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Kinetic study of the catalytic oxidation of alkanes over nickel, palladium, and platinum foils

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Abstract

The kinetics of the total oxidation of alkanes (methane, ethane, propane, n-butane and isobutane) over Ni, Pd, and Pt foils was studied under fuel-lean conditions by using a recirculating batch reactor with mass spectrometry detection. Approximate first- and zeroth-order kinetics with respect to the hydrocarbon and oxygen concentrations, respectively, was observed in all cases. Significantly slower rates were seen for methane conversion, but other subtle changes were also identified among the other hydrocarbons as well. The reactivity trends could be clearly correlated with C-H bond strengths, since higher rates were seen for the longer and more branched hydrocarbon chains. Also, platinum was found to be the most active catalyst for the oxidation of all the compounds studied here except methane, which is oxidized faster on the nickel substrate. The variations in activity among the three catalysts were shown to be associated mostly with changes in the pre-exponential factor, not the activation energy, suggesting that they have to do with the surface density of active sites on the surface. The nature of the active catalyst during reaction was determined by simple inspection to be the metallic phase in the cases of Pt and Ni but an oxide layer in the case of Pd.

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References

  1. R.B. Anderson, K.C. Stein, J.J. Feenan and L.J.E. Hofer, Ind. Eng. Chem. 53 (1961) 809.

    Article  CAS  Google Scholar 

  2. J.G. Firth, Trans. Faraday Soc. 52 (1966) 2566.

    Article  Google Scholar 

  3. R.E. Roberts and J.B. Roberts, J. Air Pollut. Control Assoc. 26 (1976) 353.

    Google Scholar 

  4. A.E.R. Budd, Environ. Pollut. Manag. (1978) 13.

  5. J.J. Spivey, Ind. Eng. Chem. Res. 26 (1987) 2165.

    Article  CAS  Google Scholar 

  6. M.R. Dongworth and A. Melvin, 16th Int. Symp. in Combustion, MIT, 1976, p. 255.

  7. A. Nishino, Catal. Today 10 (1991) 107.

    Article  CAS  Google Scholar 

  8. S.W. Radcliffe and R.G. Hickman, J. Inst. Fuel 48 (1975) 208.

    CAS  Google Scholar 

  9. D.L. Trimmand C.W. Lam, Chem. Eng. Sci. 35 (1980) 1731.

    Article  Google Scholar 

  10. W.V. Krill, J.P. Kesselring, E.K. Chu and R.M. Kendall, Mech. Eng. 102 (1980) 28.

    CAS  Google Scholar 

  11. S.M. DeCorso, S. Mumford, R.V. Carruba and R. Heck, J. Eng. Power 99 (1977) 159.

    CAS  Google Scholar 

  12. W.C. Pfefferle, J. Energy 2 (1978) 142.

    Article  CAS  Google Scholar 

  13. B.E. Enga and D.T. Thompson, Plat. Met. Rev. 23 (1979) 134.

    CAS  Google Scholar 

  14. J. Tsuji and K. Ohno, Synthesis 157 (1969) 1.

    Google Scholar 

  15. J.P. Kesserling, in: Advanced Combustion Methods, ed. F.J. Weinberg (Academic Press, New York, 1986) p. 237.

    Google Scholar 

  16. J. Wei, Adv. Catal. 24 (1975) 57.

    Article  CAS  Google Scholar 

  17. K.C. Taylor, Automobile Catalytic Converters (Springer, Berlin, 1984).

    Google Scholar 

  18. R.J. Farrauto, R.M. Heck and B.K. Speronello, Chem. Eng. News (7 Sept.) (1992) 34.

  19. H.S. Gandhi and M. Shelef, in: Catalysis and Automotive Pollution Control, eds. A. Crucq and A. Frennet (Elsevier, Amsterdam, 1987) p. 199.

