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<p>Fabricating inexpensive non-precious metal materials with exceptional electrocatalytic activity toward oxygen reduction represents a pivotal step in upgrading the performance of modern electrochemical energy systems. This work presents a facile strategy for synthesizing an efficient Fe-N-C ORR catalyst (denoted as Phenanthroline-Fe/NC-40) by pyrolyzing an iron-doped zeolitic imidazolate framework leaf (ZIF-L) precursor, where 1,10-phenanthroline serves as a critical nitrogen source and coordination modulator. The innovative use of this ligand optimally regulates the distribution of metal elements during synthesis, facilitating the formation of highly dispersed Fe−N<sub>4</sub> active sites within a hierarchically porous nitrogen-doped carbon matrix. The obtained catalyst exhibits outstanding ORR activity in 0.1&#xa0;M KOH, with a high half-wave potential (<i>E</i><sub>1/2</sub>) of 0.883&#xa0;V vs. RHE, a dominant four-electron transfer pathway (<i>n</i> = 3.97), and a low Tafel slope of 84.49&#xa0;mV dec<sup>−1</sup>, rivaling the performance of commercial Pt/C. More importantly, Phenanthroline-Fe/NC-40 demonstrates superior stability, showing a minimal negative shift of only 16&#xa0;mV in <i>E</i><sub>1/2</sub> after 2500 accelerated durability test cycles and retaining 83.81% of its initial current after 10 h, significantly outperforming Pt/C. This enhanced performance is attributed to the synergistic effects of the abundant Fe−N<sub>4</sub> sites, mass transport for favorable porous structure, and stable integration of iron species. This study provides a valuable precursor-engineering strategy to guide the strategic engineering of robust and highly efficient earth-abundant catalytic materials for sustainable energy applications.</p>

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Ligand-mediated synthesis of ZIF-L derived Fe-N-C catalysts with superior ORR activity and stability

  • 期刊论文

  • 发表日期：

    2026年6月22日

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  • Xian Li,
  • Luyifan Li,
  • Heng Guo,
  • Wenpeng Luo,
  • Yangbo Huang,
  • Hongyu Yang

摘要

Fabricating inexpensive non-precious metal materials with exceptional electrocatalytic activity toward oxygen reduction represents a pivotal step in upgrading the performance of modern electrochemical energy systems. This work presents a facile strategy for synthesizing an efficient Fe-N-C ORR catalyst (denoted as Phenanthroline-Fe/NC-40) by pyrolyzing an iron-doped zeolitic imidazolate framework leaf (ZIF-L) precursor, where 1,10-phenanthroline serves as a critical nitrogen source and coordination modulator. The innovative use of this ligand optimally regulates the distribution of metal elements during synthesis, facilitating the formation of highly dispersed Fe−N4 active sites within a hierarchically porous nitrogen-doped carbon matrix. The obtained catalyst exhibits outstanding ORR activity in 0.1 M KOH, with a high half-wave potential (E1/2) of 0.883 V vs. RHE, a dominant four-electron transfer pathway (n = 3.97), and a low Tafel slope of 84.49 mV dec−1, rivaling the performance of commercial Pt/C. More importantly, Phenanthroline-Fe/NC-40 demonstrates superior stability, showing a minimal negative shift of only 16 mV in E1/2 after 2500 accelerated durability test cycles and retaining 83.81% of its initial current after 10 h, significantly outperforming Pt/C. This enhanced performance is attributed to the synergistic effects of the abundant Fe−N4 sites, mass transport for favorable porous structure, and stable integration of iron species. This study provides a valuable precursor-engineering strategy to guide the strategic engineering of robust and highly efficient earth-abundant catalytic materials for sustainable energy applications.