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Electrocatalytic synthesis of adipic acid coupled with H2 production enhanced by a ligand modification strategy

Author

Listed:
  • Zhenhua Li

    (Beijing University of Chemical Technology)

  • Xiaofan Li

    (Beijing University of Chemical Technology)

  • Hua Zhou

    (Beijing University of Chemical Technology
    Tsinghua University
    Haihe Laboratory of Sustainable Chemical Transformations)

  • Yan Xu

    (Shandong University of Science and Technology)

  • Si-Min Xu

    (Beijing University of Chemical Technology)

  • Yue Ren

    (Beijing University of Chemical Technology)

  • Yifan Yan

    (Beijing University of Chemical Technology)

  • Jiangrong Yang

    (Beijing University of Chemical Technology)

  • Kaiyue Ji

    (Tsinghua University)

  • Li Li

    (Beijing Institute of Petrochemical Technology)

  • Ming Xu

    (Beijing University of Chemical Technology)

  • Mingfei Shao

    (Beijing University of Chemical Technology)

  • Xianggui Kong

    (Beijing University of Chemical Technology)

  • Xiaoming Sun

    (Beijing University of Chemical Technology)

  • Haohong Duan

    (Tsinghua University
    Haihe Laboratory of Sustainable Chemical Transformations)

Abstract

Adipic acid is an important building block of polymers, and is commercially produced by thermo-catalytic oxidation of ketone-alcohol oil (a mixture of cyclohexanol and cyclohexanone). However, this process heavily relies on the use of corrosive nitric acid while releases nitrous oxide as a potent greenhouse gas. Herein, we report an electrocatalytic strategy for the oxidation of cyclohexanone to adipic acid coupled with H2 production over a nickel hydroxide (Ni(OH)2) catalyst modified with sodium dodecyl sulfonate (SDS). The intercalated SDS facilitates the enrichment of immiscible cyclohexanone in aqueous medium, thus achieving 3.6-fold greater productivity of adipic acid and higher faradaic efficiency (FE) compared with pure Ni(OH)2 (93% versus 56%). This strategy is demonstrated effective for a variety of immiscible aldehydes and ketones in aqueous solution. Furthermore, we design a realistic two-electrode flow electrolyzer for electrooxidation of cyclohexanone coupling with H2 production, attaining adipic acid productivity of 4.7 mmol coupled with H2 productivity of 8.0 L at 0.8 A (corresponding to 30 mA cm−2) in 24 h.

Suggested Citation

  • Zhenhua Li & Xiaofan Li & Hua Zhou & Yan Xu & Si-Min Xu & Yue Ren & Yifan Yan & Jiangrong Yang & Kaiyue Ji & Li Li & Ming Xu & Mingfei Shao & Xianggui Kong & Xiaoming Sun & Haohong Duan, 2022. "Electrocatalytic synthesis of adipic acid coupled with H2 production enhanced by a ligand modification strategy," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-32769-0
    DOI: 10.1038/s41467-022-32769-0
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    References listed on IDEAS

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    1. Hong Nhan Nong & Lorenz J. Falling & Arno Bergmann & Malte Klingenhof & Hoang Phi Tran & Camillo Spöri & Rik Mom & Janis Timoshenko & Guido Zichittella & Axel Knop-Gericke & Simone Piccinin & Javier P, 2020. "Key role of chemistry versus bias in electrocatalytic oxygen evolution," Nature, Nature, vol. 587(7834), pages 408-413, November.
    2. Dohyung Kim & Sunmoon Yu & Fan Zheng & Inwhan Roh & Yifan Li & Sheena Louisia & Zhiyuan Qi & Gabor A. Somorjai & Heinz Frei & Lin-Wang Wang & Peidong Yang, 2020. "Selective CO2 electrocatalysis at the pseudocapacitive nanoparticle/ordered-ligand interlayer," Nature Energy, Nature, vol. 5(12), pages 1032-1042, December.
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    Cited by:

    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. Meng He & Rui Li & Chuanqi Cheng & Cuibo Liu & Bin Zhang, 2024. "Microenvironment regulation breaks the Faradaic efficiency-current density trade-off for electrocatalytic deuteration using D2O," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    3. Kejian Kong & An-Zhen Li & Ye Wang & Qiujin Shi & Jing Li & Kaiyue Ji & Haohong Duan, 2023. "Electrochemical carbon–carbon coupling with enhanced activity and racemate stereoselectivity by microenvironment regulation," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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