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Defect-Engineered Continuous 3D Single-Atom Catalysts for Enhanced Oxygen Reduction Performance.

Zhihao Chen1, Shu Wang1, Feng Du1

  • 1Institute of Advanced Materials and School of Chemistry and Chemical Engineering, Southeast University, Nanjing, 211189, China.

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|August 16, 2025
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Summary
This summary is machine-generated.

Defect engineering in iron-nitrogen-carbon structures (Fe─N4O) enhances single-atom catalysts for the oxygen reduction reaction (ORR). This approach boosts catalytic activity and stability for energy applications.

Keywords:
3D carbon foamdefect engineeringelectrochemistryoxygen reduction reactionsingle atom catalyst

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Metal atom mobility on carbon substrates causes aggregation, hindering single-atom catalyst performance.
  • Nitrogen coordination (Nx) anchors single metal atoms, preventing aggregation and forming active sites like Fe─N4-C.
  • Strong oxygen intermediate adsorption on Fe sites limits the intrinsic activity of Fe─N4-C catalysts.

Purpose of the Study:

  • To develop a novel strategy for stabilizing nitrogen-coordinated iron single atoms (Fe─N4) to enhance oxygen reduction reaction (ORR) catalytic activity.
  • To engineer defects in Fe─N4 structures to create Fe SAs/NPGN catalysts with improved performance.
  • To investigate the role of defect-synergistic structures in tuning the electronic properties of Fe sites for efficient ORR.

Main Methods:

  • Synthesis of defect-engineered Fe─N4O configuration (Fe SAs/NPGN) via ammonia-thermal etching.
  • Characterization of the catalyst's structure, surface area (2054.39 m2 g-1), and active sites.
  • Validation of catalytic performance and electronic property tuning through experimental results and theoretical calculations.

Main Results:

  • The synthesized Fe SAs/NPGN catalyst exhibits significantly boosted ORR catalytic performance.
  • The defect-engineered structure provides abundant active sites and a high specific surface area.
  • Tuned electronic properties of Fe sites facilitate more efficient ORR activity, confirmed by experiments and theory.

Conclusions:

  • Defect engineering of Fe─N4 sites creates highly active and stable single-atom catalysts for ORR.
  • The Fe SAs/NPGN catalyst demonstrates a promising pathway for advancing defect-engineered catalysts in energy applications.
  • This strategy effectively overcomes the limitations of strong oxygen intermediate adsorption in traditional Fe─N4-C catalysts.