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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Single-atom catalysts (SACs) offer high atom utilization efficiency.
  • Optimizing the Fe-N_x microenvironment is crucial for oxygen reduction reaction (ORR) activity.
  • Developing non-precious metal catalysts for energy applications is a key research area.

Purpose of the Study:

  • To synthesize and characterize Fe-N5 single-atom catalysts with a unique porous architecture.
  • To investigate the synergistic effects of Fe coordination, heteroatom doping, and pore structure on ORR performance.
  • To evaluate the catalytic activity of the developed Fe-N5 SACs in zinc-air batteries.

Main Methods:

  • A dual-confinement strategy involving wood framework and Fe3+ coordination was employed.
  • Cellulose nanocrystals (CNCs) self-assembled into a porous architecture, followed by pyrolysis.
  • X-ray absorption spectroscopy (XAS) and density functional theory (DFT) calculations were used for characterization and mechanistic studies.

Main Results:

  • Fe-N5 single-atom catalysts were successfully anchored on N, S-codoped carbon with hierarchical pores.
  • Synergistic effects from Fe-N5 coordination, S doping, and micropores optimized the catalyst's electronic structure.
  • The catalysts exhibited excellent ORR activity with a half-wave potential of 0.964 V, surpassing Pt/C in zinc-air batteries.

Conclusions:

  • The dual-confinement strategy effectively creates optimized Fe-N5 active sites within a porous carbon matrix.
  • The developed Fe-N5 SACs demonstrate high potential as efficient and cost-effective electrocatalysts for metal-air batteries.
  • This approach provides a pathway for designing advanced non-precious metal catalysts.