The CO-H2 reaction over ZrO2 to form isobutene selectively.
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概要
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The CO–H<SUB>2</SUB> reaction over ZrO<SUB>2</SUB> was studied in detail. Methanol and isobutene were selectively formed at 473–523 and 623–673 K, respectively. The activation energies for C<SUB>2</SUB>, C<SUB>3</SUB>, and linear C<SUB>4</SUB> hydrocarbon formation are 79, 84, and 96 kJ mol<SUP>−1</SUP> (523–723 K), while that for branched-chain C<SUB>4</SUB> hydrocarbons is about 210 kJ mol<SUP>−1</SUP> (523–623 K). At 673 K the rate of C<SUB>4</SUB> hydrocarbon formation is as follows: <I>r</I>=<I>kP</I><SUB>H<SUB>2</SUB></SUB>·<I>P</I>co<SUP>2</SUP>, while those of C<SUB>1</SUB>, C<SUB>2</SUB>, and C<SUB>3</SUB> are written by the functions having the maximum values regarding CO pressure. C<SUB>4</SUB> hydrocarbons consist mostly of isobutene at the temperature. From these results it was concluded that isobutene is formed via different path from those of C<SUB>1</SUB>, C<SUB>2</SUB>, C<SUB>3</SUB>, and linear C<SUB>4</SUB> hydrocarbons. The addition of high electronegative oxides such as SiO<SUB>2</SUB> and Nb<SUB>2</SUB>O<SUB>5</SUB> resulted in the decrease of isobutene and the increase of methane. The selective formation of isobutene proceeds over pure ZrO<SUB>2</SUB> and ZrO<SUB>2</SUB> modified with 3a Group and basic metal oxides. The nature of active site for isobutene formation was discussed.
- 公益社団法人 日本化学会の論文
著者
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Maruya Ken-ichi
Research Laboratory Of Resources Utilization Tokyo Institute Of Technology
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Domen Kazunari
Research Laboratory Of Resources Utilization Tokyo Institute Of Technology
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Onishi Takaharu
Research Laboratory of Resources Utilization, Tokyo Institute of Technology
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Haraoka Takashi
Research Laboratory of Resources Utilization, Tokyo Institute of Technology
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Maehashi Tatsuichi
Research Laboratory of Resources Utilization, Tokyo Institute of Technology
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Narui Shinichiro
Research Laboratory of Resources Utilization, Tokyo Institute of Technology
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Asakawa Yukihiko
Research Laboratory of Resources Utilization, Tokyo Institute of Technology
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