Role of alkali metal in a highly active Pd/alkali/Fe2O 3 catalyst for water gas shift reaction

Ryo Watanabe, Yuji Sakamoto, Keisuke Yamamuro, Sakurako Tamura, Eiichi Kikuchi, Yasushi Sekine

    Research output: Contribution to journalArticle

    16 Citations (Scopus)

    Abstract

    Pd/K/Fe2O3 catalyst shows high activity for water gas shift (WGS) reaction. The K/Pd molar ratio on the catalyst has a remarkable effect on WGS activity. The optimum K/Pd molar ratio is about 2. In this study, to clarify the role of alkali metal (potassium), WGS activities of Pd/alkali/Fe2O3 (alkali: Li, Na, K or Cs) catalysts were investigated and the reaction mechanism over the Pd/K/Fe2O 3 catalyst was examined with transient response analyses using a concentration jump method with a quadrupole mass spectrometer (Q-Mass). Results showed that the addition of alkali metals such as Na, K and Cs drastically enhanced WGS activity, except for Li-loaded catalyst. WGS reaction over the highly active Pd/K/Fe2O3 catalyst was found to proceed via reduction-oxidation (redox) using lattice oxygen. Thereby, CO was oxidized by lattice oxygen in Fe2O3. The consumed lattice oxygen was regenerated by H2O. The results of CO-TPR revealed that oxidation of CO by lattice oxygen were enhanced by K, Cs or Na addition. H2-TPR results showed that reduction of Fe2O3 was suppressed by an increment of loading amount of potassium, which brought a high stability for the WGS reaction. The result of CO/H2O-TPR showed that steam can promote the regeneration of consumed lattice oxygen. The synergistic effect brought a high release ability of lattice oxygen for CO oxidation and also high regenerating ability of consumed lattice oxygen by H2O to produce hydrogen, to the Pd/K/Fe2O3 catalyst. It enabled high catalytic performance of the Pd/K/Fe2O3 catalyst with K/Pd molar ratio of 2.

    Original languageEnglish
    Pages (from-to)1-11
    Number of pages11
    JournalApplied Catalysis A: General
    Volume457
    DOIs
    Publication statusPublished - 2013 Apr 24

    Fingerprint

    Alkali Metals
    Water gas shift
    Alkalies
    Alkali metals
    Carbon Monoxide
    Catalysts
    Oxygen
    Oxidation
    Potassium
    Steam
    Mass spectrometers
    Transient analysis
    Hydrogen
    Thermodynamic properties

    Keywords

    • Alkali metal addition
    • Hydrogen production
    • Lattice oxygen
    • Redox
    • Water gas shift

    ASJC Scopus subject areas

    • Catalysis
    • Process Chemistry and Technology

    Cite this

    Role of alkali metal in a highly active Pd/alkali/Fe2O 3 catalyst for water gas shift reaction. / Watanabe, Ryo; Sakamoto, Yuji; Yamamuro, Keisuke; Tamura, Sakurako; Kikuchi, Eiichi; Sekine, Yasushi.

    In: Applied Catalysis A: General, Vol. 457, 24.04.2013, p. 1-11.

    Research output: Contribution to journalArticle

    Watanabe, Ryo ; Sakamoto, Yuji ; Yamamuro, Keisuke ; Tamura, Sakurako ; Kikuchi, Eiichi ; Sekine, Yasushi. / Role of alkali metal in a highly active Pd/alkali/Fe2O 3 catalyst for water gas shift reaction. In: Applied Catalysis A: General. 2013 ; Vol. 457. pp. 1-11.
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    AU - Watanabe, Ryo

    AU - Sakamoto, Yuji

    AU - Yamamuro, Keisuke

    AU - Tamura, Sakurako

    AU - Kikuchi, Eiichi

    AU - Sekine, Yasushi

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    AB - Pd/K/Fe2O3 catalyst shows high activity for water gas shift (WGS) reaction. The K/Pd molar ratio on the catalyst has a remarkable effect on WGS activity. The optimum K/Pd molar ratio is about 2. In this study, to clarify the role of alkali metal (potassium), WGS activities of Pd/alkali/Fe2O3 (alkali: Li, Na, K or Cs) catalysts were investigated and the reaction mechanism over the Pd/K/Fe2O 3 catalyst was examined with transient response analyses using a concentration jump method with a quadrupole mass spectrometer (Q-Mass). Results showed that the addition of alkali metals such as Na, K and Cs drastically enhanced WGS activity, except for Li-loaded catalyst. WGS reaction over the highly active Pd/K/Fe2O3 catalyst was found to proceed via reduction-oxidation (redox) using lattice oxygen. Thereby, CO was oxidized by lattice oxygen in Fe2O3. The consumed lattice oxygen was regenerated by H2O. The results of CO-TPR revealed that oxidation of CO by lattice oxygen were enhanced by K, Cs or Na addition. H2-TPR results showed that reduction of Fe2O3 was suppressed by an increment of loading amount of potassium, which brought a high stability for the WGS reaction. The result of CO/H2O-TPR showed that steam can promote the regeneration of consumed lattice oxygen. The synergistic effect brought a high release ability of lattice oxygen for CO oxidation and also high regenerating ability of consumed lattice oxygen by H2O to produce hydrogen, to the Pd/K/Fe2O3 catalyst. It enabled high catalytic performance of the Pd/K/Fe2O3 catalyst with K/Pd molar ratio of 2.

    KW - Alkali metal addition

    KW - Hydrogen production

    KW - Lattice oxygen

    KW - Redox

    KW - Water gas shift

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