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The recycling of spent lithium-ion batteries (LIBs) is an effectual strategy for mitigating environmental and resource crises. Lithium iron phosphate batteries, renowned for their unique safety and stability, are widely utilized in energy storage systems and electric vehicles, consequently resulting in a growing number of spent LIBs. Herein, a one-pot mechanochemical process that integrates the recycling and preparation of LiFePO4 is proposed to drive the rapid regeneration of spent LiFePO4. Benefiting from the inherent characteristics of the input material, more than 98% of Li is selectively released, while less than 1.5% of Fe is leached without any impurity output. To this end, these reclaimed precursors in a ball mill can be directly re-used for the regeneration of LiFePO4 with an appropriate lithium source addition, eliminating the need to recover LiFePO4 with various degrees of lithium deficiency. As expected, the regenerated LiFePO4 delivers a discharge specific capacity of 143 mA h g−1 without negligible capacity fading after 250 cycles at 1 C, featuring significantly improved rate capability and long-term cycling stability. Designed with sustainable, integrated, and close-loop operation routes, this process pioneers a novel strategy to scale up the direct recycling for the LiFePO4 cathode. [ABSTRACT FROM AUTHOR]

The recycling of spent lithium-ion batteries (LIBs) is a crucial issue that has engaged extensive attention worldwide, along with the rapidly increasing usage of lithium-ion batteries. State-of-art recycling approaches, in terms of chemical leaching, have imperfections such as excessive chemical consumption, tedious recycling procedure and aggravated secondary pollution. In this research, a green and closed-loop route for the recycling of spent LiFePO4 involving oxidation leaching is demonstrated. By properly adjusting or controlling the leaching parameters, the leaching efficiency of lithium is up to 97.6% with the introduction of hydrogen peroxide, which is facilitated to achieve the transformed high-purity lithium carbonate and iron phosphate. The oxidation reaction mechanisms are clarified through thermodynamic and kinetic analyses, which identified that the oxidation leaching reaction is co-controlled by the internal diffusion and chemical reaction. Consequently, LiFePO4 cathode materials are regenerated by utilizing the obtained raw materials, as expected, which deliver superior cycling stability with less than 1% of capacity loss after 300 cycles and excellent rate performances. This research embodies the possibility of efficient recycling of LiFePO4 from spent lithium-ion batteries based on the principles of green chemistry that is possibly committed to the sustainability of the lithium-ion battery industry. [ABSTRACT FROM AUTHOR]