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Origin of temperature oscillations of nickel catalyst occurring in methane oxidation

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Abstract

The catalytic oxidation of methane over a nickel foil has been investigated in a wide range of methane: oxygen molar ratios at a constant reactor temperature of 680°C. Under oxygen-deficient conditions, the reaction takes place in the self-oscillating mode. Stable self-sustained oscillations of the methane oxidation rate are observed in the CH4: O2 molar ratio range from 2: 1 to 19: 1. This process is accompanied by catalyst temperature oscillations, whose amplitude reaches 80°C. It has been demonstrated by scanning electron microscopy that the origination of the self-sustained oscillations is accompanied by morphological changes in the catalyst surface. Under the action of the reaction medium, a porous layer 5–10 µm in thickness forms on the nickel foil surface. The mechanism of methane oxidation over nickel that accounts for the onset of the self-sustained oscillations is discussed. This mechanism is based on periodical nickel oxidation and reduction. When nickel is in the high-activity state, it is mainly in metallic form, and the passage of nickel into its low-activity state is accompanied by the formation of a nickel oxide layer on the foil surface. The reduction of this nickel oxide causes a periodic decrease in the catalyst temperature. The total and partial oxidations of methane on the reduced surface of the nickel foil raise the catalyst temperature. Under oxygen-deficient conditions, a carbon deposit builds up on the catalyst surface, and the combustion of this deposit complicates the catalyst temperature oscillation profile.

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Authors and Affiliations

  1. Boreskov Institute of Catalysis, Siberian Branch, Russian Academy of Sciences, Novosibirsk, 630090, Russia

    A. A. Saraev, V. V. Kaichev & V. I. Bukhtiyarov

  2. Novosibirsk State University, Novosibirsk, 630090, Russia

    A. A. Saraev, S. S. Kosolobov, V. V. Kaichev & V. I. Bukhtiyarov

  3. Rzhanov Institute of Semiconductor Physics, Siberian Branch, Russian Academy of Sciences, Novosibirsk, 630090, Russia

    S. S. Kosolobov

Authors
  1. A. A. Saraev
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  2. S. S. Kosolobov
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  3. V. V. Kaichev
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  4. V. I. Bukhtiyarov
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Corresponding author

Correspondence to V. V. Kaichev.

Additional information

Original Russian Text © A.A. Saraev, S.S. Kosolobov, V.V. Kaichev, V.I. Bukhtiyarov, 2015, published in Kinetika i Kataliz, 2015, Vol. 56, No. 5, pp. 606–613.

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Saraev, A.A., Kosolobov, S.S., Kaichev, V.V. et al. Origin of temperature oscillations of nickel catalyst occurring in methane oxidation. Kinet Catal 56, 598–604 (2015). https://doi.org/10.1134/S002315841505016X

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  • DOI: https://doi.org/10.1134/S002315841505016X

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