Metal-nitrogen-carbon oxygen reduction catalysts by high pressure pyrolysis using ammonia-generating precursors

Vijayadurga Nallathambi, Nathaniel Leonard, Scott Calabrese Barton

    Research output: Chapter in Book/Report/Conference proceedingConference contribution

    Abstract

    High surface area Metal-nitrogen-carbon (MNC) cathode catalysts for oxygen reduction in low temperature fuel cells were synthesized by pyrolysis of iron-acetate, ketjen black and nitrogen precursors in a closed, constant volume reaction vessel. Autogenic pressure generated by nitrogen precursor evaporation and decomposition during pyrolysis leads to nitrogen intermediates with high activity and mobility, contributing to increased nitrogen retention and activity. N Precursors such as ammonium hydroxide, urea and ammonium carbamate were studied, because they produce an ammonia gas intermediate that can etch non-graphitic carbon, increasing mesoporous surface area and accessible active site density. The most active catalysts were obtained in this work using ammonium carbamate, and kinetic current density as high as 15 A cm-3 at 0.8 ViR-free and over 100 h of stable current at 0.5 V were observed in single fuel cell measurements.

    Original languageEnglish (US)
    Title of host publicationACS National Meeting Book of Abstracts
    StatePublished - 2011
    Event241st ACS National Meeting and Exposition - Anaheim, CA, United States

    Other

    Other241st ACS National Meeting and Exposition
    CountryUnited States
    CityAnaheim, CA
    Period3/27/113/31/11

    Profile

    Nitrogen
    Pyrolysis
    Catalysts
    Carbon
    Afferent Loop Syndrome
    Fuel cells
    Ammonia
    Oxygen
    Metals
    Edema Disease of Swine
    Biogenic Amines
    Ammonium hydroxide
    Urea
    Evaporation
    Cathodes
    Current density
    Iron
    Decomposition
    Kinetics
    Gases

    ASJC Scopus subject areas

    • Chemistry(all)
    • Chemical Engineering(all)

    Cite this

    Metal-nitrogen-carbon oxygen reduction catalysts by high pressure pyrolysis using ammonia-generating precursors. / Nallathambi, Vijayadurga; Leonard, Nathaniel; Barton, Scott Calabrese.

    ACS National Meeting Book of Abstracts. 2011.

    Research output: Chapter in Book/Report/Conference proceedingConference contribution

    Nallathambi, V, Leonard, N & Barton, SC 2011, Metal-nitrogen-carbon oxygen reduction catalysts by high pressure pyrolysis using ammonia-generating precursors. in ACS National Meeting Book of Abstracts. 241st ACS National Meeting and Exposition, Anaheim, CA, United States, 27-31 March.

    Nallathambi, Vijayadurga; Leonard, Nathaniel; Barton, Scott Calabrese / Metal-nitrogen-carbon oxygen reduction catalysts by high pressure pyrolysis using ammonia-generating precursors.

    ACS National Meeting Book of Abstracts. 2011.

    Research output: Chapter in Book/Report/Conference proceedingConference contribution

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    AB - High surface area Metal-nitrogen-carbon (MNC) cathode catalysts for oxygen reduction in low temperature fuel cells were synthesized by pyrolysis of iron-acetate, ketjen black and nitrogen precursors in a closed, constant volume reaction vessel. Autogenic pressure generated by nitrogen precursor evaporation and decomposition during pyrolysis leads to nitrogen intermediates with high activity and mobility, contributing to increased nitrogen retention and activity. N Precursors such as ammonium hydroxide, urea and ammonium carbamate were studied, because they produce an ammonia gas intermediate that can etch non-graphitic carbon, increasing mesoporous surface area and accessible active site density. The most active catalysts were obtained in this work using ammonium carbamate, and kinetic current density as high as 15 A cm-3 at 0.8 ViR-free and over 100 h of stable current at 0.5 V were observed in single fuel cell measurements.

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