4.8 Article

Si Doping Enables Activity and Stability Enhancement on Atomically Dispersed Fe-Nx/C Electrocatalysts for Oxygen Reduction in Acid

Journal

CHEMSUSCHEM
Volume -, Issue -, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202201795

Keywords

electrocatalysis; heterogeneous catalysis; oxygen reduction reaction; Si doping; stability

Funding

  1. National Nature Science Foundation of China [22122202, 21972051]
  2. Guangdong Basic and Applied Basic Research Foundation [2022A1515011347]

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In this work, silicon-doped iron-nitrogen-carbon catalysts were developed using in situ silicon doping and metal-polymer coordination. The results showed that silicon doping not only increased the density of Fe-N-x/C active sites, but also elevated the content of graphitic carbon, leading to a Si/Fe-N-C catalyst with improved activity and stability in acidic media.
Fe-N-C represents the most promising non-precious metal catalysts (NPMCs) for the oxygen reduction reaction (ORR) in fuel cells, but often suffers from poor stability in acid due to the dissolution of metal sites and the poor oxidation resistance of carbon substrates. In this work, silicon-doped iron-nitrogen-carbon (Si/Fe-N-C) catalysts were developed by in situ silicon doping and metal-polymer coordination. It was found that Si doping could not only promote the density of Fe-N-x/C active sites but also elevated the content of graphitic carbon through catalytic graphitization. The best-performing Si/Fe-N-C exhibited a half-wave potential of 0.817 V vs. reversible hydrogen electrode in 0.5 m H2SO4, outperforming that of undoped Fe-N-C and most of the reported Fe-N-C catalysts. It also exhibited significantly enhanced stability at elevated temperature (>= 60 degrees C). This work provides a new way to develop non-precious metal ORR catalysts with improved activity and stability in acidic media.

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