The rapid growth of electronic devices, electric vehicles, and mobile energy storage has produced large quantities of spent batteries, leading to significant environmental issues and a shortage of lithium resources. Recycling spent batteries has become urgent to protect the environment. The key to treating spent lithium-ion batteries is to implement green and efficient regeneration. This study proposes a recycling method for the direct regeneration of spent lithium iron phosphate (LFP) batteries using hydrothermal reduction. Ascorbic acid (AA) was used as a low-cost and environmentally friendly reductant to reduce Fe3+ in spent LiFePO4. We also investigated the role of AA in the hydrothermal process and its effects on the electrochemical properties of the regenerated LiFePO4 cathode material (AA-SR-LFP). The results showed that the hydrothermal reduction direct regeneration method successfully produced AA-SR-LFP with good crystallinity and electrochemical properties. AA-SR-LFP exhibited excellent electrochemical properties, with an initial discharge specific capacity of 144.4 mAh g−1 at 1 C and a capacity retention rate of 98.6% after 100 cycles. In summary, the hydrothermal reduction direct regeneration method effectively repairs the defects in the chemical composition and crystal structure of spent LiFePO4. It can be regarded as a green and effective regeneration approach for spent LiFePO4 cathode materials.
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