Bidirectional Lattice Anchoring Enhances Composition Reconfiguration of Spent Lithium‐Ion Cathodes

ABSTRACT High‐value recycling of retired lithium‐ion battery materials is pivotal for the circular economy. The nickel‐rich strategy, with its merits in boosting energy density, stands out as a key approach for upcycling spent LiNi 0.54 Co 0.16 Mn 0.3 O 2 (SNCM). However, the inherent structural defects of SNCM and the heterogeneous reactions among precursors during regeneration jointly induce irreversible phase transformations, preventing the formation of an ideally ordered layered structure. Therefore, we developed a targeted bidirectional anchoring strategy involving pre‐anchoring Al species on both SNCM and Ni(OH) 2 surfaces. This method reduces the energy barrier for lithiation in the surface‐disordered structures of SNCM and suppresses the structural degradation of nickel‐rich intermediate phases, thereby addressing the root cause of structural disorder during upcycling. The upcycled cathode material exhibits a stable layered structure and a distinctive nickel concentration gradient from the surface toward the bulk. It delivers outstanding electrochemical performance, including a reversible capacity of 186.84 mAh g −1 at 0.2C and retaining 90.17% of its initial capacity after 200 cycles at 1C, outperforming current commercial materials. Furthermore, this study provides essential insights into solid‐state regeneration and establishes a pathway toward the high‐value recycling of degraded lithium‐ion batteries, demonstrating great potential for practical application.