Abstract <p>This study compares Pd/Al<sub>2</sub>O<sub>3</sub> and Pd<sub>1</sub>Ag<sub>5</sub>/Al<sub>2</sub>O<sub>3</sub> catalysts for the front-end selective hydrogenation of acetylene, with a focus on how their catalytic performance correlates with the H<sub>2</sub> : C<sub>2</sub>H<sub>2</sub> ratio and CO concentration. A combination of physicochemical characterization methods demonstrated that single-atom Pd<sub>1</sub> sites isolated from one another by Ag atoms were formed on the surface of the bimetallic sample. The acetylene hydrogenation rate increased with the H<sub>2</sub>:C<sub>2</sub>H<sub>2</sub> ratio, a correlation that was more pronounced for Pd/Al<sub>2</sub>O<sub>3</sub> than for Pd<sub>1</sub>Ag<sub>5</sub>/Al<sub>2</sub>O<sub>3</sub>. This was quantified by the apparent reaction order with respect to hydrogen (<i>n</i>(H<sub>2</sub>)), which was 1.5 and 1.0, respectively. While increasing the H<sub>2</sub> : C<sub>2</sub>H<sub>2</sub> ratio had a significant adverse impact on selectivity toward the target product, this was effectively counteracted by the addition of CO to the reaction mixture. Furthermore, promoting the Pd/Al<sub>2</sub>O<sub>3</sub> catalyst with Ag eliminated any thermal runaway effect and facilitated precise temperature control.</p>

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Effects of H2 and CO Concentrations on the Performance of PdAg/Al2O3 Catalysts in Selective Hydrogenation of Acetylene

  • I. S. Mashkovsky,
  • P. V. Markov,
  • K. Sh. Yakubov,
  • A. E. Vaulina,
  • G. N. Baeva,
  • N. S. Smirnova,
  • A. R. Kolyadenkov,
  • A. V. Kazakov,
  • A. Yu. Stakheev

摘要

Abstract

This study compares Pd/Al2O3 and Pd1Ag5/Al2O3 catalysts for the front-end selective hydrogenation of acetylene, with a focus on how their catalytic performance correlates with the H2 : C2H2 ratio and CO concentration. A combination of physicochemical characterization methods demonstrated that single-atom Pd1 sites isolated from one another by Ag atoms were formed on the surface of the bimetallic sample. The acetylene hydrogenation rate increased with the H2:C2H2 ratio, a correlation that was more pronounced for Pd/Al2O3 than for Pd1Ag5/Al2O3. This was quantified by the apparent reaction order with respect to hydrogen (n(H2)), which was 1.5 and 1.0, respectively. While increasing the H2 : C2H2 ratio had a significant adverse impact on selectivity toward the target product, this was effectively counteracted by the addition of CO to the reaction mixture. Furthermore, promoting the Pd/Al2O3 catalyst with Ag eliminated any thermal runaway effect and facilitated precise temperature control.