Achieving over 90% Faradaic Efficiency in Cyclohexanone Oxime Electrosynthesis Using the Cu–Mo Dual-Site Catalyst

化学 电合成 环己酮肟 催化作用 肟 环己酮 对偶(语法数字) 有机化学 物理化学 电化学 电极 文学类 艺术
作者
Runyao Zhao,Yiding Wang,Jiaju Fu,Fengtao Zhang,Linzi Wen,Yanfei Zhao,Bo Guan,Buxing Han,Zhimin Liu
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:146 (40): 27956-27963 被引量:82
标识
DOI:10.1021/jacs.4c11413
摘要

High Resolution Image Download MS PowerPoint Slide Coupling with the nitrate electroreduction reaction (NitRR), the electrosynthesis of cyclohexanone oxime (CHO, the vital feedstock in the nylon-6 industry) from cyclohexanone provides a promising alternative to the traditional energy consumption process. However, it still suffers from low efficiency because selective production of *NH 2 OH intermediate from NitRR under large current densities is challenging. We here report a Cu 1 MoO x /nitrogen-doped carbon (NC) electrocatalyst with high-density Cu–Mo dual sites for NitRR to selectively produce and stabilize *NH 2 OH, with the subsequent cyclohexanone oximation achieving the highest CHO Faradaic efficiency of 94.5% and a yield rate of 3.0 mol g –1 h –1 at an industrially relevant current density of 0.5 A cm –2 . Furthermore, in situ characterizations evidenced that the Cu–Mo dual sites in Cu 1 MoO x /NC effectively inhibited hydrodeoxygenation of hydroxyl-containing intermediates of NitRR, selectively producing *NH 2 OH and thus achieving cyclohexanone oximation with high efficiency. This work provides a high-performance catalyst for CHO electrosynthesis from nitrogenous waste, showing promising application potential in industrial production of CHO.
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