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Irreversible catalytic methylcyclohexane dehydrogenation by surface protonics at low temperature

机译：低温下表面质子的不可逆催化甲基环己烷脱氢

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摘要

Liquid organic hydrides are regarded as promising for use as hydrogen carriers via the methylcyclohexane (MCH)-toluene-hydrogen cycle. Because of the endothermic nature of MCH dehydrogenation, the reaction is usually conducted at temperatures higher than 623 K. In this work, low-temperature catalytic MCH dehydrogenation was demonstrated over 3 wt% Pt/CeO2 catalyst by application of electric field across a fixed-bed flow reactor. Results show that a high conversion of MCH beyond thermodynamic equilibrium was achieved even at 423 K. Kinetic analyses exhibited a positive correlation of hydrogen to the reaction rates and an " inverse" kinetic isotope effect (KIE), suggesting that accelerated proton hopping with the H atoms of MCH promotes the reaction. Operando analyses and DFT calculation proved that the reverse reaction (i. e. toluene hydrogenation) was suppressed by the facilitation of toluene desorption in the electric field. The electric field promoted MCH dehydrogenation by surface proton hopping, even at low temperatures with an irreversible pathway.
机译：液体有机氢化物被认为是通过甲基环己烷（MCH） - 氢循环的氢载体的承诺。由于MCH脱氢的吸热性，反应通常在高于623k的温度下进行。在该工作中，通过在固定的情况下施加电场，在3wt％Pt / CeO 2催化剂上证明了低温催化MCH脱氢。床流量反应器。结果表明，即使在423k中，均达到了超出热力学平衡的高转化率。动力学分析表现出氢与反应速率的正相关和“逆”动力学同位素效应（kie），表明加速质子跳跃与h MCH原子促进反应。 Operando分析和DFT计算证明，通过促进电场中的甲苯解吸来抑制反应（即甲苯氢化）。电场通过表面质子跳跃促进MCH脱氢，即使在具有不可逆途径的低温下也是如此。

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  • 来源
    《RSC Advances》 |2019年第11期|共7页
  • 作者

    Takise Kent; Sato Ayaka; Murakami Kota; Ogo Shuhei; Seo Jeong Gil; Imagawa Ken-ichi; Kado Shigeru; Sekine Yasushi;

  • 作者单位

    Waseda Univ Dept Appl Chem Shinjuku Ku 3-4-1 Okubo Tokyo 1698555 Japan;

    Waseda Univ Dept Appl Chem Shinjuku Ku 3-4-1 Okubo Tokyo 1698555 Japan;

    Waseda Univ Dept Appl Chem Shinjuku Ku 3-4-1 Okubo Tokyo 1698555 Japan;

    Waseda Univ Dept Appl Chem Shinjuku Ku 3-4-1 Okubo Tokyo 1698555 Japan;

    Waseda Univ Dept Appl Chem Shinjuku Ku 3-4-1 Okubo Tokyo 1698555 Japan;

    Chiyoda Corp R&

    D Ctr 3-13 Moriya Cho Yokohama Kanagawa 2210022 Japan;

    Chiyoda Corp R&

    D Ctr 3-13 Moriya Cho Yokohama Kanagawa 2210022 Japan;

    Waseda Univ Dept Appl Chem Shinjuku Ku 3-4-1 Okubo Tokyo 1698555 Japan;

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  • 正文语种 eng
  • 中图分类 化学;
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