SciELO - Scientific Electronic Library Online

 
vol.61 índice de autoresíndice de materiabúsqueda de artículos
Home Pagelista alfabética de revistas  

Servicios Personalizados

Articulo

Indicadores

Links relacionados

  • En proceso de indezaciónCitado por Google
  • En proceso de indezaciónSimilares en Google

Compartir


South African Journal of Chemistry

versión On-line ISSN 1996-840X
versión impresa ISSN 0379-4350

S.Afr.j.chem. (Online) vol.61  Durban  2008

 

RESEARCH ARTICLE

 

Synthesis, characterization and activity of sulphate-modified V2O5/SnO2 catalysts

 

 

Sreejarani K. Pillai; Omanakutty Gheevarghese*

Department of Chemistry, Tshwane University of Technology, Pretoria 0001, South Africa

 

 


ABSTRACT

Sulphate-modified V2O5/SnO2 catalysts were prepared by a simple impregnation method and characterized using different physicochemical techniques, such as EDX, BET-SA, XRD, FT-IR, TGA and 51V NMR spectroscopy. A simple, effective and environmentally friendly method for the gas phase conversion of cyclohexanone oxime to E-caprolactam by these modified catalysts is presented. The optimal protocol allows ε-caprolactam to be synthesized in excellent yields. NH3-TPD and cumene conversion reactions were used to determine the acid structural properties of the catalysts. Definite correlation was observed between the concentration of medium strength acid sites or Bronsted sites and the E-caprolactam selectivity. Time-on-stream studies showed fast decline in the activity of the catalyst resulting from the basic nature of the reactant and product molecules.

Keywords: Sulphated V2O5/SnO2 catalysts, acidity, vapour phase Beckmann rearrangement


 

 

Full text available only in pdf format.

 

 

References

1 J.E. Kent and S. Riegel, Handbook of Industrial Chemistry, 8th edn., Van Nostrand, New York, USA, 1983, p. 402.         [ Links ]

2 D.S. Mao, G.Z. Lu and Q.L. Chen, Appl. Catal. A. Gen, 2005, 279, 145-153.         [ Links ]

3 O. Immel, H.H. Schwarz, K. Starke and W. Swodenk, Chem. Ing. Tech., 1984, 56, 612-613.         [ Links ]

4 T. Ushikubo and K. Wada, J. Catal, 1994, 148, 138-148.         [ Links ]

5 D. Shouro, Y. Ohya, S. Mishima and T. Nakajima, Appl. Catal. A. Gen., 2001, 214, 59-67.         [ Links ]

6 K. Chaudhari, R. Bal, A. Chandwadkar and S. Sivasanker, J. Mol. Catal. A. Chem., 2002, 177, 247-253.         [ Links ]

7 L. Forni, C. Tosi, G. Fornassari, F. Trifiro, A. Vaccari and J.B. Nagy, J. Mol. Catal. A. Chem., 2004, 221, 97-103.         [ Links ]

8 G.P. Heitmann, G. Dahlhoff, J.P.M. Niederer and W.F. Hölderich, J. Catal., 2000, 194, 122-129.         [ Links ]

9 J.-C. Chang and A.-N. Ko, Catal. Today, 2004, 97, 241-247.         [ Links ]

10 T. Komatsu, T. Maeda and T. Yashima, Micropor. Mesopor. Mater., 2000, 35-36, 173-180.         [ Links ]

11 A. Aucejo, M.C. Burguet, A. Corma and V. Fornes, Appl. Catal., 1986, 22, 187-200.         [ Links ]

12 H. Ichihashi, M. Ishida, A. Shiga, M. Kitamura, T. Suzuki, K. Suenobu and K. Sugita, Catal. Survey Asia, 2003, 7, 261-270.         [ Links ]

13 M. Ghiaci, A. Abbaspur and R.J. Kalbasi, Appl. Catal. A. Gen., 2005,287, 83-88.         [ Links ]

14 D.S. Mao, G.Z. Lu, Q.L. Chen, Z.K. Xie and Y.X. Zhang, Catal. Lett, 2001, 77, 119-124.         [ Links ]

15 D.S. Mao, Q.L. Chen and G.Z. Lu, React. Kinet. Catal. Lett., 2002, 75, 75-80.         [ Links ]

16 D.S. Mao, G.Z. Lu and Q.L. Chen, Appl. Catal. A. Gen., 2005, 244, 145-153.         [ Links ]

17 X. Guo, W. Hou, W. Ding, Y. Fan, Q. Yan and Y. Chen, Micropor. Mesopor. Mater., 2005, 80, 269-274.         [ Links ]

18 K. Arata, Appl. Catal., 1996, 146, 3-32.         [ Links ]

19 J.G. Eon, R. Olier and J.-C. Volta, J. Catal., 1994, 145, 318-326.         [ Links ]

20 H.H. Kung and M.C. Kung, Appl. Catal. A, 1997, 157, 105-116.         [ Links ]

21 A. Khodakov, B. Olthof, A.T. Bell and E. Iglesia, J. Catal., 1999, 181, 205-216.         [ Links ]

22 I.E. Wachs, R.Y. Saleh, S.S. Chan and C.C. Chersch, Appl. Catal. A, 1985, 15, 339.         [ Links ]

23 H. Bosch and F. Janssen, Catal. Today, 1988, 15, 339-352.         [ Links ]

24 B.M. Reddy, A. Khan, Y. Yamada, T. Kobayashi, S. Loridant and J.-C. Volta, J. Phys. Chem. B, 2002, 106, 10964-10972.         [ Links ]