    Google Scholar 

  20. J.G. Firth and H.B. Holland, Trans. Faraday Soc. 65 (1969) 1121.

    Article  CAS  Google Scholar 

  21. D.L. Trimm, Appl. Catal. 7 (1983) 249.

    Article  CAS  Google Scholar 

  22. G.I. Golodets, Heterogeneous Catalytic Reactions Involving Molecular Oxygen, Studies in Surface Science and Catalysis Series, Vol. 15 (Elsevier, Amsterdam, 1983).

    Google Scholar 

  23. R. Burch and M.J. Hayes, J. Mol. Catal.A100 (1995) 13.

    Article  CAS  Google Scholar 

  24. M. Niwa, K. Awano and Y. Murakami, Appl. Catal. 7 (1983) 317.

    Article  CAS  Google Scholar 

  25. C.F. Cullis and B.M. Williatt, J. Catal. 86 (1984) 187.

    Article  CAS  Google Scholar 

  26. R.F. Hicks, H. Qi, M.L. Young and R.G. Lee, J. Catal. 122 (1990) 295.

    Article  CAS  Google Scholar 

  27. T.R. Baldwin and R. Burch, Appl. Catal. 66 (1990) 359.

    Article  CAS  Google Scholar 

  28. P. Briot and M. Primet, Appl. Catal. 68 (1991) 301.

    Article  CAS  Google Scholar 

  29. S. Oh, P.J. Mitchell and R.M. Siewert, J.Catal. 132 (1991) 287.

    Article  CAS  Google Scholar 

  30. K. Otto, L.P. Haack and J.E. De Vries, Appl. Catal. B 1 (1992) 1.

    Article  CAS  Google Scholar 

  31. R.J. Farrauto, M.C. Hobson, T. Kennelly and E.M. Waterman, Appl. Catal.A81 (1992) 227.

    Article  CAS  Google Scholar 

  32. P.E. Marti, M. Maciejewski and A. Baiker, J. Catal. 141 (1993) 494.

    Article  CAS  Google Scholar 

  33. F.H. Ribeiro, M. Chow and R.A. Dalla Betta, J. Catal. 146 (1994) 537.

    Article  CAS  Google Scholar 

  34. E. Garbowski, C. Feumi-Jantou, N. Mouaddib and M. Primet, Appl. Catal. 109 (1994) 277.

    Article  CAS  Google Scholar 

  35. S.S. Peri and C.R.F. Lund, J. Catal. 152 (1995) 410.

    Article  CAS  Google Scholar 

  36. R. Burch and F.J. Urbano, Appl. Catal.A124 (1995) 121.

    Article  CAS  Google Scholar 

  37. P. Salomonsson, S. Johansson and B. Kasemo, Catal. Lett. 33 (1995) 1.

    Article  CAS  Google Scholar 

  38. S. Su, J. Carstens and A.T. Bell, 15th Meeting North American Catalysis Society, Chicago 1997, paper D21, p. 91.

  39. K. Fujimoto, F.H. Ribeiro, M. Avalos-Borja and E. Iglesias, 15th Meeting North American Catalysis Society, Chicago 1997, paperD23, p. 93.

