Direct Regeneration of LFP Cathode Material from Spent Li-Ion Batteries via Aqueous Relithiation

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Lithium iron phosphate (LFP) is a commonly used cathode material in lithium-ion batteries, particularly for electric vehicle (EV) battery energy storage systems. To support sustainability and the principles of a circular economy, recycling spent LFP batteries is essential. This study focuses on the direct regeneration of spent LFP cathode material using an aqueous relithiation method conducted at low temperature, followed by post-annealing. The waste precursors and regenerated LFP were fully characterized for its structural, morphological, and compositional properties. Fourier-transform infrared (FTIR) analysis confirmed the presence of additive carbon and electrolyte residues in the spent LFP. XRD analysis revealed that certain components of the LFP structure in the as received spent cathode material decomposed, as evidenced by the presence of impurity peaks due to FePO4 and P2O5, which disappeared after relithiation. The lattice parameter values (a=4.6897 Å and c=10.3211 Å) of the regenerated LFP were also found to be close to the theoretical (a=4.6925 Å and c=10.3253 Å), suggesting successful structure repair after regeneration. SEM indicated that regenerated LFP particles appeared to be more well-dispersed and finer than spent LFP particles. EDS mapping revealed a relatively homogeneous elemental distrbution of the major identified elements. ICP analysis further confirmed the successful restoration of Li content. The composition of the spent cathode, initially Li0.85FePO4, transformed to Li1.03FePO4 after regeneration, corresponding to an increase in Li content from the as-received 3.75 to 4.53 wt% Li after relithiation.

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March 2026

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