Synthesis and characterization of precursor derived TiN@Si–Al–C–N ceramic nanocomposites for oxygen reduction reaction

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Eranezhuth Wasan, Awin ; Günther, Timon E. ; Loukrakpam, Rameshwori ; Schafföner, Stefan ; Roth, Christina ; Motz, Günter:
Synthesis and characterization of precursor derived TiN@Si–Al–C–N ceramic nanocomposites for oxygen reduction reaction.
In: International Journal of Applied Ceramic Technology. Bd. 20 (2023) Heft 1 . - S. 59-69.
ISSN 1744-7402
DOI: https://doi.org/10.1111/ijac.14234

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Abstract

Abstract The development of efficient and durable catalysts is critical for the commercialization of fuel cells, as the catalysts’ durability and reactivity dictate their ultimate lifetime and activity. In this work, amorphous silicon-based ceramics (Si–C–N and Si–Al–C–N) and TiN@Si–Al–C–N nanocomposites were developed using a precursor derived ceramics approach. In TiN@Si–Al–C–N nanocomposites, TiN nanocrystals (with sizes in the range of 5–12 nm) were effectively anchored on an amorphous Si–Al–C–N support. The nanocomposites were found to be mesoporous in nature and exhibited a surface area as high as 132 m2/g. The average pore size of the nanocomposites was found to increase with an increase in the pyrolysis temperature, and a subsequent graphitization of free carbon was observed as revealed from the Raman spectra. The ceramics were investigated for electrocatalytic activity toward the oxygen reduction reaction using the rotating disk electrode method. The TiN@Si–Al–C–N nanocomposites showed an onset potential of 0.7 V versus reversible hydrogen electrode for oxygen reduction, which seems to indicate a 4-electron pathway at the pyrolysis temperature of 1000°C in contrast to a 2-electron pathway exhibited by the nanocomposites pyrolyzed at 750°C via the Koutecky–Levich plot.