  40. M.A. Accomazzo and K. Nobe, Ind. Eng. Chem. Proc. Res. Develop. 4 (1965) 425.

    Article  CAS  Google Scholar 

  41. Y.-F.Y. Yao, Ind. Eng. Chem. Prod. Res. Develop. 19 (1980) 293.

    Article  CAS  Google Scholar 

  42. A. Schwartz, L.L. Holbrook and H. Wise, J. Catal. 21 (1971) 199.

    Article  CAS  Google Scholar 

  43. C.A. Müller, M. Maciejewski, R.A. Koeppel and A. Baiker, J. Catal. 166 (1997) 36.

    Article  Google Scholar 

  44. R.F. Hicks, H. Qi, M.L. Young and R.G. Lee, J. Catal. 122 (1990) 280.

    Article  CAS  Google Scholar 

  45. K. Otto, Langmuir 5 (1989) 1364.

    Article  CAS  Google Scholar 

  46. J.G. McCarty, Catal. Today 26 (1995) 283.

    Article  CAS  Google Scholar 

  47. R. Burch, F.J. Urbano and P.K. Loader, Appl. Catal. A 123 (1995) 173.

    Article  CAS  Google Scholar 

  48. L. Hiam, H. Wise and S. Chaikin, J. Catal. 9/10 (1968) 272.

    Article  Google Scholar 

  49. C.F. Cullis and T.G. Nevell, Proc. Roy. Soc. London A 349 (1976) 523.

    Article  CAS  Google Scholar 

  50. V.A. Drozdov, P.G. Tsyrulnikov, V.V. Popovskii, N.N. Bulgakov, E.M. Moroz and T.G. Galeev, React. Kinet. Catal. Lett. 27 (1985) 425.

    Article  CAS  Google Scholar 

  51. M.F.M. Zwinkels, S.G. Järås and P.G. Menon, Catal. Rev.-Sci. Eng. 35 (1993) 319.

    CAS  Google Scholar 

  52. A. Loaiza, M. Xu and F. Zaera, J. Catal. 159 (1996) 127.

    Article  CAS  Google Scholar 

  53. R.C. Weast, ed., CRC Handbook of Chemistry and Physics (CRC Press, Cleveland, 1974).

    Google Scholar 

  54. G.C. Bond, Catalysis by Metals (Academic Press, London, 1962).

    Google Scholar 

  55. B.C. Gates, J.R. Katzer and G.C.A. Schuit, Chemistry of Catalytic Processes (McGraw-Hill, New York, 1979).

    Google Scholar 

  56. M.F. Umstead, F.G. Woods and J.E. Johnson, J. Catal. 5 (1966) 293.

    Article  Google Scholar 

  57. J.E. Johnson, J.G. Christian and H.W. Carhart, Ind. Eng. Chem. 53 (1961) 900.

    Article  CAS  Google Scholar 

  58. J.R. Regalbuto, An Analysis of Post-Combustion Catalytic Emissions Treatment, Gas Research Institute, Final Task Report GRI 92/0445 (1992).

  59. Y. Moro-oka, Y. Morikawa and A. Ozaki, J. Catal. 7 (1967) 23.

    Article  CAS  Google Scholar 

  60. J. Tsuji and K. Ohno, Tetrahedron Lett. (1970) 823.

  61. K.J. Laidler, Chemical Kinetics, 3rd Ed. (Harper and Row, New York, 1987).

    Google Scholar 

  62. C.T. Rettner, H.E. Pfnür and D.J. Auerbach, Phys. Rev. Lett. 54 (1985) 2716.

    Article  CAS  Google Scholar 

  63. S.G. Brass and G. Ehrlich, J. Chem. Phys. 87 (1987) 4285.

    Article  CAS  Google Scholar 

  64. A.C. Luntz and D.S. Bethune, J. Chem. Phys. 90 (1989) 1274.

    Article  CAS  Google Scholar 

  65. M.C. McMaster and R.J. Madix, Surf. Sci. 275 (1992) 265.

    Article  CAS  Google Scholar 

  66. W.H. Weinberg, Langmuir 9 (1993) 655.

    Article  CAS  Google Scholar 

  67. S.S. Bharadwaj and L.D. Schmidt, J. Catal. 146 (1994) 11.

    Article  CAS  Google Scholar 

  68. M. Huff, P.M. Torniainen and L.D. Schmidt, Catal. Today 21 (1994) 113.

    Article  CAS  Google Scholar 

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Authors
  1. M. Aryafar
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  2. F. Zaera
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Aryafar, M., Zaera, F. Kinetic study of the catalytic oxidation of alkanes over nickel, palladium, and platinum foils. Catalysis Letters 48, 173–183 (1997). https://doi.org/10.1023/A:1019055810760

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