Abstract
Mechanistic considerations show that pressure must be taken into account in evaluating oxidative coupling catalyst performance, and predict an upper limit of around 30% yield of higher hydrocarbons at one atmosphere.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
H. Mimoun, Nouv. J. Chim. 11 (1987) 513.
J.A. Roos, A.G. Bakker, H. Bosch, J.G. van Ommen and J.R.H. Ross, Catal. Today 1 (1987) 133.
J.A. Labinger and K.C. Ott, J. Phys. Chem. 91 (1987) 2682.
K. Otsuka, Q. Liu, M. Hatano and A. Morikawa, Chem. Lett. (1986) 903. It should also be noted that these and related results utilize chloride-containing catalysts, and there is evidence that gas-phase Cl species are responsible for some of the better performances; hence they degrade with use.
K. Aika, T. Moriyama, N. Takasaki and E. Iwamatsu, J. Chem. Soc., Chem. Commun. (1986) 1210.
I. Matsuura, T. Doi and Y. Utsumi, Chem. Lett. (1987) 1473.
C.A. Jones, J.J. Leonard and J.A. Sofranko, J. Catal. 103 (1987) 311
C.A. Jones, J.J. Leonard and J.A. Sofranko, Energy & Fuels 1 (1987) 12.
D.L. Grimmett, L. Breeden, C.E. McBride, A. Goldman and J.A. Labinger, unpublished results cited in Labinger et al., in:Catalysis 1987: Proceedings of the 10th North American Meeting of the Catalysis Society, ed. J.W. Ward (Elsevier, New York, 1988) p. 513.
T. Ito, J.-X. Wang, C.-H. Lin and J.H. Lunsford, J. Am. Chem. Soc. 107 (1985) 5062;
C.-H. Lin, K.D. Campbell, J.-X. Wang and J.H. Lunsford, J. Phys. Chem. 90 (1986) 534
K.D. Campbell, E. Morales and J.H. Lunsford, J. Am. Chem. Soc. 109 (1987) 7900.
Lunsford has noted that the C-H bond in ethylene isstronger than that in methane, and suggested that a catalyst might be found for which the former is less reactive and hence the constraints discussed here need not apply J.H. Lunsford, in:Methane Conversion, eds. D.M. Bibby, C.D. Chang, R.F. Howe and S. Yurchak (Elsevier, New York, 1988) 359.). However, since ethylene is more reactive even for gas-phase reactions with OH and related species, in spite of its stronger bond, it does not seem very likely that this could be achieved.
J.W. Sutherland, J.V. Michael and R.B. Klemm, J. Phys. Chem. 90 (1986) 5941. It may be noted in fig. 2 that this assumption produces curves that extrapolate to 100% selectivity at 0 conversion; i.e., there is no direct CO2 formation, and a still lower value fork 5 would not give any improvement.
J.L. Jezl, G.O. Michaels and M.J. Spangler, U.S. Patent 4,754,091 (1988).
A.M. Gaffney, C.A. Jones, J.J. Leonard, J.A. Sofranko and H.P. Withers, in:Catalysis 1987: Proceedings of the 10th North American Meeting of the Catalysis Society, ed. J.W. Ward (Elsevier, New York, 1988) 523.
Author information
Authors and Affiliations
Rights and permissions
About this article
Cite this article
Labinger, J.A. Oxidative coupling of methane: An inherent limit to selectivity?. Catal Lett 1, 371–375 (1988). https://doi.org/10.1007/BF00766166
Received:
Accepted:
Issue Date:
DOI: https://doi.org/10.1007/BF00766166