The tremendous consumption of lithium-ion batteries (LIBs) raises concern about sustainable resources especially for the valuable metals. Recycling valuable metals from spent LIBs is expected to meet the demand growth of LIBs. Herein, a novel approach combined with oxalic acid leaching, calcination relithiation, and annealing is proposed to regenerate spent LiNi0.5Co0.2Mn0.3O2 (NCM523) cathodes. This approach can reduce the recycling cost, accompanied with small energy consumption. Moreover, almost 98% of the valuable metals (Ni, Co, Mn) can be directly regenerated. The regenerated NCM523 cathode exhibits an initial capacity of 146.1 mAh g–1, with ∼85% capacity retention after 100 cycles. This work not only provides an efficient and simple method for recycling spent cathodes but also gives a new perspective of sustainable manufacturing of energy materials.

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