Breaking the Superexchange Interlock for High-Performance Regeneration of Degraded Single-Crystal Cathodes

Consequently, the decoupled lattice structurally relaxes in situ to form a highly reactive layered NiOOH intermediate. This profound electronic reconfiguration drastically alleviates the electrostatic barrier for rapid Li+ insertion, enabling complete phase reconstruction while eliminating conventional reliance on high Li-salt concentration gradients. Moreover, the specific adsorption of free Cl− in the molten salt regulates isotropic crystal growth, thereby exposing abundant active facets that accelerate Li+ migration.

The developed one-pot, dual-temperature-zone, bifunctional molten-salt strategy regenerates spent single-crystal Li1−xNi0.6Co0.1Mn0.3O2 into submicron, pillow-like single crystals. Benefiting from this unique architecture, the regenerated cathode delivers a high reversible capacity (177.7 mAh g−1) and exceptional rate capability (121.1 mAh g−1 at 10C, with 84.1% retention after 100 cycles), outperforming commercial counterparts.

This study simultaneously achieves direct regeneration and morphological engineering of spent materials, providing a commercially viable, closed-loop recycling strategy for degraded single-crystal cathodes.