi SC (1993) J Electrochem Soc 140:3065

    Article  CAS  Google Scholar 

  35. Koebel M, Elsener M, Madia G (2001) Ind Eng Chem Res 40:52

    Article  CAS  Google Scholar 

  36. Qi G, Yang RT (2003) Appl Catal B 44:217

    Article  CAS  Google Scholar 

  37. Curry-Hyde HE, Musch H, Baiker A (1990) Applied catalysis 65:211

    Article  CAS  Google Scholar 

  38. Inomata M, Miyamoto A, Murakami Y (1980) J Catal 62:140

    Article  CAS  Google Scholar 

  39. Oyama ST, Went GT, Lewis KB, Bell AT, Somorjai GA (1989) J Phys Chem 93:6786

    Article  CAS  Google Scholar 

  40. Chen Z, Yang Q, Li H, Li X, Wang L, Chi Tsang S (2010) J Catal 276:56

    Article  CAS  Google Scholar 

  41. Qi G, Yang RT (2004) J Phys Chem B 108:15738

    Article  CAS  Google Scholar 

Download references

Acknowledgments

This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (No. 2010-0023963).

Author information

Authors and Affiliations

Authors

Corresponding authors

Correspondence to Sung Su Kim or Sung Chang Hong.

Rights and permissions

Reprints and permissions

About this article

Cite this article

Park, K.H., Lee, S.M., Kim, S.S. et al. Reversibility of Mn Valence State in MnOx/TiO2 Catalysts for Low-temperature Selective Catalytic Reduction for NO with NH3 . Catal Lett 143, 246–253 (2013). https://doi.org/10.1007/s10562-012-0952-8

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10562-012-0952-8

Keywords

Navigation