Recycling Ni‐Rich <scp>NCM</scp> Cathode Materials From Spent Li‐Ion Batteries as Efficient Electrocatalyst for Urea Oxidation

The burgeoning electric vehicle industry has intensified the demand for high‐energy Ni‐Co‐Mn (NCM) cathodes, yet their end‐of‐life management remains a critical environmental challenge. Here, we show that spent high‐Ni NCM (LiNi 0.92 Co 0.05 Mn 0.03 O 2 ) cathode materials can be directly upcycled into robust urea oxidation (UOR) catalysts. A facile solvent‐only delamination converts discarded cathodes into printable inks; drop‐casting onto carbon paper yields electrodes delivering ~10 mA mg −1 at 1.50 V versus RHE. Operando synchrotron X‐ray diffraction reveals that K + ions spontaneously intercalate into Li‐deficient interlayers, expanding the (003) interplanar spacing from 4.7 to 7.1 Å. An electrochemical–chemical (E–C) reaction mechanism is proposed, in which Ni 3+ species are electrochemically generated on the catalyst surface and are then chemically reduced during urea oxidation, a process promoted by K + intercalation. This lattice‐engineered redox process stabilizes the layered framework and suppresses metal dissolution, ensuring &gt;24 h of continuous urea electrolysis. The work offers a circular economy solution for battery waste treatment while providing atomistic design principles for next‐generation, earth‐abundant environmental catalysts.