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Tuning Nitrogen Configurations in Nitrogen-Doped Graphene Encapsulating Fe3C Nanoparticles for Enhanced Nitrate

Taiquan Rao1, Jiayu Zhan1, Yida Du1

  • 1National-Local Joint Engineering Laboratory for Energy Conservation in Chemical Process Integration and Resources Utilization, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin, 300130, P. R. China.

Chemsuschem
|January 8, 2025
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Summary

This study presents Fe3C@NG-X catalysts for electrochemical nitrate reduction, achieving high ammonia production efficiency. The catalyst demonstrates excellent performance and stability for ammonia synthesis and nitrate removal.

Keywords:
ElectrocatalysisNitrate reductionNitrogen configurationsNitrogen-doped grapheneStructural reconstruction

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Environmental Chemistry

Background:

  • Electrochemical nitrate reduction reaction (NO3RR) is a key technology for sustainable ammonia synthesis and wastewater nitrate remediation.
  • Developing efficient electrocatalysts is crucial for advancing NO3RR applications.

Purpose of the Study:

  • To fabricate and characterize novel Fe3C nanoparticles embedded in pyridinic-N doped graphene (Fe3C@NG-X) for electrochemical nitrate reduction.
  • To investigate the catalytic performance and structural evolution of the Fe3C@NG-X catalysts during NO3RR.

Main Methods:

  • A self-sacrificing template method was employed to synthesize Fe3C@NG-X catalysts.
  • Electrochemical measurements were conducted to evaluate Faradaic efficiency (FE) and ammonia yield rate.
  • In-situ structural analysis was performed to understand catalyst reconstruction.

Main Results:

  • Fe3C@NG-10 demonstrated a high FE of 94.03% for ammonia production at -0.5 V vs. RHE.
  • An impressive ammonia yield rate of 477.73 mmol h-1 gcat-1 was achieved.
  • The catalyst maintained high FE (>90%) over a wide potential and nitrate concentration range (12.5-500 mM).
  • Structural reconstruction to Fe/Fe3C@NG-X heterojunction was observed during catalysis, enhancing activity.

Conclusions:

  • The Fe3C@NG-X catalysts, particularly Fe3C@NG-10, exhibit remarkable performance for electrochemical nitrate reduction to ammonia.
  • The high pyridinic-N content and the formation of Fe/Fe3C@NG-X heterojunctions are responsible for the enhanced catalytic activity.
  • These findings offer a promising pathway for efficient ammonia synthesis and nitrate removal in wastewater treatment.