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Sol–gel derived mesoporous Cr/Al2O3 catalysts for SCR of NO by ammonia

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Catalytic performances of Cr/Al2O3 catalysts were investigated in Selective Catalytic Reduction (SCR) of NO by NH3 in the presence of oxygen. Solids were prepared either by sol–gel method or by impregnation and were characterized by different techniques such as chemical analysis, N2 physisorption, XRD, 27Al MAS NMR, DRIFT, UV–Vis Diffuse Reflectance (DRS), Raman Spectroscopy and Temperature Programmed Reduction by H2 (H2-TPR). The physisorption of N2 at 77 K reveals that solids are mesoporous. On the other hand, XRD shows that xerogels are amorphous but supercritical drying leads to a nanosized crystallite state. No crystalline α-Cr2O3 was found which indicate that metal species reside essentially on the surface of Al2O3 and their size measured less than 4 nm. Furthermore, 27Al MAS NMR reveals that part of chromium ions occupies sites on/in Al2O3 in close vicinity of tetrahedral 27Al. This, apparently, is not the case for aerogels. DRIFT results show that there is a consumption of hydroxyl groups of alumina after calcination. The esterification reaction between hydroxyl groups and chromium oxide during calcination leads to the formation of anchored (poly-)chromates according to DRS, Raman, and H2-TPR results. The catalysts are active in the studied reaction by NH3 and the activity is principally governed by preparation method and operating conditions. When compared to xerogels, aerogels are more active in NO reduction and less selective toward N2O. Preparation method and drying mode seem to involve the predominance of active species which are essentially mono and polychromates but Cr3+ ions incorporated inside alumina seem to be inactive.

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References

  1. G.J.K. Acres, B. Harrison, Top. Catal. 28, 141 (2004). doi:10.1023/B:TOCA.0000024329.85506.94

    Article  Google Scholar 

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

    Article  CAS  Google Scholar 

  3. H. Bosch, F. Janssen, Catal. Today 2, 369 (1988). doi:10.1016/0920-5861(88)80001-4

    Article  CAS  Google Scholar 

  4. J.H.A. Kiel, A.C.S. Edelaar, W. Prins, W.P.M. van Swaaij, Appl. Catal. B: Environ. 1, 41 (1992)

    Article  CAS  Google Scholar 

  5. H. Niyama, K. Murata, A. Ebitani, E. Echigoya, J. Catal. 48, 194 (1977). doi:10.1016/0021-9517(77)90090-2

    Article  Google Scholar 

  6. H. Niyama, K. Murata, E. Echigoya, J. Catal. 48, 201 (1977). doi:10.1016/0021-9517(77)90091-4

    Article  Google Scholar 

  7. H.E. Curry-Hyde, A. Baiker, Ind. Eng. Chem. Res. 29, 1985 (1990). doi:10.1021/ie00106a001

    Article  CAS  Google Scholar 

  8. H.E. Curry-Hyde, H. Musch, A. Baiker, Appl. Catal. 65, 211 (1990). doi:10.1016/S0166-9834(00)81598-5

    Article  CAS  Google Scholar 

  9. H.E. Curry-Hyde, H. Musch, M. Schrame-Marth, A. Wokaun, A. Baiker, J. Catal. 133, 397 (1992). doi:10.1016/0021-9517(92)90249-H

    Article  CAS  Google Scholar 

  10. H. Schneider, U. Scharf, A. Wokaun, A. Baiker, J. Catal. 147, 145 (1994)

    Google Scholar 

  11. B.L. Duffy, H.E. Curry-Hyde, N.W. Cant, P.F. Nelson, J. Catal. 149, 11 (1994). doi:10.1006/jcat.1994.1268

    Article  CAS  Google Scholar 

  12. C. Fountzoula, H.K. Matralis, C. Papadopoulou, G.A. Voyiatzis, C. Kordulis, J. Catal. 172, 391 (1997). doi:10.1006/jcat.1997.1845

    Article  CAS  Google Scholar 

  13. H. Zarrouk, A. Ghorbel, G.M. Pajonk, S.J. Teichner, in Proc 9th Ibero Americain Symposium on Catalysis, Lisbon, 16–21 July, 1984, p. 339

  14. A. Sayari, A. Ghorbel, G.M. Pajonk, S.J. Teichner, Bull. Soc. Chim. Fr. 5-6(part I), 220 (1981)

    Google Scholar 

  15. S. Zine, A. Sayari, A. Ghorbel, Can. J. Chem. Eng. 65, 127 (1987). doi:10.1002/cjce.5450650120

    Article  CAS  Google Scholar 

  16. S. Zine, A. Ghorbel, in The 2nd International Symposium of Heterogeneous Catalysis and Fine Chemicals, Poitiers, 2–5 October, 1990, p. 455

