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<p>The practical applications of high-performance metal-air batteries are limited by the slow dynamics of the oxygen reduction reaction (ORR). In this work, we demonstrate a convenient method of one-step pyrolysis to synthesize a novel Fe-N-C embedded 1D carbon nanotube/2D graphene (Fe-NCNTs@Gr-N) as the electrocatalyst for enhanced ORR performances. The controlled stage temperature calcination method and <i>ex-situ</i> characterizations techniques were used to investigate the growth mechanism of 1D/2D hierarchical catalyst, with the results revealing that the formation of Fe3C is the key to constructing 1D carbon nanotubes and 2D graphene during the pyrolysis process. Owing to the advantages of good electronic transfer capability and confinement microenvironment, Fe-NCNTs@Gr-N exhibits the outstanding ORR activity [onset potential of 1.04 V <i>vs.</i> reversible hydrogen electrode (RHE), half-wave potential of 0.82 V <i>vs.</i> RHE] and catalytic stability (over 20000 cycles CVs stable). For Fe-NCNTs@Gr-N based Zn-air, Al-air, and Mg-air batteries, they also achieve the exceptional performance, surpassing the Pt/C based cells. This work paves the way for the rational design of transition metal-based electrocatalysts for highly efficient, stable ORR processes and has significant implications for the development of next-generation metal-air batteries.</p>

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Controlled Synthesis of Fe-N-C Embedded 1D Carbon Nanotube/2D Graphene for Enhanced Oxygen Reduction in Metal-Air Batteries

  • 期刊论文

  • 发表日期：

    2025年9月3日

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  • Jingzhi He,
  • Mengfan Xu,
  • Zixuan Zhang,
  • Jingqi Guan,
  • Limei Duan,
  • Yin Wang

摘要

The practical applications of high-performance metal-air batteries are limited by the slow dynamics of the oxygen reduction reaction (ORR). In this work, we demonstrate a convenient method of one-step pyrolysis to synthesize a novel Fe-N-C embedded 1D carbon nanotube/2D graphene (Fe-NCNTs@Gr-N) as the electrocatalyst for enhanced ORR performances. The controlled stage temperature calcination method and ex-situ characterizations techniques were used to investigate the growth mechanism of 1D/2D hierarchical catalyst, with the results revealing that the formation of Fe3C is the key to constructing 1D carbon nanotubes and 2D graphene during the pyrolysis process. Owing to the advantages of good electronic transfer capability and confinement microenvironment, Fe-NCNTs@Gr-N exhibits the outstanding ORR activity [onset potential of 1.04 V vs. reversible hydrogen electrode (RHE), half-wave potential of 0.82 V vs. RHE] and catalytic stability (over 20000 cycles CVs stable). For Fe-NCNTs@Gr-N based Zn-air, Al-air, and Mg-air batteries, they also achieve the exceptional performance, surpassing the Pt/C based cells. This work paves the way for the rational design of transition metal-based electrocatalysts for highly efficient, stable ORR processes and has significant implications for the development of next-generation metal-air batteries.