Based on a combination of spontaneous lithium migration and targeted electrically-driven lithiation, a two-step resting-output current process was conducted to directly regenerate retired LiFePO4 cathode, which can reduce energy consumption and environmental pollution.

As lithium-ion batteries (LIBs) are undergoing unprecedented development in electric vehicles (EVs) and renewable grids, recycling spent battery disposal is becoming the dominating issue considering the urgent demand for sustainable resources and eco-friendly development. However, existing recovery methods for spent LIBs still suffer from complex processes and low processing efficiency. Herein, an effective pyroprocessing-based strategy was proposed to recycle spent lithium iron phosphate (LFP) materials, featuring full element regeneration and conversion of high-value products. Specifically, over 99% Li was extracted and converted into high purity lithium carbonate (>99%), while Fe and P were further converted into value-added Fe2P2O7 and Na4P2O7, respectively. Due to the benefits of high efficiency of metal extraction and the reuse of all valuable elements, the pyroprocessing-based strategy potentially generates the profit of 1.44 $ kg–1 of LFP batteries, over three times more than that of the conventional hydrometallurgical process, while the discharges of wastewater and residue are reduced by 66.3 and 93.9%, respectively. This study provides a new pyroprocessing-based approach to the green recovery of all elements of LFP materials in spent LFP batteries.

Lithium-ion batteries (LIBs) account for the majority of energy storage devices due to their long service life, high energy density, environmentally friendly, and other characteristics. Although the cathode materials of LIB led by LiFePO4 (LFP), LiCoO2 (LCO), and LiNixCoyMn1-x-yO2 (NCM) occupy the majority of the market share at present, the demand of LiMn2O4 (LMO) cathode battery is also increasing year by year in recent years. With the rising price of various raw materials of LIBs and the need of environmental protection, the efficient recycling of spent LIBs has become a hot research topic. At present, the recycling of spent LIBs mainly focuses on LFP, LCO, and NCM batteries. However, with the continuous improvement of people’s safety of LIBs, LiMnxFe1-xPO4 (LMFP) batteries show better potential, which also improves the recycling value of LMO batteries. Therefore, this paper reviews current methods of spent LMO recovery, focusing on the characteristics of the recovery and separation process, which can serve as a reference for subsequent research on LMO recovery, increasing environmentally friendly recovery routes. Finally, the future development direction of LIBs recycling is prospected. Overall, this review is helpful to understand the current progress of LMO battery recycling.

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