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FeNC Oxygen Reduction Electrocatalyst with High Utilization Penta-Coordinated Sites.

Jesús Barrio1,2, Angus Pedersen1,2, Saurav Ch Sarma2

  • 1Department of Materials, Royal School of Mines, Imperial College London, London, SW7 2AZ, UK.

Advanced Materials (Deerfield Beach, Fla.)
|February 5, 2023
PubMed
Summary

This study introduces a novel synthesis for highly porous iron-nitrogen-carbon electrocatalysts, significantly boosting iron utilization for oxygen reduction reactions in fuel cells. The new method enhances catalyst performance and stability, offering a promising alternative to platinum-based catalysts.

Keywords:
FeNC materialscarbon materialselectrocatalysisoxygen reduction reactionsingle atom catalysts

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Atomic iron in nitrogen-doped carbon (FeNC) electrocatalysts are promising alternatives to platinum for oxygen reduction in fuel cells.
  • Controlled synthesis and stability of FeNC catalysts for practical applications remain challenging.
  • Low iron utilization in current FeNC catalysts is due to insufficient porosity and poor exposure of active sites.

Purpose of the Study:

  • To develop a highly porous nitrogen-doped carbon support for improved iron coordination and electrochemical active site density.
  • To enhance the utilization and stability of atomic FeNC electrocatalysts for oxygen reduction reactions.
  • To investigate the structure and coordination of iron single atoms in the developed catalyst.

Main Methods:

  • A two-step synthesis involving pyrolysis of 2,4,6-triaminopyrimidine with a Mg2+ salt template to create a porous carbon support.
  • Coordination of iron within the porous support to form FeNC electrocatalysts.
  • Characterization using aberration-corrected HAADF-STEM, in situ nitrite stripping, ex situ XAS, low-temperature Mössbauer spectroscopy, and DFT calculations.

Main Results:

  • Achieved a highly porous carbon support with a surface area of ≈3295 m² g⁻¹.
  • Obtained a high electrochemical active site density of 2.54 × 10¹⁹ sites gFeNC⁻¹.
  • Demonstrated a record 52% FeNx electrochemical utilization with no Fe clustering after stress testing, suggesting stable penta-coordinated Fe sites.

Conclusions:

  • The developed synthesis method effectively creates highly porous FeNC electrocatalysts with significantly enhanced iron utilization and stability.
  • The study identifies penta-coordinated Fe sites as crucial for the catalyst's performance.
  • These findings pave the way for practical applications of FeNC catalysts in proton exchange membrane fuel cells.