Direct regeneration and performance of spent LiFePO4 via a green efficient hydrothermal technique

With the quick development of electric vehicles and grid energy storage, the demand and production of lithium ion batteries (LIBs) are rapidly increasing, and the problem of lithium resource shortage becomes more and more serious. Both in terms of economic value and environmental protection, the recycling and regeneration of the spent lithium batteries is extremely urgent. Herein, a green and efficient hydrothermal technique for direct regeneration of spent lithium iron phosphate (LiFePO4 or LFP) was proposed. LFP loses the partial lithium during the long cycle and converts to FePO4 (FP), therefore, the replacement of the lost lithium is crucial for the regeneration of spent LFP. Herein, the effects of hydrothermal conditions such as reaction temperature, Li+ concentration and reducing agent concentration on the performance of product are systemically studied. Besides, it has been found that the control of hydrothermal condition is conductive to the supplement of Li and the enhancement of electrochemical performance of the product. Under hydrothermal conditions of 200 °C for 3 h, the regenerated LFP shows the optimal electrochemical performance of 165.9, 151.93, 145.92, 133.11 and 114.96 mAh g−1 at 0.1, 0.5, 1, 2, and 5 C, respectively. In addition, the capacity retention is as high as 99.1% after 200 cycles at 1 C. Therefore, this work provides a new idea for the direct regeneration of spent LFP cathode materials.