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 *NHOH intermediate from NitRR under large current densities is challenging. We here report a CuMoO/nitrogen-doped carbon (NC) electrocatalyst with high-density Cu-Mo dual sites for NitRR to selectively produce and stabilize *NHOH, with the subsequent cyclohexanone oximation achieving the highest CHO Faradaic efficiency of 94.5% and a yield rate of 3.0 mol g h at an industrially relevant current density of 0.5 A cm. Furthermore, in situ characterizations evidenced that the Cu-Mo dual sites in CuMoO/NC effectively inhibited hydrodeoxygenation of hydroxyl-containing intermediates of NitRR, selectively producing *NHOH 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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| http://dx.doi.org/10.1021/jacs.4c11413 | DOI Listing |
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