Streamlined Precise Delamination and Structural Restoration of Spent LiFePO ₄ Cathode Materials

ABSTRACT Efficient recycling of spent lithium‐ion battery cathodes remains both critical and challenging. Achieving high‐purity separation hinges on the precise delamination of active materials from current collectors, which directly influences downstream recycling efficiency. Guided by density functional theory, we develop a versatile strategy that enables rapid, high‐efficiency delamination by first deactivating the binder, followed by structural restoration of the separated LiFePO 4 (LFP) through electron activation using a designed bi‐phase electron‐rich reagent (BER). Experimentally, the approach attains > 99% separation efficiency for LFP and multiple electrode chemistries within minutes, while fully preserving the structural integrity of both active materials and metal foils. The phase I BER (BER‐I) maintains stable performance over more than ten cycles after simple zeolite purification, showing negligible changes in viscosity or chemical composition. Notably, BER‐I can be converted in situ into a repairing phase II BER that replenishes lithium loss and heals structural defects, enabling direct regeneration. The regenerated LFP delivers a specific capacity of 154.7 mAh g −1 at 0.1 C, while its 0.5 Ah pouch cell maintains 91.1% capacity after 400 cycles at 1 C. Techno‐economic analysis further reveals that this integrated separation‐regeneration route offers a more sustainable and economically advantageous solution than existing recycling processes.