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- Title
Boosting urea electrooxidation on oxyanion-engineered nickel sites via inhibited water oxidation.
- Authors
Gao, Xintong; Bai, Xiaowan; Wang, Pengtang; Jiao, Yan; Davey, Kenneth; Zheng, Yao; Qiao, Shi-Zhang
- Abstract
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. Urea electrooxidation reaction is of great importance in energy related applications and devices but is limited by competing oxygen evolution reaction. Here, the authors report oxyanion-engineered nickel catalysts that can achieve efficient urea oxidation while suppressing oxygen evolution reaction.
- Subjects
OXIDATION of water; UREA; NICKEL catalysts; SCISSION (Chemistry); NICKEL; OXYGEN evolution reactions; OXIDATION
- Publication
Nature Communications, 2023, Vol 14, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-023-41588-w