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Effect of the Nature of the CeO2 Support of the Rh Catalyst on Triggering the Oxidative Reforming of n-Butane for H2 Production from Ambient Temperature

Authors

  • Dr. Katsutoshi Sato,

    1. Elements Strategy Initiative for Catalysts and Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245 (Japan)
    2. Department of Applied Chemistry, Faculty of Engineering, Oita University, 700 Dannoharu, Oita 870-1192 (Japan), Fax: (+81) 97-554-7979
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  • Kouhei Adachi,

    1. Department of Applied Chemistry, Faculty of Engineering, Oita University, 700 Dannoharu, Oita 870-1192 (Japan), Fax: (+81) 97-554-7979
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  • Prof. Dr. Yusaku Takita,

    1. Department of Applied Chemistry, Faculty of Engineering, Oita University, 700 Dannoharu, Oita 870-1192 (Japan), Fax: (+81) 97-554-7979
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  • Dr. Katsutoshi Nagaoka

    Corresponding author
    1. Elements Strategy Initiative for Catalysts and Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245 (Japan)
    2. Department of Applied Chemistry, Faculty of Engineering, Oita University, 700 Dannoharu, Oita 870-1192 (Japan), Fax: (+81) 97-554-7979
    3. Core Research for Evolutional Science and Technology (CREST), Japan Science and Technology Agency (JST), 7 Gobancho, Chiyoda-ku, Tokyo 102-0076 (Japan)
    • Elements Strategy Initiative for Catalysts and Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245 (Japan)

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Abstract

Three Rh catalysts supported on CeO2 with different specific surface areas and redox properties were prepared and evaluated for their ability to trigger the oxidative reforming of n-butane from ambient temperature (≈300 K). The reference CeO2 catalysts supplied by the Catalyst Society of Japan (JRC-CEO-1, -3, and -4) were used as supports. Temperature-programmed reduction and O2 titration measurements over the reduced catalysts indicated that a high number of surface CeO2 sites that were reducible below 573 K were present on the Rh/CEO-3 catalyst; this catalyst had the largest specific surface area, and it generated sufficient heat by oxidizing CeO2−xH(298 K)=−368 kJ; x=0.5] after H2 reduction at 773 K. Furthermore, the temperature-programmed reactions revealed that forming fine Rh particles on the high surface area of CEO-3 lowers the autoignition temperature (498 K) of the oxidative reforming of n-butane because the number of exposed Rh sites initiating reactions between n-butane and O2 is large. Thus, the Rh/CEO-3 catalyst could trigger the oxidative reforming of n-butane at ambient temperature after H2 reduction at 773 K owing to the heat generated by the spontaneous oxidation of CeO2−x. In contrast, other catalysts could not trigger the reaction after reduction at the same temperature.

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