Boosting electrocatalytic oxidation of heterocyclic alcohols with low usage aminoxyl radicals via MOF‐derived NiOOH

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 s...

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Bibliographic Details
Published in:AIChE journal 2024-10, Vol.70 (10), p.n/a
Main Authors: Li, Kai, Ren, Linhan, Li, Suiqin, Liu, LiHao, He, Jiahui, Xu, Yinjie, Wang, Mengxin, Zhao, Shuying, Wang, Yuhang, Chen, Ying, Wang, Jieyu, Zhong, Xing, Wang, Jianguo
Format: Article
Language:English
Subjects:
Alcohols
Carboxylic acids
Electrocatalysts
electrocatalytic oxidation
enantiomeric retention
heterocyclic alcohol
In situ measurement
Industrial applications
Nickel
NiOOH
Oxidation
Radicals
reconstruction
Scale (corrosion)
Synergistic effect
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Summary: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. In addition, the synergistic system was extended to the oxidation of various heterocyclic alcohols. The scale‐up synthesis of chiral acid (LEV‐CO2H) 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/m3 h. The practicality and effectiveness of this synergistic electrocatalytic strategy in practical electrosynthesis was further demonstrated.
ISSN:0001-1541
1547-5905
DOI:10.1002/aic.18531