Catalysis by alkaline earth metal oxides. I. The mechanism of ethylene hydrogenation on calcium oxide.
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概要
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The mechanism of ethylene hydrogenation on a thermally activated CaO was studied in the overall temperature range of 197–623 K. The maximum in the reaction rate was observed around 320 K, while the activation energy was found to vary with the range of reaction temperatures, <I>i.e.,</I> 12.6 kJ/mol (197–273 K) and −16.7 kJ/mol (373–623 K). The partial pressure dependence of the rate was also different in these ranges; the reaction orders with respect to the hydrogen and ethylene pressures were 0.7 and nearly zero at 273 K respectively, whereas the orders shifted to 1.0 and 0.9 at 523 K in the pressure range from 6 to 40 Torr (1 Torr=133.3 Pa). The reaction with deuterium at 523 K produced ethane containing widely distributed deuterium and was accompanied by the formation of highly-exchanged ethylene, HD, and H<SUB>2</SUB> molecules in the gas phase. On the contrary, the reaction at 273 K formed ethane [D<SUB>2</SUB>] (>60%) selectively, and the hydrogen-deuterium exchange occurred to a lesser extent in both ethylene and deuterium. By the proposed associative mechanism, the variation in the kinetic behavior with the temperature was explained in terms of the change in the slow step from the reaction between the adsorbed hydrogen and surface ethylene to the hydrogenation of the ethyl radical. The poisoning of the hydrogenation by preadsorbed CO indicated that only 0.5% of the total surface atoms contributed actively to the reaction. On the basis of these results, the structures of active sites are 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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Kasama Kaname
Department of Chemistry, Tokyo Institute of Technology
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