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Boosting urea electrooxidation on oxyanion-engineered nickel sites via inhibited water oxidation

Author

Listed:
  • Xintong Gao

    (The University of Adelaide)

  • Xiaowan Bai

    (The University of Adelaide)

  • Pengtang Wang

    (The University of Adelaide)

  • Yan Jiao

    (The University of Adelaide)

  • Kenneth Davey

    (The University of Adelaide)

  • Yao Zheng

    (The University of Adelaide)

  • Shi-Zhang Qiao

    (The University of Adelaide)

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.

Suggested Citation

  • Xintong Gao & Xiaowan Bai & Pengtang Wang & Yan Jiao & Kenneth Davey & Yao Zheng & Shi-Zhang Qiao, 2023. "Boosting urea electrooxidation on oxyanion-engineered nickel sites via inhibited water oxidation," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-41588-w
    DOI: 10.1038/s41467-023-41588-w
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    References listed on IDEAS

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    1. Shi-Kui Geng & Yao Zheng & Shan-Qing Li & Hui Su & Xu Zhao & Jun Hu & Hai-Bo Shu & Mietek Jaroniec & Ping Chen & Qing-Hua Liu & Shi-Zhang Qiao, 2021. "Nickel ferrocyanide as a high-performance urea oxidation electrocatalyst," Nature Energy, Nature, vol. 6(9), pages 904-912, September.
    2. Lichen Bai & Chia-Shuo Hsu & Duncan T. L. Alexander & Hao Ming Chen & Xile Hu, 2021. "Double-atom catalysts as a molecular platform for heterogeneous oxygen evolution electrocatalysis," Nature Energy, Nature, vol. 6(11), pages 1054-1066, November.
    3. Yanbin Qi & Yue Zhang & Li Yang & Yuhan Zhao & Yihua Zhu & Hongliang Jiang & Chunzhong Li, 2022. "Insights into the activity of nickel boride/nickel heterostructures for efficient methanol electrooxidation," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    4. Shanlin Li & Ruguang Ma & Jingcong Hu & Zichuang Li & Lijia Liu & Xunlu Wang & Yue Lu & George E. Sterbinsky & Shuhu Liu & Lei Zheng & Jie Liu & Danmin Liu & Jiacheng Wang, 2022. "Coordination environment tuning of nickel sites by oxyanions to optimize methanol electro-oxidation activity," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
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    1. Xiang Liu & Yu-Quan Zhu & Jing Li & Ye Wang & Qiujin Shi & An-Zhen Li & Kaiyue Ji & Xi Wang & Xikang Zhao & Jinyu Zheng & Haohong Duan, 2024. "Electrosynthesis of adipic acid with high faradaic efficiency within a wide potential window," Nature Communications, Nature, vol. 15(1), pages 1-16, December.

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