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

    Year: 2022

    Journal: Nat. Commun., Volume 13, AUG 25

    Authors: 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

    Organizations: National Natural Science Foundation of China [21978147, 21935001, 22108008, 22090031, 22105026, 21991102, 32000922]; Beijing Municipal Natural Science Foundation [2214063]; Fundamental Research Funds for the Central Universities [buctrc202011]; Haihe Laboratory of Sustainable Chemical Transformations

    Adipic acid is an important building block of polymers, although its production relies on harmful reagents. Here, authors examined surfactant-modified nickel hydroxide for adipic acid electrosynthesis coupled with hydrogen gas evolution. 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.
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