Catalysis by mixed oxide perovskites. II. The hydrogenolysis of C3-C5 hydrocarbons on LaCoO3.
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概要
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The catalytic hydrogenolysis of C<SUB>3</SUB>–C<SUB>5</SUB> alkanes on LaCoO<SUB>3</SUB> perovskite oxide was found to show a highly selective formation of methane in the temperature range of 350–620 K. The reaction order with respect to the hydrocarbon pressure was unity in every hydrogenolysis, whereas the hydrogen order increased from zero for propane to 1.0 for butane and isobutane and to 2.0 for pentane, isopentane, and neopentane. The activation energies of the reactions ranged from 120 for propane to 32 kJ mol<SUP>−1</SUP> for butane. The reaction of propane or butane with D<SUB>2</SUB> on LaCoO<SUB>3</SUB> provided large fractions of methane [D<SUB>3</SUB>] and [D<SUB>4</SUB>], but a negligible amount of deuterium-exchanged alkanes. An equilibrium among the gaseous H<SUB>2</SUB>, HD, and D<SUB>2</SUB> was reached. These hydrogenolyses are described by a mechanism involving the almost concurrent repture of all the carbon-carbon bonds in the alkanes by the attack of adsorbed hydrogen atoms, and were proposed to be catalyzed by a synergetic effect; the CO<SUP>3+</SUP> ion is effective in breaking the C–C bond, whereas the La<SUP>3+</SUP> and O<SUP>2−</SUP> ions serve to supply hydrogen atoms to the decomposed species. The reaction of propene or butenes with hydrogen produced the corresponding alkanes and methane. The kinetic analyses showed that the fractions of methane produced consecutively <I>via</I> the alkanes amounted to 16% for propene and to more than 93% for butenes. The observed pressure dependence and deuterium distributions in the alkene hydrogenation were interpreted in terms of the associative mechanism. The correlation between the structures of the reactant molecules and of the active sites present on LaCoO<SUB>3</SUB> was briefly discussed.
- 公益社団法人 日本化学会の論文
著者
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INOUE Yasunobu
Department of Chemistry, Nagaoka University of Technology
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Yasumori Iwao
Department Of Applied Chemistry Faculty Of Engineering Kanagawa University
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Ichimura Kenji
Department of Chemistry, Tokyo Institute of Technology
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