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Synergistic enhancement of electrochemical alcohol oxidation by combining NiV-layered double hydroxide with an aminoxyl radical

Author

Listed:
  • Suiqin Li

    (Zhejiang University of Technology)

  • Shibin Wang

    (Zhejiang University of Technology)

  • Yuhang Wang

    (Zhejiang University of Technology)

  • Jiahui He

    (Zhejiang University of Technology)

  • Kai Li

    (Zhejiang University of Technology)

  • James B. Gerken

    (University of Wisconsin-Madison)

  • Shannon S. Stahl

    (University of Wisconsin-Madison)

  • Xing Zhong

    (Zhejiang University of Technology)

  • Jianguo Wang

    (Zhejiang University of Technology)

Abstract

Electrochemical alcohol oxidation (EAO) represents an effective method for the production of high-value carbonyl products. However, its industrial viability is hindered by suboptimal efficiency stemming from low reaction rates. Here, we present a synergistic electrocatalysis approach that integrates an active electrode and aminoxyl radical to enhance the performance of EAO. The optimal aminoxyl radical (4-acetamido-2,2,6,6-tetramethylpiperidine 1-oxyl) and Ni0.67V0.33-layered double hydroxide (LDH) are screen as cooperative electrocatalysts by integrating theoretical predictions and experiments. The Ni0.67V0.33-LDH facilitates the adsorption and activation of N-(1-hydroxy-2,2,6,6-tetramethylpiperidin-4-yl)acetamide (ACTH) via interactions with ketonic oxygen, thereby improving selectivity and yield at high current densities. The electrolysis process is scaled up to produce 200 g of the steroid carbonyl product 8b (19-Aldoandrostenedione), achieving a yield of 91% and a productivity of 243 g h-1. These results represent a promising method for accelerating electron transfer to enhance alcohol oxidation, highlighting its potential for practical electrosynthesis applications.

Suggested Citation

  • Suiqin Li & Shibin Wang & Yuhang Wang & Jiahui He & Kai Li & James B. Gerken & Shannon S. Stahl & Xing Zhong & Jianguo Wang, 2025. "Synergistic enhancement of electrochemical alcohol oxidation by combining NiV-layered double hydroxide with an aminoxyl radical," Nature Communications, Nature, vol. 16(1), pages 1-14, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-024-55616-w
    DOI: 10.1038/s41467-024-55616-w
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    References listed on IDEAS

    as
    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.
    2. Ganceng Yang & Yanqing Jiao & Haijing Yan & Ying Xie & Chungui Tian & Aiping Wu & Yu Wang & Honggang Fu, 2022. "Unraveling the mechanism for paired electrocatalysis of organics with water as a feedstock," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    3. Lin Chen & Chang Yu & Xuedan Song & Junting Dong & Jiawei Mu & Jieshan Qiu, 2024. "Integrated electrochemical and chemical system for ampere-level production of terephthalic acid alternatives and hydrogen," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    4. Artavazd Badalyan & Shannon S. Stahl, 2016. "Cooperative electrocatalytic alcohol oxidation with electron-proton-transfer mediators," Nature, Nature, vol. 535(7612), pages 406-410, July.
    5. Jian Jiang & Fanfei Sun & Si Zhou & Wei Hu & Hao Zhang & Jinchao Dong & Zheng Jiang & Jijun Zhao & Jianfeng Li & Wensheng Yan & Mei Wang, 2018. "Atomic-level insight into super-efficient electrocatalytic oxygen evolution on iron and vanadium co-doped nickel (oxy)hydroxide," Nature Communications, Nature, vol. 9(1), pages 1-12, December.
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