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<p>Synergistic effect between M-N<sub>X</sub> sites and M<sub>X</sub>O<sub>Y</sub> particles in hierarchical porous M–N-C catalysts holds great promises in boosting oxygen reduction reaction (ORR). In this work, 1,4-dicyanobenzene was utilized as a molecular template to prepare the hierarchical porous Fe–N-C catalysts with size-tunable Fe<sub>3</sub>O<sub>4</sub> particles for enhanced ORR in Zn-air battery. The as-prepared Fe<sub>3</sub>O<sub>4</sub>#Fe–N/C<sub>DB0.1</sub> owned a half-potential of 0.90&#xa0;V vs RHE, exceeding that of commercial 20%Pt/C (E<sub>1/2</sub> = 0.82&#xa0;V vs RHE), showing a maximum power density of 321 mW cm<sup>−2</sup> in a homemade Zn-air battery. Density functional theory (DFT) calculations indicate that the electronic interaction between Fe<sub>3</sub>O<sub>4</sub> and Fe-N<sub>4</sub> sites enhances the adsorption energy of *OOH, effectively optimizing the energy barrier for *O formation, significantly reducing the limiting energy barrier. Such superior ORR activity in Fe<sub>3</sub>O<sub>4</sub>#Fe–N/C originated from the optimized hierarchical pores and synergistic effect between Fe-N<sub>X</sub> sites and Fe<sub>3</sub>O<sub>4</sub> particles. This work provides a new and facile template strategy for engineering hierarchical porous carbon-based materials to achieve highly efficient catalytic reactions.</p>

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Molecular template engineering hierarchical porous Fe–N-C with tunable Fe3O4 particle size for efficient oxygen reduction reaction

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月12日

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  • Lijuan Wang,
  • Yaqin Shi,
  • Yuan Wang,
  • Chunijang Jia,
  • Jie Hou,
  • Yizhen Su,
  • Ben Bin Xu,
  • Zhijian Liao,
  • Linhua Zhu

摘要

Synergistic effect between M-NX sites and MXOY particles in hierarchical porous M–N-C catalysts holds great promises in boosting oxygen reduction reaction (ORR). In this work, 1,4-dicyanobenzene was utilized as a molecular template to prepare the hierarchical porous Fe–N-C catalysts with size-tunable Fe3O4 particles for enhanced ORR in Zn-air battery. The as-prepared Fe3O4#Fe–N/CDB0.1 owned a half-potential of 0.90 V vs RHE, exceeding that of commercial 20%Pt/C (E1/2 = 0.82 V vs RHE), showing a maximum power density of 321 mW cm−2 in a homemade Zn-air battery. Density functional theory (DFT) calculations indicate that the electronic interaction between Fe3O4 and Fe-N4 sites enhances the adsorption energy of *OOH, effectively optimizing the energy barrier for *O formation, significantly reducing the limiting energy barrier. Such superior ORR activity in Fe3O4#Fe–N/C originated from the optimized hierarchical pores and synergistic effect between Fe-NX sites and Fe3O4 particles. This work provides a new and facile template strategy for engineering hierarchical porous carbon-based materials to achieve highly efficient catalytic reactions.