Closed‐Loop Direct Upcycling of Spent Ni‐Rich Layered Cathodes into High‐Voltage Cathode Materials

Abstract Facing the resource and environmental pressures brought by the retiring wave of lithium‐ion batteries (LIBs), direct recycling methods are considered to be the next generation's solution. However, the contradiction between limited battery life and the demand for rapidly iterating technology forces the direct recovery paradigm to shift toward “direct upcycling.” Herein, a closed‐loop direct upcycling strategy that converts waste current collector debris into dopants is proposed, and a highly inclusive eutectic molten salt system is utilized to repair structural defects in degraded polycrystalline LiNi_0.83Co_0.12Mn_0.05O₂ cathodes while achieving single‐crystallization transformation and introducing Al/Cu dual‐doping. Upcycled materials can effectively overcome the two key challenges at high voltages: strain accumulation and lattice oxygen evolution. It exhibits comprehensive electrochemical performance far superior to commercial materials at 4.6 V, especially its fast charging capability at 15 C, and an impressive 91.1% capacity retention after 200 cycles in a 1.2 Ah pouch cell. Importantly, this approach demonstrates broad applicability to various spent layered cathodes, particularly showcasing its value in the recycling of mixed spent cathodes. This work effectively bridges the gap between waste management and material performance enhancement, offering a sustainable path for the recycling of spent LIBs and the production of next‐generation high‐voltage cathodes.