Hypervelocity kinetics blocks harmful intermediates to enhance stability of Fe-N-C catalysts
摘要
Hydrogen peroxide that is produced through the two-electron pathway during the catalysis of oxygen reduction reaction (ORR) is recognized as harmful to the stability of nitrogen-doped carbon and Fe-based nonprecious catalyst (Fe-N-C) for fuel cell application. A major remaining scientific question is how fast the removal of these deleterious intermediates can contribute to stability enhancement. Here, we report that the stability of Fe-N-C catalysts is positively correlated with the kinetic constant of hydrogen peroxide decomposition. Modulation of the H2O2 decomposition kinetics by applying the frequency factor of the Arrhenius equation from 800 to 30000 s−1 for TiO2, CeO2 and ZrO2 reduced the decay rate of Fe-N-C catalysts from 0.151% to −0.1% in a 100-hour stability test. Fe-N-C/ZrO2 with a frequency factor of 30000 s−1 showed a 10% increase in current density during a 100-hour stability test and almost no decay during 15 hours of continuous fuel cell operation at a high potential of 0.7 V.