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

利用Cu-Mo双位点催化剂在环己酮肟电合成中实现超过90%的法拉第效率

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Abstract

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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