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Cited by 92Electrocatalysts for Energy ConversionCO2 Reduction Techniques and CatalystsAmmonia Synthesis and Nitrogen Reduction

Pairing N‐Vacancy and Adjacent Ni‐Sites in the Local Microenvironment to Regulate the Urea Oxidation Reaction Pathway With Enhanced Kinetics

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Ji, Chengwei, Duan, Huimei, Wang, Chuanhui, Liang, Guizeng, Long, Xiaojing, She, Xilin, Zhang, Rongrong, Gong, Feilong +3 more·2025·Advanced Materials
DOI 10.1002/adma.202503879PMC PMC12272033
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Abstract

The urea oxidation reaction (UOR) is a promising approach for replacing the oxygen evolution reaction in hydrogen production, offering lower energy consumption. However, the kinetics of Ni‐based catalysts for UOR are hindered by the high formation potential of NiOOH and its repeated transition with Ni(OH) 2 . In this study, a local microenvironment featuring electron‐deficient N‐vacancies (V N ) paired with adjacent electron‐rich Ni‐sites on Ni 3 N (Ni 3 N‐V N ) to enhance UOR kinetics is constructed. The electron‐rich Ni‐sites significantly reduce the energy barrier for NiOOH formation and promote the conversion of Ni(OH) 2 to NiOOH. Meanwhile, the V N sites induce low charge transfer resistance in Ni 3 N, facilitating efficient electron transfer and boosting UOR performance while ensuring the stability of the active NiOOH phase. The V N sites promote the adsorption of the urea N atom at the active site, favoring the reaction pathway toward “NCO⁻” formation without requiring complete urea dissociation. This pathway alleviates the NiOOH/Ni(OH) 2 conversion cycle, lowers charge transfer resistance, and improves reaction kinetics. Ni 3 N‐V N demonstrates excellent UOR activity (low potential of 1.46 V at 1000 mA cm −2 ) and industrial prospects (integrating into an anion exchange membrane flow electrolyzer with 20% Pt/C, producing 600 mA cm −2 at 1.84 V), highlighting its potential for practical applications.

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  • Nitrogen doping enhances the UOR through the formation of M-Nx coordination sites, which modulate the electronic structure of the metal centres by increasing local electron density and facilitating charge transfer.

    “Nitrogen doping enhances the UOR through the formation of M–Nx coordination sites [62,63], which modulate the electronic structure of the metal centres by increasing the local electron density and facilitating charge transfer during catalysis [64].”

    From Impact of carbon and nitrogen doping on trimetallic iron–nickel–cobalt aerogels as electrocatalysts for enhanced urea oxidation: A strategy for energy-efficient hydrogen production (2026) · cites this paper as [63]

    The Introduction and Results and Discussion (pages not provided) report that nitrogen vacancies in Ni3N create electron-rich Ni sites, alter their electronic environment, and improve charge transfer and UOR kinetics. They do not attribute those effects to nitrogen doping that forms M–Nx coordination sites; the reported intervention is the introduction of nitrogen vacancies, with a reduced Ni–N coordination number. (LLM, conf=0.88)

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Cited by

Sorted by citations

Authors
Ji, C., Duan, H., Wang, C., Liang, G., Long, X., She, X., Zhang, R., Gong, F., Li, D., Yang, D., & Liu, J.
Affiliations
  • Qingdao University (CN)
  • Jilin University (CN)
  • Zhengzhou University of Light Industry (CN)
  • Inner Mongolia University (CN)
Corresponding author
  • Li, Daohao
  • Yang, Dongjiang
  • Liu, Jian
ORCID
Venue
Advanced Materials
Publisher
Wiley
Published
2025-04-16
Volume
37
Issue
28
Pages
e2503879-e2503879
ISSN
  • 0935-9648 (ISSN-L)
  • 1521-4095
DOI
10.1002/adma.202503879
PMC
PMC12272033
OpenAlex
W4409508390
Cited by
92
References
3
Citations by year
2026: 70 · 2025: 22
FWCI
12.70
Type
journal article
Language
en
Open access
Licence
Locations
  • Advanced Materials (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
Funders
  • National Natural Science Foundation of China (52302272, 22376110, 62227815)
  • Natural Science Foundation of Shandong Province (ZR2022QB023, ZR2024JQ037)
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
  • Physical Sciences › Chemical Engineering › Catalysis › Ammonia Synthesis and Nitrogen Reduction
Keywords
urea oxidation reaction, nickel nitride, nitrogen vacancies, nickel oxyhydroxide, nickel hydroxide, reaction pathways, charge transfer resistance, anion exchange membrane water electrolyzer, oxygen evolution reaction replacement, hydrogen production, urea adsorption, electrocatalysis

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