Boosting urea electrooxidation on oxyanion-engineered nickel sites via inhibited water oxidation
Date
2023
Authors
Gao, X.
Bai, X.
Wang, P.
Jiao, Y.
Davey, K.
Zheng, Y.
Qiao, S.-Z.
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Advisors
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Journal article
Citation
Nature Communications, 2023; 14(1):5842-1-5842-10
Statement of Responsibility
Xintong Gao, Xiaowan Bai, Pengtang Wang, Yan Jiao, Kenneth Davey, Yao Zheng, Shi-Zhang Qiao
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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.
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Published online: 20 September 2023
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© The Author(s) 2023. Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.