A sustainable revival process for defective LiFePO4 cathodes through the synergy of defect-targeted healing and in-situ construction of 3D-interconnected porous carbon networks.

The reutilization of spent cathode materials plays a key role in the sustainable development of Li-ion battery technology. However, current recycling approaches generally based on hydro-/pyrometallurgy fail to cater to Co-free cathodes (e.g., LiFePO, or LFP) owing to high consumption and secondary contamination. Here, a sustainable process is proposed for the revival of defective LFP cathodes through the synergy of defect-targeted healing and surface modification. Li deficiency and Fe oxidation of cathodes are precisely repaired by solution-based relithiation; meanwhile, 3D-interconnected porous carbon networks (3dC) are in-situ constructed with the intervention of salt template during annealing, which enhances the rate performance and electronic/ionic conductivity, by providing more convenient migration channels for Li ions and controlling carbon hybridization. Nitrogen is also doped via induction of urea to fabricate advanced nanohybrid rLFP@3dC-N. New cells using rLFP@3dC-N as cathode exhibit a reversible capacity of up to 169.74 and 141.79 mAh g at 0.1 and 1C, respectively, with an excellent retention rate of over 95.7% at 1C after 200 cycles. Impressively, a high capacity of 107.18 mAh g is retained at 5C. This novel concepts for Li replenishment and the construction of ion-transfer channels as well as conductive networks facilitate the regeneration of spent LFP and the optimization of its high-rate performance.