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Atomically Dispersed Zr-N Moieties Modulate Fe Coordination for Robust Oxygen Reduction Electrocatalysis.

Siqi Qiu1, Hao Wan2, Yuechao Yao1

  • 1Guangdong Provincial Key Laboratory of New Energy Materials Service Safety & Shenzhen Key Laboratory of Special Functional Materials & Shenzhen Engineering Laboratory for Advance Technology of Ceramics, College of Materials Science and Engineering, Shenzhen University, Shenzhen, Guangdong, 518060, P. R. China.

Advanced Science (Weinheim, Baden-Wurttemberg, Germany)
|September 29, 2025
PubMed
Summary

This study introduces a novel iron-zirconium dual-atom catalyst (Fe,Zr-NC) for the oxygen reduction reaction (ORR). The catalyst demonstrates exceptional stability and performance, outperforming platinum/carbon (Pt/C) in energy applications.

Keywords:
Fe coordination environmentdual‐atom catalystsoxygen reduction reactionzinc–air batteries

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Catalysis

Background:

  • Iron-nitrogen-carbon (Fe-N-C) materials are promising non-precious metal catalysts for the oxygen reduction reaction (ORR).
  • Long-term stability of Fe-N-C catalysts is limited by Fe dissolution and carbon corrosion.
  • Developing stable and efficient ORR catalysts is crucial for energy technologies like fuel cells and metal-air batteries.

Purpose of the Study:

  • To develop a highly stable and efficient non-precious metal catalyst for the oxygen reduction reaction (ORR).
  • To investigate the synergistic effects of dual-atom doping (Fe and Zr) on catalyst performance and stability.
  • To provide design principles for next-generation ORR electrocatalysts.

Main Methods:

  • One-step solid-state synthesis of a Fe-Zr dual-atom carbon-based catalyst (Fe,Zr-NC).
  • Density Functional Theory (DFT) calculations to understand electronic structure and reaction mechanisms.
  • Experimental characterization using Extended X-ray Absorption Fine Structure (EXAFS) and electrochemical testing (cyclic voltammetry, zinc-air battery performance).

Main Results:

  • The Fe,Zr-NC catalyst exhibits a dual-metal coordination structure with atomically dispersed Zr-N units adjacent to Fe-N4 centers.
  • DFT calculations and EXAFS confirmed optimal Fe-Zr synergy and weakened *OH adsorption, addressing the ORR rate-limiting step.
  • The catalyst achieved a high half-wave potential (0.891 V vs RHE), negligible activity loss over 5000 cycles, outperforming Pt/C.
  • In zinc-air batteries, it delivered a peak power density of 185.7 mW cm⁻² and stable operation for over 453 hours.

Conclusions:

  • Dual-atom synergy in Fe,Zr-NC catalysts effectively modulates electronic structure and intermediate binding energies for enhanced ORR activity and stability.
  • The developed Fe,Zr-NC catalyst presents a viable, high-performance alternative to precious metal catalysts for energy conversion applications.
  • This work offers valuable insights and design strategies for creating advanced electrocatalysts for the oxygen reduction reaction.