Abstract
LiCl-Na2MoO4 was found to be an active catalyst for oxidative coupling of methane at temperatures around 620 °C. In these systems, the selectivity for the formation of C3-products exceeds the selectivity for the formation of C2-products. While the homogeneous reaction of CH4 and O2 leads to C3H6 as C3-product, the 50% LiCl-50% Na2MoO4 catalyst leads to C3H8 as the predominant C3-product, indicating that in the latter case the reaction cannot be purely homogeneous. The dependency of the product distribution on temperature, gas composition, reactor dimensions, flow rate, CH4/O2 ratio and type of catalyst has been studied. The reaction was studied by co-feeding CH4, O2 and a diluent gas at atmospheric pressure continuously in a conventional flow reactor containing the catalyst. The reaction products observed were: C2H4, C2H6, C3H6, C3H8, H2O and CO + CO2. The two latter gases were the main oxidation products observed. Characterization of the catalysts used was carried out by X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD).
Similar content being viewed by others
References
G.E. Keller and M.M. Bhasin, J. Catal. 73 (1982) 9.
G.J. Hutchings, M.S. Scurrell and J.R. Woodhouse, Chem. Soc. Rev. 18 (1989) 251.
J.R. Anderson, Appl. Catal. 47 (1989) 177.
J.C. Mackie, Catal. Rev. Sci-Eng. 33 (1991) 169.
J. Kiwi, K.R. Thampi and M. Grätzel, J. Chem. Soc. Chem. Commun. (1990) 1690.
J. Kiwi, K.R. Thampi, M. Grätzel, P. Albers and K. Seibold, J. Phys. Chem. 96 (1992) 1344.
H. Matsuhashi, K. Sakurai and K. Arata, Chem. Lett. 4 (1989) 585.
M. Baerns, Catal. Today 1 (1987) 357.
J. Carreiro and M. Baerns, React. Kinet. Catal. Lett. 35 (1987) 349.
J.M. Berty, Appl. Ind. Catal. 1 (1983) 207.
C.F. Cullis, D.E. Keene and D.L. Trimm, J. Catal. 19 (1970) 378.
R. Burch, G.D. Squire and S.C. Tsang, Appl. Catal. 46 (1989) 69.
R. Burch, S. Chalker, G.D. Squire and S.C. Tsang, J. Chem. Soc. Faraday Trans. 86 (1990) 1607.
R. Burch, S. Chalker and P. Loader,Proc. Xth Int. Congr. on Catalysis, Budapest 1992, pp. 8–17.
D.C. Yates and N.E. Zlotin, J. Catal. 124 (1990) 562.
M. Hatano, P. Hinson, K.S. Vines and J.H. Lunsford, J. Catal. 124 (1990) 557.
Z. Kalenik and E. Wolf, J. Catal. 124(1990)566.
G. Lane, E. Miro and E. Wolf, J. Catal. 119 (1989) 161.
T.A. Garibyan and L. Ya. Margolis, Catal. Rev. Sci-Eng. 31 (1990) 355.
E. Drauglis and R. Jaffe,The Physical Basis for Heterogeneous Catalysis (Plenum Press, New York, 1975).
R. Busey and O. Keller, J. Chem. Phys. 41 (1964) 215.
S.J. Korf, J.A. Roos, N.A. de Bruijn, J.G. van Ommen and J.R. Ross, J. Chem. Soc. Chem. Commun. (1987) 1433.
T. Komatsu, T. Amaya and K. Otsuka, Catal. Lett. 3 (1989) 317.
T. Ito, J.-X. Wang, C.-H. Lin and J.H. Lunsford, J. Am. Chem. Soc. 107 (1985) 5062.
H. Zanthoff and M. Baerns, Ind. Eng. Chem. Res. 29 (1990) 2.
V. Kazansky and B. Shelimov, Res. Chem. Interm. 15(1991) 1.
E. Tsang and P. Hampton, J. Phys. Chem. Data 15 (1986) 1087.
A. Proctor and P. Sherwood, Anal. Chem. 52 (1980) 2315.
C.D. Wagner,Handbook of X-ray Photoelectron Spectroscopy (Perkin Elmer, Phys. Elect. Div., Minneapolis, 1979).
T.A. Patterson, J.C. Carrer, D.E. Leyden and D.M. Hercules, J. Phys. Chem. 80 (1976) 1700.
S.O. Grim and L.J. Matienzo, Inorg. Chem. 14 (1975) 1014.
Author information
Authors and Affiliations
Rights and permissions
About this article
Cite this article
Kiwi, J., Ravidranathan Thampi, K., Mouaddib, N. et al. Oxidative coupling of methane. The effect of alkali chlorides on molybdate based catalyst leading to high selectivity in C3-product formation. Catal Lett 18, 15–26 (1993). https://doi.org/10.1007/BF00769494
Received:
Accepted:
Issue Date:
DOI: https://doi.org/10.1007/BF00769494