<p><sup>57</sup>Fe–N–C electrocatalysts were synthesized via ultrasonic treatment and electron beam (e-beam) irradiation, enabling rapid nanoparticle formation under mild conditions. Mössbauer spectroscopy was used to analyze the oxidation and spin states of Fe–N<sub>4</sub> species. The <sup>57</sup>Fe-labeled samples prepared using e-beam irradiation exhibited three Fe(II)–N<sub>4</sub> configurations: low-spin (D1), medium-spin (D2), and high-spin (D3), observed at 4.2&#xa0;K. A higher proportion of low-spin Fe(II)–N<sub>4</sub> sites strongly correlated with improved oxygen reduction reaction (ORR) activity. Notably, e-beam irradiation promoted the selective formation of these catalytically active low-spin sites, offering a scalable and efficient synthesis strategy.</p>

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Enhanced oxygen reduction catalysis in electron beam derived 57Fe–N–C: impact of precursor coordination and iron speciation

  • Young Rang Uhm,
  • Hyunkyung Choi,
  • Chul Sung Kim,
  • Sung Baek Kim

摘要

57Fe–N–C electrocatalysts were synthesized via ultrasonic treatment and electron beam (e-beam) irradiation, enabling rapid nanoparticle formation under mild conditions. Mössbauer spectroscopy was used to analyze the oxidation and spin states of Fe–N4 species. The 57Fe-labeled samples prepared using e-beam irradiation exhibited three Fe(II)–N4 configurations: low-spin (D1), medium-spin (D2), and high-spin (D3), observed at 4.2 K. A higher proportion of low-spin Fe(II)–N4 sites strongly correlated with improved oxygen reduction reaction (ORR) activity. Notably, e-beam irradiation promoted the selective formation of these catalytically active low-spin sites, offering a scalable and efficient synthesis strategy.