Electrocatalytic synthesis of adipic acid coupled with H<sub>2</sub> production enhanced by a ligand modification strategy.

Li, Zhenhua; Li, Xiaofan; Zhou, Hua; Xu, Yan; Xu, Si-Min; Ren, Yue; Yan, Yifan; Yang, Jiangrong et al. · Nat Commun · 2022

basic_science · Level V

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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 H<sub>2</sub> production over a nickel hydroxide (Ni(OH)<sub>2</sub>) 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)<sub>2</sub> (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<sub>2</sub> production, attaining adipic acid productivity of 4.7 mmol coupled with H<sub>2</sub> productivity of 8.0 L at 0.8 A (corresponding to 30 mA cm<sup>-2</sup>) in 24 h.