Kinetic and mechanistic studies on the Koelbel-Engelhardt reaction over an iron oxide catalyst.
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概要
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The yield and selectivity to hydrocarbons in the Kölbel-Engelhardt (KE) reaction over a Fe<SUB>2</SUB>O<SUB>3</SUB> catalyst at 548–593 K under atmospheric pressure were as low as 0.6–2.2% and 2.0–3.8%, respectively, but the observed four characteristic features of the reaction, <I>i.e.</I>, the distribution of produced hydrocarbons following the Schulz-Flory plot, the decrease in propagation probability with increasing reaction temperature, nearly the same value of propagation probability irrespective of a great change in contact time of the reaction, and the remarkable decrease in the yield ratio of olefins to paraffins with increasing contact time of the reaction agreed with the common features of the synthesis of hydrocarbons by the Fischer-Tropsch reaction. The catalyst was composed of Fe<SUB>3</SUB>O<SUB>4</SUB> with a low concentration of χ-type carbide (Fe<SUB>5</SUB>C<SUB>2</SUB>) during the KE reaction, and the results of the effect of contact time on the reaction revealed that formation of hydrocarbons took place following the water-gas shift (WGS) reaction. Furthermore, both the rates of formation of hydrocarbons in the reactions of carbided iron catalyst (Fe<SUB>5</SUB>C<SUB>2</SUB>) with H<SUB>2</SUB>O and with H<SUB>2</SUB> at 573 K were smaller by a factor of >5 than the rate of formation of hydrocarbons in the KE reaction at a steady state at 573 K. Thus, it is concluded that a much greater portion of hydrocarbons produced in the KE reaction was <I>via</I> a sequential reaction pathway involving the WGS reaction followed by the Fischer-Tropsch reaction, not <I>via</I> the decomposition of carbided iron catalyst with H<SUB>2</SUB>O and its reduction with H<SUB>2</SUB>. Based on the observed increase in the catalytic activity of Fe<SUB>2</SUB>O<SUB>3</SUB> upon addition of a small amount of such metal oxides as Cu, Pt, Co, Ni, and Rh oxides, the mechanical mixture of a WGS reaction catalyst and a Fischer-Tropsch reaction catalyst is proposed to be an effective catalyst for the production of hydrocarbons and one illustration of this view is presented.
- 公益社団法人 日本化学会の論文
著者
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Akimoto Masamichi
Department Of Applied Chemistry And Biotechnology Faculty Of Engineering Niigata Institute Of Techno
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Miyata Yasushi
Department of Chemical Engineering, Tokyo Institute of Technology
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Ooba Nobukazu
Department of Chemical Engineering, Tokyo Institute of Technology
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Echigoya Etsuro
Department of Chemical Engineering, Tokyo Institute of Technology
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