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<p>Pyrolysis-induced metal aggregation and pore collapse remain critical challenges for Fe–N-C oxygen reduction reaction (ORR) catalysts. This study develops an F127 surfactant-assisted approach to synthesize hierarchical core–shell Fe/N-doped carbon electrocatalysts from iron-modified ZIF-8 precursors. The F127 template performs three key functions: it reduces ZIF-8 particle size from 360 to 200&#xa0;nm, forms protective graphitic carbon shells during pyrolysis, and generates hierarchical mesopores (4 nm, 17.8 nm, and 28&#xa0;nm) through micelle carbonization. This triple action preserves structural integrity, yielding high surface area (946.6 m<sup>2</sup>·g⁻<sup>1</sup>) and pore volume (1.174 cm<sup>3</sup>·g<sup>−2</sup>). Material analysis confirms F127 enhances defect density (<i>I</i><sub>D</sub>/<i>I</i><sub>G</sub> = 1.04) and optimizes nitrogen configuration (72.22% pyridinic/graphitic N), boosting Fe-N<sub>4</sub> site formation while preventing iron migration. The resulting catalyst exhibits exceptional ORR performance in 0.1&#xa0;M KOH: 0.87&#xa0;V half-wave potential, 5.14&#xa0;mA&#xa0;cm<sup>−2</sup> limiting current density, near-ideal 4e<sup>−</sup> transfer (&lt; 2% H<sub>2</sub>O<sub>2</sub> yield), and 97.93% stability retention after 6&#xa0;h, surpassing Pt/C benchmarks. This work establishes a paradigm-shifting strategy for balancing active site density and structural integrity in non-precious metal ORR catalysts through rational surfactant templating.</p>

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F127-mediated synthesis of hierarchical core–shell Fe/N-Doped carbon catalyst for enhanced oxygen reduction reaction

  • 期刊论文

  • 发表日期：

    2025年10月21日

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  • Jianglong Zhou,
  • Yong Tang,
  • Lining Zhang,
  • Hongzhang Yang,
  • Xinfu He,
  • Hongju Wu,
  • Yating Zhang,
  • Anning Zhou

摘要

Pyrolysis-induced metal aggregation and pore collapse remain critical challenges for Fe–N-C oxygen reduction reaction (ORR) catalysts. This study develops an F127 surfactant-assisted approach to synthesize hierarchical core–shell Fe/N-doped carbon electrocatalysts from iron-modified ZIF-8 precursors. The F127 template performs three key functions: it reduces ZIF-8 particle size from 360 to 200 nm, forms protective graphitic carbon shells during pyrolysis, and generates hierarchical mesopores (4 nm, 17.8 nm, and 28 nm) through micelle carbonization. This triple action preserves structural integrity, yielding high surface area (946.6 m2·g⁻1) and pore volume (1.174 cm3·g−2). Material analysis confirms F127 enhances defect density (ID/IG = 1.04) and optimizes nitrogen configuration (72.22% pyridinic/graphitic N), boosting Fe-N4 site formation while preventing iron migration. The resulting catalyst exhibits exceptional ORR performance in 0.1 M KOH: 0.87 V half-wave potential, 5.14 mA cm−2 limiting current density, near-ideal 4e− transfer (< 2% H2O2 yield), and 97.93% stability retention after 6 h, surpassing Pt/C benchmarks. This work establishes a paradigm-shifting strategy for balancing active site density and structural integrity in non-precious metal ORR catalysts through rational surfactant templating.