Ambient-pressure relithiation of spent LiFePO4 using alkaline solutions enables direct regeneration of lithium-ion battery cathodes

Abstract

Lithium iron phosphate (LiFePO₄) is widely recognized for its cost-effectiveness in manufacturing and high safety during usage, making it a favored choice for electric vehicles and energy storage stations. Nevertheless, the development of efficient and low-cost recycling methods has emerged as an urgent priority due to the economic and environmental benefits associated with it. Here, the present study successfully demonstrates the ambient-pressure relithiation of lithium-deficient LiFePO₄ particles in alkaline solutions. Specifically, the incorporation of reductive sodium nitrite with lower redox potential in the alkaline environment spontaneously repairs the compositional and structural defects, facilitating effective lithium-ion insertion back into the original site. Consequently, the short-term annealing step promotes the formation of more thermodynamically stable particles, resulting in enhanced cycling stability and rate capability comparable to that of the pristine materials. The regenerated LiFePO₄ cathode exhibits improved electrochemical performance in terms of long-term cyclability, high-rate properties and reduced polarization (a high retention of 93 % after 1000 cycles at 5C). The findings of this study suggest the significant potential for utilizing various reductants in an alkaline environment to achieve ambient-pressure relithiation, thereby facilitating the recycling and remanufacturing of spent lithium-ion cathode materials.