Streamlined Precise Delamination and Structural Restoration of Spent LiFePO₄ Cathode Materials

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 LiFePO₄ (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. © 2026 Wiley-VCH GmbH.