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Boosting electrocatalytic oxidation of heterocyclic alcohols with low usage aminoxyl radicals via MOF-derived NiOOH
  • +10
  • Jian-guo Wang,
  • Kai Li,
  • Linhan Ren,
  • Suiqin Li,
  • LiHao Liu,
  • Jiahui He,
  • Yinjie Xu,
  • Mengxin Wang,
  • Shuying Zhao,
  • Yuhang Wang,
  • Ying Chen,
  • Jieyu Wang,
  • Xing Zhong
Jian-guo Wang
Zhejiang University of Technology College of Chemical Engineering

Corresponding Author:[email protected]

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Kai Li
Zhejiang University of Technology College of Chemical Engineering
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Linhan Ren
Zhejiang University of Technology College of Chemical Engineering
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Suiqin Li
Zhejiang University of Technology College of Chemical Engineering
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LiHao Liu
Zhejiang University of Technology College of Chemical Engineering
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Jiahui He
Zhejiang University of Technology College of Chemical Engineering
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Yinjie Xu
Zhejiang University of Technology College of Chemical Engineering
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Mengxin Wang
Zhejiang University of Technology College of Chemical Engineering
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Shuying Zhao
Zhejiang University of Technology College of Chemical Engineering
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Yuhang Wang
Zhejiang University of Technology College of Chemical Engineering
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Ying Chen
Zhejiang University of Technology College of Chemical Engineering
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Jieyu Wang
Zhejiang University of Technology College of Chemical Engineering
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Xing Zhong
Zhejiang University of Technology College of Chemical Engineering
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Abstract

Aminoxyl-mediated electrocatalysis offers a sustainable approach for the oxidation of alcohols to carboxylic acids. However, the high dosage of aminoxyl radicals and the limiting current density hinder the practicality of industrial application. Herein, a nickel-based electrocatalyst (Ni-tpdc) was synthesized on a three-dimensional porous graphite felt substrate. Taking advantage of the synergistic effect of the electrochemically activated Ni-tpdc/GF electrocatalyst with 4-acetamido-TEMPO, the yield of 4-pyridinecarboxylic acid was up to 99% with only 1 mol% ACT. A series of in situ measurements showed that NiOOH enhanced the activity of the intrinsic electrocatalyst. Additionally, the synergistic system was extended to the oxidation of various heterocyclic alcohols. The scale-up synthesis of chiral acid (LEV-CO 2H) was achieved in an improved electrolyzer with a yield of 95.4%, enantiomeric retention of 99.2%, and space-time yield of 34.12 kg/(m 3·h). The practicality and effectiveness of this synergistic electrocatalytic strategy in practical electrosynthesis was further demonstrated.
13 Feb 2024Review(s) Completed, Editorial Evaluation Pending
13 Feb 2024Assigned to Editor
13 Feb 2024Submission Checks Completed
15 Feb 2024Reviewer(s) Assigned