25 J. Matta, D. Courcot, E.A. Aad and A. Aboukais, Chem. Mater., 2002, 14, 4118-4125.         [ Links ]

26 J. Buiten, J. Catal., 1968, 10, 188-199.         [ Links ]

27 M. Ai and S. Suzuki, Shokubai, 1973, 15, 159.         [ Links ]

28 T. Seiyama, M. Egashira, T. Sakamoto and I. Aso, J. Catal., 1972, 24, 76-81.         [ Links ]

29 J.R. Sohn, S.G. Cho, Y.I. Pae and S. Hayashi, J. Catal., 1996, 150, 170-177.         [ Links ]

30 H. Matsuhashi, M. Hino and K. Arata, Appl. Catal., 1990, 59,205-212.         [ Links ]

31 A. Corma, Chem. Rev, 1995, 95, 559-614.         [ Links ]

32 X. Song and A. Sayari, Catal. Rev. Sci. Eng., 1996, 38, 329-412.         [ Links ]

33 A.K. Dalai, R. Sethuraman, S.P.R. Katikeneni and R.O. Idem, Ind. Eng. Chem. Res., 1998, 37, 3869-3878.         [ Links ]

34 S.K. Samantray, T. Mishra and K.M. Parida, J. Mol. Catal. A. Gen., 2000, 156, 267-274.         [ Links ]

35 K. Hadjiivanov, A. Davydov and D. Klissurski, Kinet. Catal., 1988, 29, 161-167.         [ Links ]

36 I. E. Wachs, Catal. Today, 1996, 27, 437-455.         [ Links ]

37 G. Busca, G. Centi, L. Marchetti and F. Trifiro, Langmuir, 1989, 2, 568-576.         [ Links ]

38 N.Y. Topsoe, H. Topsoe and J.A. Dumesic, J. Catal., 1995, 151, 226-240.         [ Links ]

39 C. Morterra, G. Cerrato, C. Emanuel and V. Bolis, J. Catal., 1993, 142, 349-367.         [ Links ]

40 M. Pontzi, C. Duschatzky, A. Carraseull and E. Ponzi, Appl. Catal. A. Gen., 1998, 169, 373-379.         [ Links ]

41 R. Srinivasan, R.A. Keogh, D.R. Milburn and B.H. Davis, J. Catal., 1995, 153, 123-130.         [ Links ]

42 H. Eckert, G. Deo, I. E. Wachs and A. M. Hirt, Coll. Surf., 1995, 45, 347-359.         [ Links ]

43 G. Deo and I.E. Wachs, J. Phys. Chem., 1991, 95, 5889-5895.         [ Links ]

44 F. Roozeboom, M.C. Mitteimeilijer, J.A. Moulijn, J. Medema, V.H. J. de Beer and P.J. Gellings, J. Phys. Chem., 1980, 84, 2783-2791.         [ Links ]

45 A. Francesco, D. Roberto and P. Adolfo, Appl. Catal. A. Gen., 1998, 170, 127-137.         [ Links ]

46 H.G. Karge and V Dondur, J. Phys. Chem., 1990, 94, 765-772.         [ Links ]

47 A. Corma and B.W. Wojciechowski, Catal. Rev. Sci. Eng., 1982, 24, 1-65.         [ Links ]

48 W. Przystajko, R. Fiedorow and I.G. Dalla Lana, Appl. Catal., 1985, 15, 265-272.         [ Links ]

49 T. Yamaguchi, Appl. Catal., 1990, 61, 1-25.         [ Links ]

50 A. Corma, V. Fornes, M.I. Juan Rajadell and J.M. Lopez Nieto, Appl. Catal. A. Gen., 1994, 116, 151-158.         [ Links ]

51 A. Clearfield, G.P.D. Serrete and A.H. Khazi-Syed, Catal. Today, 1994, 20, 295-312.         [ Links ]

52 M. Ai, J. Catal., 1975, 40, 318-326.         [ Links ]

53 M. Ai, Bull. Chem. Soc. Jpn., 1976, 49, 1328-1334.         [ Links ]

54 A. K. Dalai, R. Sethuraman, S.P.R. Katikeneni and R.O. Idem, Ind. Eng. Chem. Res., 1998, 37, 3869-3878.         [ Links ]

55 T. Curtin, J.B. McMonagle, M. Ruwett and B.K. Hodnett, J. Catal., 1993, 142, 172-181.         [ Links ]

56 BASF. Ger. Patent, No. 1, 1967, 227 028.         [ Links ]

57 B.-Q. Xu, S.-B. Cheng, S. Jiang and Q.-M. Zhu, Appl. Catal. A. Gen., 1999, 188, 361-368.         [ Links ]

58 D.S. Mao, Q.L. Chen and G.Z. Lu, Appl. Catal. A. Gen., 2003, 244, 273-282.         [ Links ]

59 D.S. Mao, G.Z. Lu and Q.L. Chen, Appl. Catal. A. Gen., 2005, 279, 145-153.         [ Links ]

 

 

Received 19 July 2007
Revised 8 February 2008
Accepted 13 February 2008

 

 

* To whom correspondence should be addressed: E-mail: gheevargheseo@tut.ac.za

Creative Commons License Todo el contenido de esta revista, excepto dónde está identificado, está bajo una Licencia Creative Commons