Catalytic Conversion of Methane and Propylene to 1-Butene
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The oxidative cross-coupling of methane with propylene has been studied over several catalysts. A material containing 1.9 wt % Mn and 5 wt % NaCl on SiO2 was found to be the most effective for this reaction. At 650°C, it was possible to attain selectivities to 1-butene and butadiene of 57% and 8.0%, respectively, at a propylene conversion of 38%. Experiments utilizing 13CH4 confirm that methane was indeed involved in the formation of the C4 products. Methyl radicals derived from CH4 and allyl radicals derived from C3D6 were simultaneously detected over the catalysts using a matrix isolation electron spin resonance method. These surface-generated radicals enter the gas phase, where most of the coupling is believed to occur. In addition to the cross-coupling reaction, methyl radicals couple to form ethane, and allyl radicals couple to form 1,5-hexadiene. The latter hydrocarbon reacts extensively back to propylene over the catalysts at 650°C.
author list (cited authors)
Lunsford, J. H., Rosynek, M. P., Smith, C. E., Xu, M., & Yu, Z.