  17. Y. Kadri, A. Ghorbel, C. Naccache, J. Chim. Phys. 94, 1993 (1995)

    Google Scholar 

  18. Y. Kadri, A. Ghorbel, A. Rives, R. Hubaut, J. Chem. Soc. Faraday Trans. 94, 455 (1998). doi:10.1039/a705555b

    Article  Google Scholar 

  19. F. Ayari, M. Mhamdi, G. Delahay, A. Ghorbel, J. Sol–gel Sci. Technol. 49, 170 (2009). doi:10.1007/s10971-008-1860-7

    Article  CAS  Google Scholar 

  20. M.A. Siddiqi, R.A. Siddiqui, B. Atakan, Surf. Coat. Tech. 201, 9055 (2007). doi:10.1016/j.surfcoat.2007.04.036

    Article  CAS  Google Scholar 

  21. P.P. Semyannikov, I.K. Igumenov, S.V. Trubin, T.P. Chusova, Z.I. Semenova, Thermochim. Acta 432, 91 (2005). doi:10.1016/j.tca.2005.02.034

    Article  CAS  Google Scholar 

  22. S. Brunauer, L. Deming, W. Deming, E.J. Teller, J. Am. Chem. Soc. 62, 1723 (1940). doi:10.1021/ja01864a025

    Article  CAS  Google Scholar 

  23. J.H. DeBoer, B.C. Lippens, J. Catal. 3, 38 (1946). doi:10.1016/0021-9517(64)90090-9

    Article  Google Scholar 

  24. H. Xiong, Y. Zhang, S. Wang, J. Li, Catal. Commun. 6, 512 (2005). doi:10.1016/j.catcom.2005.04.018

    Article  CAS  Google Scholar 

  25. M. Afzal, F. Mahmood, Collect. Czech. Chem. Commun. 58, 474 (1993). doi:10.1135/cccc19930474

    Article  CAS  Google Scholar 

  26. A.K. Khattak, M. Afzal, M. Saleem, G. Yasmeen, R. Ahmad, Colloids Surf. A Physicochem. Eng. Asp. 162, 99 (2000). doi:10.1016/S0927-7757(99)00218-6

    Article  CAS  Google Scholar 

  27. G. Buelna, Y.S. Lin, Microporous Mesoporous Mater. 30, 359 (1999). doi:10.1016/S1387-1811(99)00065-7

    Article  CAS  Google Scholar 

  28. K. Wefers, C. Mirsa, Oxides and Hydroxides of Aluminum, Alcoa Technical Paper No. 19, Alcoa Laboratories (1987)

  29. J.W. Akitt, in Multinuclear NMR, ed. by J. Mason (Plenum, New York, 1987), Chapter 9

  30. A.T. Bell, A. Pines, NMR Techniques in Catalysis (Dekker, New York, 1994)

  31. S. Acosta, R. Corria, D. Leclercq, P.H. Mutin, A. Vioux, Sol–gel Sci. Technol. 2, 25 (1994). doi:10.1007/BF00486208

    Article  CAS  Google Scholar 

  32. Y. Jaymes, A. Douy, P. Florian, D. Massiot, J.P. Loutures, Sol–gel Sci. Technol. 2, 367 (1994). doi:10.1007/BF00486272

    Article  CAS  Google Scholar 

  33. B.M. Weckhuysen, L.M. De Ridder, R.J. Grobet, R.A. Schoonheydt, J. Phys. Chem. 99, 320 (1995). doi:10.1021/j100001a048

    Article  CAS  Google Scholar 

  34. A. Abragam, The Principles of Nuclear Magnetism (Clarendon Press, Oxford, 1961)

  35. N. Bloembergen, Physica 15, 386 (1949). doi:10.1016/0031-8914(49)90114-7

    Article  CAS  Google Scholar 

  36. A. Carrington, A.D. McLachlan, Introduction to Magnetic Resonance (Harper & Row, New York, 1967)

  37. E. Heracleous, A.A. Lemonidou, J.A. Lercher, Appl. Catal. A 264, 73 (2004). doi:10.1016/j.apcata.2003.12.030

    Article  CAS  Google Scholar 

  38. C.C.S. Macedo, F.R. Abreu, A.P. Tavares, M.B. Alves, L.F. Zara, J.C. Rubima, P.A.Z. Suarez, J. Braz. Chem. Soc. 17, 1291 (2006). doi:10.1590/S0103-50532006000700014

