Abstract
Hydrogen exchange between undeuterated and perdeuterated light alkanes (CD4-C3H8, C3D8-C3H8) occurs on H-ZSM5 and on Ga- and Zn-exchanged H-ZSM5 at 773 K. Alkane conversion to aromatics occurs much more slowly because it is limited by rate of disposal of H-atoms formed in C-H scission steps and not by C-H bond activation. Kinetic coupling of these C-H activation steps with hydrogen transfer to acceptor sites (Gan+, Znm+) and ultimately to stoichiometric hydrogen acceptors (H+, CO2,O2, CO) often increases alkane activation rates and the selectivity to unsaturated products. Reactions of13 CH4/C3H8 mixtures at 773 K lead only to unlabelled alkane, alkene, and aromatic products, even though exchange between CD4 and C3H8 occurs at these reaction conditions. This suggests that the non-oxidative conversion of CH4 to higher hydrocarbons on solid acids is limited by elementary steps that occur after the initial activation of C-H bonds.
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References
G.A. Olah and J. Lucas, J. Am. Chem. Soc. 89 (1967) 2227, 4743;
G. A. Olah and R.H. Schlossberg, J. Am. Chem. Soc. 90 (1968) 2276.
R. Periana, D.J. Taube, E.R. Evitt, D.G. Loffler, P.R. Wentrcek, G. Voss and T. Masuda, Science 259 (1993) 340.
D.E. Walsh, S. Han and R.E. Palermo, J. Chem. Soc. Chem. Commun (1991) 1259;
S. Han, D.J. Martenak, R.E. Palermo, J.A. Pearson and D.E. Walsh, J. Catal. 136 (1992) 578.
J.R. Mawry, R.F. Anderson and J.A. Johnson, Oil Gas J. 83 (1985) 1288.
H. Kitagawa, Y. Sendoda and Y. Ono, J. Catal. 101 (1986) 12.
T. Mole, J.R. Anderson and G. Greer, Appl. Catal. 17 (1985) 141.
E. Iglesia, J.E. Baumgartner and G.L. Price, J. Catal. 134 (1992) 549.
E. Iglesia, J.E. Baumgartner and G.D. Meitzner, in:Proc. 10th Int. Congr. on Catalysis, Budapest 1992, eds. L. Guczi, F. Solymosi and P. Tétényi (Elsevier, Amsterdam), in press.
G.D. Meitzner, E. Iglesia, J.E. Baumgartner and E.S. Huang, J. Catal. 140 (1993) 209.
J.S. Lee and S.T. Oyama, Catal. Rev.-Sci. Eng. 30 (1988) 249.
J.H. Lunsford, Langmuir 5 (1989) 12.
Y. Amenomiya, V.I. Birss, M. Goladzinowski, J. Galuszka and A.R. Sanger, Catal. Rev.-Sci. Eng. 32 (1990) 163.
E. Iglesia, J.E. Baumgartner, G.L. Price, J.L. Robbins and K.D. Rose, J. Catal. 125 (1990) 95.
G.L. Price and E. Iglesia, Ind. Eng. Chem. Res. 28 (1989) 839.
S. Delaverenne, M. Simon, M. Fauconet and J. Sommer, J. Chem. Soc. Chem. Commun. 15 (1989) 1049;
J. Bukala, J.C. Oilman and J. Sommer, J. Chem. Soc. Chem. Commun 6 (1992) 481.
H. Hamada, Y. Kintaichi, M. Sasaki, M. Tabata and T. Ito, Appl. Catal. 64 (1990) Ll.
K. Yogo, S. Tanaka, M. Ihara, T. Hishiki and E. Kikuchi, Chem. Lett. (1992) 1025.
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Iglesia, E., Baumgartner, J.E. Hydrogen transfer and activation of propane and methane on ZSM5-based catalysts. Catal Lett 21, 55–70 (1993). https://doi.org/10.1007/BF00767371
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DOI: https://doi.org/10.1007/BF00767371