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Electrocatalytic synthesis of adipic acid coupled with H(2) production enhanced by a ligand modification strategy

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 gr...

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Detalles Bibliográficos
Autores principales: Li, Zhenhua, Li, Xiaofan, Zhou, Hua, Xu, Yan, Xu, Si-Min, Ren, Yue, Yan, Yifan, Yang, Jiangrong, Ji, Kaiyue, Li, Li, Xu, Ming, Shao, Mingfei, Kong, Xianggui, Sun, Xiaoming, Duan, Haohong
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9411531/
https://www.ncbi.nlm.nih.gov/pubmed/36008416
http://dx.doi.org/10.1038/s41467-022-32769-0
Descripción
Sumario: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 H(2) 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 H(2) production, attaining adipic acid productivity of 4.7 mmol coupled with H(2) productivity of 8.0 L at 0.8 A (corresponding to 30 mA cm(−2)) in 24 h.