Energy‐Saving Ambient Electrosynthesis of Nylon‐6 Precursor Coupled with Electrocatalytic Upcycling of Polyethylene Terephthalate

Abstract Cyclohexanone oxime is an important intermediate in the chemical industry, especially for the manufacture of nylon‐6. The traditional cyclohexanone oxime production strongly relies on cyclohexanone‐hydroxylamine and cyclohexanone ammoxidation processes, which require harsh reaction conditions and consume considerable amounts of energy. Herein, direct electrosynthesis of cyclohexanone oxime is reported from environmental pollutants nitrite and cyclohexanone with almost 100% yield by using low‐cost Cu 2 Se nanosheets as electrocatalysts. Combination of in situ Fourier transform infrared spectroscopy and theoretical calculations verifies that the p–d orbital hybridization between Cu and Se elements could synergistically optimize the surface electronic structure and enable improved adsorption and formation of the key active N intermediate NH 2 OH*, thereby enhancing cyclohexanone/nitrite‐to‐cyclohexanone oxime conversion over the Cu 2 Se nanosheets. Based on these, an efficient asymmetric co‐electrolysis system is further demonstrated by coupling cyclohexanone/nitrite‐to‐cyclohexanone oxime conversion with the upcycling of polyethylene terephthalate plastics, achieveing energy‐saving simultaneously production of value‐added products (cyclohexanone oxime and glycolic acid).