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Nonredox trivalent nickel catalyzing nucleophilic electrooxidation of organics

Author

Listed:
  • Yuandong Yan

    (Nanjing University)

  • Ruyi Wang

    (Nanjing University)

  • Qian Zheng

    (Nanjing University)

  • Jiaying Zhong

    (Nanjing University)

  • Weichang Hao

    (Beihang University)

  • Shicheng Yan

    (Nanjing University
    Nanjing University)

  • Zhigang Zou

    (Nanjing University
    Nanjing University)

Abstract

A thorough comprehension of the mechanism behind organic electrooxidation is crucial for the development of efficient energy conversion technology. Here, we find that trivalent nickel is capable of oxidizing organics through a nucleophilic attack and electron transfer via a nonredox process. This nonredox trivalent nickel exhibits exceptional kinetic efficiency in oxidizing organics that possess the highest occupied molecular orbital energy levels ranging from −7.4 to −6 eV (vs. Vacuum level) and the dual local softness values of nucleophilic atoms in nucleophilic functional groups, such as hydroxyls (methanol, ethanol, benzyl alcohol), carbonyls (formamide, urea, formaldehyde, glucose, and N-acetyl glucosamine), and aminos (benzylamine), ranging from −0.65 to −0.15. The rapid electrooxidation kinetics can be attributed to the isoenergetic channels created by the nucleophilic attack and the nonredox electron transfer via the unoccupied eg orbitals of trivalent nickel (t2g6eg1). Our findings are valuable in identifying kinetically fast organic electrooxidation on nonredox catalysts for efficient energy conversions.

Suggested Citation

  • Yuandong Yan & Ruyi Wang & Qian Zheng & Jiaying Zhong & Weichang Hao & Shicheng Yan & Zhigang Zou, 2023. "Nonredox trivalent nickel catalyzing nucleophilic electrooxidation of organics," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-43649-6
    DOI: 10.1038/s41467-023-43649-6
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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.
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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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