Gas-solid reaction-based selective lithium leaching strategy for efficient LiFePO4 recycling
Kyoung Sun Kim, Min Ku Jeon, Sung Wook Kim, Hyunkyung Choi, Young Rang Uhm, Sooyeon Hwang, Seokjae Hong, Dongju Lee, Seungho Yu, Hyungsub Kim
Abstract
• Cl 2 gas was used for selective lithium leaching to recycle LiFePO 4 batteries. • 99.8 % lithium leaching efficiency was achieved in just 10 min at 200 °C. • LiCl solution after leaching was recycled into Li 2 CO 3 . • Lithium-leached FePO 4 was regenerated into LiFePO 4 using solid state synthesis. • The gas–solid reaction efficiently reduced the generation of acidic wastewater. As the electric-vehicle market continues to expand, LiFePO 4 (LFP) batteries, valued for their intrinsic safety and cost-effectiveness, are being increasingly utilized. However, this widespread adoption highlights the urgent need for innovative and environmentally friendly recycling methods for spent LFP batteries due to their relatively low material value and the environmental challenges associated with traditional recycling processes. In this study, we present a novel selective lithium leaching technique that involves a gas–solid reaction with chlorine gas. This method achieves a remarkable leaching efficiency of 99.8 % and a selectivity of 98.8 % at 200 °C within just 10 min, without generating acidic wastewater. The resulting LiCl solution was successfully converted into Li 2 CO 3 with an excellent purity of 99.5 %, while producing NaCl solution as the only byproduct. Notably, the olivine structure of the LFP was preserved as FePO 4 after lithium leaching. The regenerated LFP demonstrated excellent performance, retaining 94.1 % of its capacity after 150 cycles, while the lithium-leached FePO 4 delivered a reversible capacity exceeding 150 mAh/g. This approach not only enhances the efficiency of LFP recycling but also paves the way for more sustainable battery technologies.