    Article  CAS  Google Scholar 

  39. B.M. Weckhuysen, I.E. Wachs, R.A. Schoonheydt, Chem. Rev. 96, 3327 (1996). doi:10.1021/cr940044o

    Article  CAS  Google Scholar 

  40. Z.G. Szabo, K. Kamaras, S. Szebeni, I. Ruff, Specrochim. Acta 34a, 607 (1978). doi:10.1016/0584-8539(78)80059-2

    Article  CAS  Google Scholar 

  41. B.M. Weckhuysen, L.M. De Ridder, R.A. Schoonheydt, J. Phys. Chem. 97, 4756 (1993). doi:10.1021/j100120a030

    Article  CAS  Google Scholar 

  42. F. Cavani, M. Koutyrev, F. Trifirò, A. Bertolini, D. Ghisletti, R. Iezzi, A. Santucci, G. Del Piero, J. Catal. 158, 236 (1996). doi:10.1006/jcat.1996.0023

    Article  CAS  Google Scholar 

  43. R. Puurunen, B.M. Weckhuysen, J. Catal. 210, 418 (2002). doi:10.1006/jcat.2002.3686

    Article  CAS  Google Scholar 

  44. B.M. Weckhuysen, R.A. Schoonheydt, J.M. Jehng, I.E. Wachs, S.J. Cho, R. Ryoo, S. Kijlstra, E. Poels, J. Chem. Soc. Faraday Trans. 91, 3245 (1995). doi:10.1039/ft9959103245

    Article  CAS  Google Scholar 

  45. A. Cimino, D. Cordischi, S. De Rossi, G. Ferraris, D. Gazzoli, V. Indovina, M. Occhiuzzi, M. Valigi, J. Catal. 127, 761 (1991). doi:10.1016/0021-9517(91)90197-C

    Article  CAS  Google Scholar 

  46. F.D. Hardcastle, I.E. Wachs, J. Mol. Catal. 46, 173 (1988). doi:10.1016/0304-5102(88)85092-2

    Article  Google Scholar 

  47. D.H. Cho, S.D. Yim, G.H. Cha, J.S. Lee, Y.G. Kim, J.S. Chung, I.S. Nam, J. Phys. Chem. A 102, 7913 (1998). doi:10.1021/jp981927c

    Article  CAS  Google Scholar 

  48. S.D. Yim, D.J. Koh, I.S. Nam, Y.G. Kim, Catal. Lett. 64, 201 (2000). doi:10.1023/A:1019076112539

    Article  CAS  Google Scholar 

  49. O.F. Gorriz, L.E. Cadús, Appl. Catal. A 180, 247 (1999). doi:10.1016/S0926-860X(98)00344-5

    Article  CAS  Google Scholar 

  50. M. Cherian, M.S. Rao, A.M. Hirt, I.E. Wachs, G. Deo, J. Catal. 211, 482 (2002)

    CAS  Google Scholar 

  51. A.B. Gaspar, J.L.F. Brito, L.C. Dieguez, J. Mol. Catal. Chem. 203, 251 (2003). doi:10.1016/S1381-1169(03)00381-9

    Article  CAS  Google Scholar 

  52. A.B. Gaspar, L.C. Dieguez, Appl. Catal. 227, 241 (2002). doi:10.1016/S0926-860X(01)00942-5

    Article  CAS  Google Scholar 

  53. B.M. Weckhuysen, A.A. Verberckmoes, A.R. De Baets, R.A. Schoonheydt, J. Catal. 166, 160 (1997). doi:10.1006/jcat.1997.1518

    Article  CAS  Google Scholar 

  54. D. Shi, Z. Zhao, C. Xu, A. Duan, J. Liu, T. Dou, J. Mol. Catal. Chem. 245, 106 (2006). doi:10.1016/j.molcata.2005.09.031

    Article  CAS  Google Scholar 

  55. J.H. Hillier, V.R. Saunders, Chem. Phys. Lett. 9, 219 (1971). doi:10.1016/0009-2614(71)85034-0

    Article  CAS  Google Scholar 

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  1. Laboratoire de Chimie des Matériaux et Catalyse, Département de Chimie, Faculté des Sciences de Tunis, Campus Universitaire Tunis ElManar, 2092, Tunis, Tunisia

    F. Ayari, M. Mhamdi & A. Ghorbel

  2. Institut Charles Gerhardt Montpellier, UMR 5253, CNRS-UM2-ENSCM-UM1, Eq. “Matériaux Avancés pour la Catalyse et la Santé”, ENSCM (MACS – Site la Galéra), 8, rue Ecole Normale, 34296, Montpellier Cedex 5, France

    G. Delahay

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  1. F. Ayari
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Ayari, F., Mhamdi, M., Delahay, G. et al. Sol–gel derived mesoporous Cr/Al2O3 catalysts for SCR of NO by ammonia. J Porous Mater 17, 265–274 (2010). https://doi.org/10.1007/s10934-009-9288-1

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