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Driving Adsorbate Evolution via Oxygenated Surface Species Modulation for Ammonia Electrooxidation.

Jeongwon Kim1,2,3, Yucheng Hang1, Hyundo Park3

  • 1UNIST-NUIST Energy and Environment Jointed Lab (UNNU), School of Environment Science and technology, Nanjing University of Information Science and Technology, No.219, Ningliu Road, Nanjing, 210044, P.R. China.

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Summary

This study introduces a novel catalyst for electrochemical ammonia oxidation to nitrogen, enhancing sustainable nitrogen cycles and hydrogen production. The new catalyst shows improved kinetics and stability, paving the way for efficient electrocatalysis.

Keywords:
AlloyAmmoniaHydroperoxideIn situ FT‐IRSurface activationWastewater

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Sustainable Chemistry

Background:

  • Electrochemical ammonia oxidation (eAOR) to dinitrogen is key for sustainable nitrogen cycles and hydrogen generation.
  • Conventional catalysts like Pt and Pt-Ir alloys exhibit sluggish kinetics and poor stability in eAOR.
  • Understanding reaction mechanisms, including *NHx dehydrogenation and proton-coupled electron transfer, is crucial.

Purpose of the Study:

  • To develop a novel catalyst that enhances the kinetics and stability of the electrochemical ammonia oxidation reaction (eAOR) to dinitrogen.
  • To investigate the role of oxygenated co-adsorbates in steering the adsorbate-evolution pathway for improved eAOR performance.
  • To establish an adsorbate-assisted mechanism design approach for advanced nitrogen species electrocatalysis.

Main Methods:

  • Synthesis of an exsolved Pt3Ni alloy on a perovskite scaffold.
  • In situ Fourier transform infrared spectroscopy (FTIR) to study reaction intermediates.
  • Density functional theory (DFT) calculations to elucidate the reaction mechanism.
  • Electrochemical performance testing in a solar-driven ammonia electrolyzer.

Main Results:

  • The Pt3Ni alloy catalyst selectively stabilizes *OOH and strengthens *NH2 binding, enhancing the eAOR.
  • The catalyst exhibits a mass activity of 862 A gPt−1, surpassing current benchmarks.
  • In a solar-driven electrolyzer, it achieved 13.7 mA at 1.0 V and stable hydrogen production (394 L kWh−1).

Conclusions:

  • Controlling oxygenated co-adsorbates is an effective strategy to steer the adsorbate-evolution pathway in eAOR.
  • The exsolved Pt3Ni alloy catalyst demonstrates superior performance and stability for sustainable ammonia electrooxidation.
  • This work provides a new mechanism-based design approach for developing efficient electrocatalysts for nitrogen-based reactions.