Selective Lithium Recovery via Stepwise Transition Metal Crystallization in a Natural Deep Eutectic Solvent
Date
2025
Authors
Wang, J.
Yuwono, J.
Wang, Y.
Lyu, Y.
Liu, S.
Hall, T.
Zeng, R.
Mao, J.
Guo, Z.
Editors
Advisors
Journal Title
Journal ISSN
Volume Title
Type:
Journal article
Citation
Advanced Science, 2025; e14509-1-e14509-12
Statement of Responsibility
Jingxiu Wang, Jodie Yuwono, Yan Wang, Yanqiu Lyu, Sailin Liu, Tony Hall, Rong Zeng, Jianfeng Mao, and Zaiping Guo
Conference Name
Abstract
The global shift toward electric vehicles is driving unprecedented demand for lithium-ion batteries, underscoring the urgent need for sustainable lithium (Li) recycling technologies. Deep eutectic solvents (DESs) have emerged as promising green alternatives to conventional leaching agents, yet challenges persist in preferential Li selectivity and process scalability. Here, a natural DES composed of choline chloride, lactic acid, and ascorbic acid (1ChCl-10LA-VC) is designed to overcome these limitations. In this system, LA provides high acidity, VC serves as a mild reductant, and ChCl promotes selective complexation and controlled precipitation of transition metals (TMs: Co, Ni, Mn, Fe). This synergistic formulation enables a stepwise separation mechanism: Li+ remains solubilized, while TMs undergo rapid reduction, complexation, hydrolysis, and eventual crystallization within one hour. The method is broadly effective across various cathode chemistries —including LiCoO2, LiNiO2, LiMn2O4, LiFePO4, and NCMs (NCM 111, NCM 523, NCM811)—and demonstrates exceptional selectivity, particularly for high-Ni cathodes. Co-dissolved Mn impurities are effectively removed via antisolvent crystallization, enabling high-purity Li2CO3 recovery. When applied to black mass, the method achieves >96% Li leaching, >94% overall recovery, and excellent DES recyclability over four cycles. Furthermore, scale-up to gram-scale in a 2-liter glass reactor confirmed process robustness and industrial feasibility.
School/Discipline
Dissertation Note
Provenance
Description
Available online 12 September 2025
Access Status
Rights
© 2025 The Author(s). Advanced Science published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.