Liu Xiang, Zhu Yu-Quan, Li Jing, Wang Ye, Shi Qiujin, Li An-Zhen, Ji Kaiyue, Wang Xi, Zhao Xikang, Zheng Jinyu, Duan Haohong
Department of Chemistry, Tsinghua University, Beijing, China.
Hubei Key Laboratory of Pollutant Analysis & Reuse Technology, College of Chemistry and Chemical Engineering, Hubei Normal University, Huangshi, China.
Nat Commun. 2024 Sep 3;15(1):7685. doi: 10.1038/s41467-024-51951-0.
Electrosynthesis of adipic acid (a precursor for nylon-66) from KA oil (a mixture of cyclohexanone and cyclohexanol) represents a sustainable strategy to replace conventional method that requires harsh conditions. However, its industrial possibility is greatly restricted by the low current density and competitive oxygen evolution reaction. Herein, we modify nickel layered double hydroxide with vanadium to promote current density and maintain high faradaic efficiency (>80%) within a wide potential window (1.5 ~ 1.9 V vs. reversible hydrogen electrode). Experimental and theoretical studies reveal two key roles of V modification, including accelerating catalyst reconstruction and strengthening cyclohexanone adsorption. As a proof-of-the-concept, we construct a membrane electrode assembly, producing adipic acid with high faradaic efficiency (82%) and productivity (1536 μmol cm h) at industrially relevant current density (300 mA cm), while achieving >50 hours stability. This work demonstrates an efficient catalyst for adipic acid electrosynthesis with high productivity that shows industrial potential.
由KA油（环己酮和环己醇的混合物）电合成己二酸（尼龙-66的前体）是一种可持续的策略，用以取代需要苛刻条件的传统方法。然而，其工业应用可能性受到低电流密度和竞争性析氧反应的极大限制。在此，我们用钒修饰镍层状双氢氧化物，以提高电流密度，并在较宽的电位窗口（相对于可逆氢电极1.5~1.9V）内保持高法拉第效率（>80%）。实验和理论研究揭示了钒修饰的两个关键作用，包括加速催化剂重构和增强环己酮吸附。作为概念验证，我们构建了一个膜电极组件，在工业相关电流密度（300 mA cm）下，以高法拉第效率（82%）和生产率（1536 μmol cm h）生产己二酸，同时实现了>50小时的稳定性。这项工作展示了一种用于己二酸电合成的高效催化剂，具有高生产率，显示出工业应用潜力。
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