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.
Article PDF
Similar content being viewed by others
Explore related subjects
Discover the latest articles, news and stories from top researchers in related subjects.Avoid common mistakes on your manuscript.
References
J.C.J. Bart and R.P.A. Sneeden, Catal. Today 2 (1987) 1.
G.C. Chinchen, K.C. Waugh and D.A. Whan, Appl. Catal. 25 (1986) 101.
J.L. Robbins, E. Iglesia, C.P. Kelkar and B. DeRites,Catal. Lett. 10 (1991) 1.
K. Klier, Adv. Catal. 31 (1982) 243.
L.E.Y. Nonneman and V. Ponec, Catal. Lett. 7 (1990) 213.
Y. Okamoto, K. Fukino, T. Imanaka and S. Teranishi, J. Chem. Soc. Chem. Commun. (1982) 1405; J. Phys. Chem. 87 (1983) 3747.
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.
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.
J.C. Frost, Nature 334 (1988) 577.
R. Burch, S.E. Golunski and M.S. Spencer, J. Chem. Soc. Faraday Trans. 86 (1990) 2683; Catal. Lett. 5 (1990) 55.
B.S. Clausen and H. Topsøe, Catal. Today 9 (1991) 189.
B.S. Clausen, G. Steffensen, B. Fabius, J. Villadsen, R. Feidenhans'l and H. Topsøe, J. Catal. 132 (1991) 524.
B.S. Clausen, L. Gråbæk, G. Steffensen, P.L. Hansen and H. Topsøe, Catal. Lett. 20 (1993) 23.
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.
G. Sankar, J.M. Thomas, D. Waller, J.W. Couves, C.R.A. Catlow and G.N. Greaves, J. Phys. Chem. 96 (1992) 7485.
G.D. Moggridge, T. Rayment, R.M. Ormerod, M.A. Morris and R.M. Lambert, Nature 358 (1992) 658.
K. Tohji, Y. Udagawa, T. Mizushima and A. Ueno, J. Phys. Chem. 89 (1985) 5671.
T.L. Neils and J.M. Burlitch, J. Catal. 118 (1989) 79.
D. Duprez, Z. Ferhat-Hamida and M.M. Bettahar, J. Catal. 124 (1990) 1.
T.H. Fleisch and R.L. Mieville, J. Catal. 90 (1984) 165.
G.G. Chinchen, M.S. Spencer, K.C. Waugh and D.A. Whan, J. Chem. Soc. Faraday Trans. I 83 (1987) 2193.
J. Szanyi and D.W. Goodman, Catal. Lett. 10 (1991) 383.
P.B. Rasmussen, P.M. Holmblad, T. Askgaard, C.V. Ovesen, P. Stoltze, J.K. Nørskov and I. Chorkendorff, to be published.
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.
Y. Amenomiya and T. Tagawa, in:Proc. 8th Int. Congr. on Catalysis, Vol. 2 (Dechema, Berlin, 1984) p. 557.
G.G. Chinchen, P.J. Denny, D.G. Parker, M.S. Spencer and D.A. Whan, Appl. Catal. 30 (1987) 333.
A.Ya. Rozovskii, Russian Chem. Rev. 58 (1989) 41.
P.A. Taylor, P.B. Rasmussen, C.V. Ovesen, P. Stoltze and I. Chorkendorff, Surf. Sci. 261 (1992) 191.
M. Muhler, L.P. Nielsen, E. Törnqvist, B.S. Clausen and H. Topsøe, Catal. Lett. 14 (1992) 241.
G.G. Chinchen and K.C. Waugh, J. Catal. 97 (1986) 280.
M. Bowker, R.A. Hadden, H. Houghton, J.N.K. Hyland and K.C. Waugh, J. Catal. 109 (1988) 263.
G.G. Chinchen, C.M. Hay, H.D. Vandervell and K.C. Waugh, J. Catal. 103 (1987) 79.
B.S. Clausen, L. Gråbæk, C. Ovesen, H. Topsøe, J. Schiøtz, K.V. Jakobsen and J.K. Nørskov, Catal. Lett., submitted.
C.T. Campbell, Appl. Catal. 32 (1987) 367.
J. Nakamura, J.A. Rodriguez and C.T. Campbell, J. Phys.: Condens. Matter 1 (1989) SB149.
P.B. Rasmussen, P.A. Taylor and I. Chorkendorff, Surf. Sci. 269/270 (1992) 352;
I. Chorkendorff, P.B. Rasmussen, H. Christoffersen and P.A. Taylor, Surf. Sci. 287/288 (1993) 208.
Author information
Authors and Affiliations
Additional information
On leave from Institute of Physics, University of Aarhus, DK-8000 Aarhus C, Denmark.
Rights and permissions
About this article
Cite this article
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
Received:
Revised:
Issue Date:
DOI: https://doi.org/10.1007/BF00815409