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<p>Urea electrooxidation offered an energy-efficient alternative to water oxidation for hydrogen generation, but its implementation was hindered hindered by sluggish kinetics and instability under industrial current densities. We report a monolayer asymmetrically coordinated trimetallic atom sites catalyst (A-NiCoMn-TAC/LDH) with a defect-rich coordination environment. It requires 1.26 ± 0.01 V <i>vs</i>. RHE at 10 mA cm<sup>-2</sup> and maintains stability for 600 h at 500 mA cm<sup>-2</sup> in half-cell tests, and operates for 1500 h at an industrial level of 1000 mA cm<sup>-2</sup> in an anion-exchange membrane electrolyzer. X-ray absorption spectra reveal the defective coordination structures around the heterotrimetallic atoms and their electrochemical dynamic structural adaptation during the urea oxidation reaction. Through <i>operando</i> spectroscopy and theoretical calculations, we identify defect engineering induced strong <i>d-p-d</i> orbital coupling, creating a π-donation-mediated charge transfer pathway. This configuration lowers the energy barrier for the formation of CON<sub>2</sub>* and enhances urea adsorption over OH*, enabling high-performance urea oxidation.</p>

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Pronounced orbital-coupled asymmetrically coordinated NiCoMn heterotrimetallic atomic sites enable efficient thousand-hour urea electrooxidation-coupled hydrogen production

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月4日

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  • Teng Li,
  • Yarui Hu,
  • Zhiyi Sun,
  • Mingzi Sun,
  • Bolong Huang,
  • Wenxing Chen,
  • Bin Liu

摘要

Urea electrooxidation offered an energy-efficient alternative to water oxidation for hydrogen generation, but its implementation was hindered hindered by sluggish kinetics and instability under industrial current densities. We report a monolayer asymmetrically coordinated trimetallic atom sites catalyst (A-NiCoMn-TAC/LDH) with a defect-rich coordination environment. It requires 1.26 ± 0.01 V vs. RHE at 10 mA cm-2 and maintains stability for 600 h at 500 mA cm-2 in half-cell tests, and operates for 1500 h at an industrial level of 1000 mA cm-2 in an anion-exchange membrane electrolyzer. X-ray absorption spectra reveal the defective coordination structures around the heterotrimetallic atoms and their electrochemical dynamic structural adaptation during the urea oxidation reaction. Through operando spectroscopy and theoretical calculations, we identify defect engineering induced strong d-p-d orbital coupling, creating a π-donation-mediated charge transfer pathway. This configuration lowers the energy barrier for the formation of CON2* and enhances urea adsorption over OH*, enabling high-performance urea oxidation.