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On the role of adsorbed atomic oxygen and CO2 in copper based methanol synthesis catalysts

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Abstract

The role of adsorbed atomic oxygen in methanol synthesis is investigated by a series of transient experiments of the interaction of CO and CO2 with a ternary Cu/ZnO/Al2O3 catalyst under methanol synthesis conditions. In particular, the response of adding CO and CO2 aspulses and assteps to the reaction gas mixture is studied. Hereby it is possible to study both the formation of CO2 from the reaction of adsorbed atomic oxygen (O-*) with CO, and the dissociation of CO2 in situ, i.e., while the catalyst is producing methanol. The experiments show no evidence of a significant coverage of O-* under methanol synthesis conditions. In addition, it is shown that CO2 is the main carbon source in methanol synthesis under the given conditions.

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References

  1. J.C.J. Bart and R.P.A. Sneeden, Catal. Today 2 (1987) 1.

    Google Scholar 

  2. G.C. Chinchen, K.C. Waugh and D.A. Whan, Appl. Catal. 25 (1986) 101.

    Google Scholar 

  3. J.L. Robbins, E. Iglesia, C.P. Kelkar and B. DeRites,Catal. Lett. 10 (1991) 1.

    Google Scholar 

  4. K. Klier, Adv. Catal. 31 (1982) 243.

    Google Scholar 

  5. L.E.Y. Nonneman and V. Ponec, Catal. Lett. 7 (1990) 213.

    Google Scholar 

  6. Y. Okamoto, K. Fukino, T. Imanaka and S. Teranishi, J. Chem. Soc. Chem. Commun. (1982) 1405; J. Phys. Chem. 87 (1983) 3747.

    Google Scholar 

  7. F. Trifirò, A. Vaccari, G. Del Piero, V. Fattore and B. Notari,Proc. 5th Int. Symp. on Heterogeneous Catalysis, Varna, 3–6 October 1983, Part II, p. 303.

  8. J.R. Rostrup-Nielsen and P.E. Højlund Nielsen, in:Deactivation and Poisoning of Catalysts, eds. J. Oudar and H. Wise (Dekker, New York, 1985) p. 259.

    Google Scholar 

  9. J.C. Frost, Nature 334 (1988) 577.

    Google Scholar 

  10. R. Burch, S.E. Golunski and M.S. Spencer, J. Chem. Soc. Faraday Trans. 86 (1990) 2683; Catal. Lett. 5 (1990) 55.

    Google Scholar 

  11. B.S. Clausen and H. Topsøe, Catal. Today 9 (1991) 189.

    Google Scholar 

  12. B.S. Clausen, G. Steffensen, B. Fabius, J. Villadsen, R. Feidenhans'l and H. Topsøe, J. Catal. 132 (1991) 524.

    Google Scholar 

  13. B.S. Clausen, L. Gråbæk, G. Steffensen, P.L. Hansen and H. Topsøe, Catal. Lett. 20 (1993) 23.

    Google Scholar 

  14. J.W. Couves, J.M. Thomas, D. Waller, R.H. Jones, A.J. Dent, G.E. Derbyshire and G.N. Greaves, Nature 354 (1991) 465.

    Google Scholar 

  15. G. Sankar, J.M. Thomas, D. Waller, J.W. Couves, C.R.A. Catlow and G.N. Greaves, J. Phys. Chem. 96 (1992) 7485.

    Google Scholar 

  16. G.D. Moggridge, T. Rayment, R.M. Ormerod, M.A. Morris and R.M. Lambert, Nature 358 (1992) 658.

    Google Scholar 

  17. K. Tohji, Y. Udagawa, T. Mizushima and A. Ueno, J. Phys. Chem. 89 (1985) 5671.

    Google Scholar 

  18. T.L. Neils and J.M. Burlitch, J. Catal. 118 (1989) 79.

    Google Scholar 

  19. D. Duprez, Z. Ferhat-Hamida and M.M. Bettahar, J. Catal. 124 (1990) 1.

    Google Scholar 

  20. T.H. Fleisch and R.L. Mieville, J. Catal. 90 (1984) 165.

    Google Scholar 

  21. G.G. Chinchen, M.S. Spencer, K.C. Waugh and D.A. Whan, J. Chem. Soc. Faraday Trans. I 83 (1987) 2193.

    Google Scholar 

  22. J. Szanyi and D.W. Goodman, Catal. Lett. 10 (1991) 383.

    Google Scholar 

  23. P.B. Rasmussen, P.M. Holmblad, T. Askgaard, C.V. Ovesen, P. Stoltze, J.K. Nørskov and I. Chorkendorff, to be published.

  24. I. Dybkjær, P.E. Højlund Nielsen and J. Bøgild Hansen, Synthesis of methanol on Cu-based catalyst, paper presented at the 73rd Annual Meeting AIChe, New Orleans, 1980.

  25. Y. Amenomiya and T. Tagawa, in:Proc. 8th Int. Congr. on Catalysis, Vol. 2 (Dechema, Berlin, 1984) p. 557.

    Google Scholar 

  26. G.G. Chinchen, P.J. Denny, D.G. Parker, M.S. Spencer and D.A. Whan, Appl. Catal. 30 (1987) 333.

    Google Scholar 

  27. A.Ya. Rozovskii, Russian Chem. Rev. 58 (1989) 41.

    Google Scholar 

  28. P.A. Taylor, P.B. Rasmussen, C.V. Ovesen, P. Stoltze and I. Chorkendorff, Surf. Sci. 261 (1992) 191.

    Google Scholar 

  29. M. Muhler, L.P. Nielsen, E. Törnqvist, B.S. Clausen and H. Topsøe, Catal. Lett. 14 (1992) 241.

    Google Scholar 

  30. G.G. Chinchen and K.C. Waugh, J. Catal. 97 (1986) 280.

    Google Scholar 

  31. M. Bowker, R.A. Hadden, H. Houghton, J.N.K. Hyland and K.C. Waugh, J. Catal. 109 (1988) 263.

    Google Scholar 

  32. G.G. Chinchen, C.M. Hay, H.D. Vandervell and K.C. Waugh, J. Catal. 103 (1987) 79.

    Google Scholar 

  33. B.S. Clausen, L. Gråbæk, C. Ovesen, H. Topsøe, J. Schiøtz, K.V. Jakobsen and J.K. Nørskov, Catal. Lett., submitted.

  34. C.T. Campbell, Appl. Catal. 32 (1987) 367.

    Google Scholar 

  35. J. Nakamura, J.A. Rodriguez and C.T. Campbell, J. Phys.: Condens. Matter 1 (1989) SB149.

    Google Scholar 

  36. P.B. Rasmussen, P.A. Taylor and I. Chorkendorff, Surf. Sci. 269/270 (1992) 352;

    Google Scholar 

  37. I. Chorkendorff, P.B. Rasmussen, H. Christoffersen and P.A. Taylor, Surf. Sci. 287/288 (1993) 208.

    Google Scholar 

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On leave from Institute of Physics, University of Aarhus, DK-8000 Aarhus C, Denmark.

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Muhler, M., Törnqvist, E., Nielsen, L.P. et al. On the role of adsorbed atomic oxygen and CO2 in copper based methanol synthesis catalysts. Catal Lett 25, 1–10 (1994). https://doi.org/10.1007/BF00815409

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  • DOI: https://doi.org/10.1007/BF00815409

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