Owing to scarcity of Li resources and environmental burden, efficient resource recycling ways of spent lithium iron phosphate batteries (LFPs) have attracted extensive attention. However, the existing recycling strategy still has obstacles due to low efficiency of Li recovery and high consumption of acid and base. In this study, a novel strategy was reported to regenerate lithium iron phosphate through a combination of recovering high-purity heterosite FePO4 and reinjecting Li+ ions via a facile hydrothermal route. The findings show that crystal phase of recovered FePO4 was heterosite structure, which indicates that the original olivine crystal phase of spent LFPs is maintained through the proposed recovery strategy. As a result, the purity of obtained FePO4 reach 95.97%, and the embedding rate of lithium into the recovered FePO4 achieves to 99.98% with a low iron dissolution rate of 1.264%. Furthermore, the reassembled LiFePO4 displayed an initial discharge capacity of 154.32 mAh·g−1 at 0.1C, approaching to the theoretical specific capacity of lithium iron phosphate (170 mAh·g−1) and maintained a capacity retention of 95.39% after 200 cycles at 1C, demonstrating excellent electrochemical performance. This work extremely cut down the recovery and regeneration process of spent LFPs batteries, indicating significant decrease of energy consumption, which provides a new process for large-scale recovery of spent LFP batteries.
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