Boosting urea electrooxidation on oxyanion-engineered nickel sites via inhibited water oxidation
Open accessAbstract
Renewable energy-based electrocatalytic oxidation of organic nucleophiles (e.g.methanol, urea, and amine) are more thermodynamically favourable and, economically attractive to replace conventional pure water electrooxidation in electrolyser to produce hydrogen. However, it is challenging due to the competitive oxygen evolution reaction under a high current density (e.g., >300 mA cm−2), which reduces the anode electrocatalyst’s activity and stability. Herein, taking lower energy cost urea electrooxidation reaction as the model reaction, we developed oxyanion-engineered Nickel catalysts to inhibit competing oxygen evolution reaction during urea oxidation reaction, achieving an ultrahigh 323.4 mA cm−2 current density at 1.65 V with 99.3 ± 0.4% selectivity of N-products. In situ spectra studies reveal that such in situ generated oxyanions not only inhibit OH− adsorption and guarantee high coverage of urea reactant on active sites to avoid oxygen evolution reaction, but also accelerate urea’s C − N bond cleavage to form CNO − intermediates for facilitating urea oxidation reaction. Accordingly, a comprehensive mechanism for competitive adsorption behaviour between OH− and urea to boost urea electrooxidation and dynamic change of Ni active sites during urea oxidation reaction was proposed. This work presents a feasible route for high-efficiency urea electrooxidation reaction and even various electrooxidation reactions in practical applications.
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UOR has a theoretical potential of 0.37 V.
“replacing OER with the urea oxidation reaction (UOR), which has a much lower theoretical potential (0.37 V) [3,6].”
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- Authors
- Gao, X., Bai, X., Wang, P., Jiao, Y., Davey, K., Zheng, Y., & Qiao, S.-Z.
- Affiliations
- The University of Adelaide (AU)
- Corresponding author
- Zheng, Yao
- Qiao, Shi-Zhang
- Venue
- Nature Communications
- Published
- 2023-09-20
- Volume
- 14
- Issue
- 1
- Pages
- 5842-5842
- ISSN
- 2041-1723 (ISSN-L)
- PMC
- PMC10511637
- OpenAlex
- W4386887861
- Cited by
- 306
- References
- 43
- Citations by year
- 2026: 74 · 2025: 125 · 2024: 102 · 2023: 5
- FWCI
- 14.62
- Type
- journal article
- Language
- en
- Open access
- gold
- doi.org
- Locations
- Nature Communications (publishedVersion, cc-by)
- PubMed Central (publishedVersion, cc-by)
- PubMed (publishedVersion)
- RePEc: Research Papers in Economics (submittedVersion)
- Adelaide Research & Scholarship (AR&S) (University of Adelaide) (submittedVersion, cc-by)
- DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
- Funders
- Australian Nuclear Science and Technology Organisation
- Australian Synchrotron
- University of Adelaide
- China Scholarship Council
- Australian Research Council (FT200100062, DP190103472, DP220102596, LP210301397, FL170100154)
- 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 › Engineering › Electrical and Electronic Engineering › Fuel Cells and Related Materials
- Keywords
- urea electrooxidation, nickel-based electrocatalysts, competitive adsorption, hydroxide adsorption, C–N bond cleavage, electrocatalytic hydrogen production, anode catalysts
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