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Highly efficient overall urea electrolysis via single-atomically active centers on layered double hydroxide.

Huachuan Sun1, Linfeng Li1, Hsiao-Chien Chen2

  • 1School of Optical and Electronic Information, Wuhan National Laboratory for Optoelectronics, Optics Valley Laboratory, Huazhong University of Science and Technology, Wuhan 430074, China.

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|December 22, 2022
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Summary

A new Rh/NiV-LDH electrocatalyst efficiently drives urea electrolysis for hydrogen fuel production and wastewater treatment. This single-atom catalyst achieves high activity and stability, overcoming challenges in urea oxidation reactions.

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High turnover frequencyHydrogen evolution reactionLayer double hydroxideOverall urea electrolysisSingle-atomically active centers

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Environmental Engineering

Background:

  • Anodic urea oxidation reaction (UOR) offers a sustainable alternative to oxygen evolution reaction (OER) for simultaneous hydrogen fuel generation and wastewater purification.
  • Achieving high efficiency in overall urea electrolysis remains a significant challenge due to the sluggish kinetics of UOR.

Purpose of the Study:

  • To develop a multifunctional electrocatalyst, Rh/NiV-LDH, for efficient overall urea electrolysis.
  • To investigate the synergistic effects between rhodium single-atom catalyst (SAC) and nickel-vanadium layered double hydroxide (NiV-LDH) support.

Main Methods:

  • Integration of nickel-vanadium layered double hydroxide (NiV-LDH) with rhodium single-atom catalyst (SAC).
  • Electrochemical characterization including hydrogen evolution reaction (HER) and urea oxidation reaction (UOR) activity measurements.
  • Theoretical calculations to understand the catalytic mechanism and synergistic effects.

Main Results:

  • The Rh/NiV-LDH catalyst exhibited high HER mass activity (0.262 A mg⁻¹) and turnover frequency (2.125 s⁻¹ at 100 mV).
  • Exceptional UOR activity was achieved, requiring 1.33 V to reach 10 mA cm⁻², surpassing OER limitations.
  • Overall urea electrolysis using Rh/NiV-LDH required only 1.47 V to deliver 100 mA cm⁻² with excellent stability.

Conclusions:

  • The synergistic interaction between NiV-LDH support and atomically dispersed Rh sites enhances catalytic performance.
  • This multifunctional SAC design provides a promising pathway for efficient hydrogen fuel generation and urea-rich wastewater treatment via overall urea electrolysis.