The ecologically friendly and cost-effective recycling process still encounters significant obstacles, despite the significant importance of regenerating spent LiFePO4 (LFP) cathode materials in addressing resource shortages and environmental pollution. Herein, we proposed a new strategy to synthesize newly high-performance nitrogen-doped carbon/graphene@LiFePO4 (N-DC/G@LFP) cathode materials by utilizing the spent LFP cathode material as raw materials. The regeneration strategy was designed and performed in an alkaline solution, after repeated freezing and thawing, spray-drying, and subsequently thermal annealing under an Ar atmosphere process. Benefiting from the synergistic effects of the tight contact between LiFePO4 and high conductivity nitrogen-doped carbon and graphene network, the refabricated N-DC/G@LFP cathodes deliver 124.8 mAh g-1 of excellent reversible discharge capacities at 2 C, 117.5 mAh g-1 at 5 C, and 149.7 mAh g-1 at 0.2 C current rate. Furthermore, a 94.2% high capacity retention ratio was observed over 500 cycles at 0.2 C. This regeneration approach offers a novel insight into the transformation from spent LFP cathode to new cathode materials with efficient reutilization, which takes full advantage of the valuable components within the spent cathodes, to acquire the win-win situation of environment protection and sustainable development of the LIBs industry.
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