Holistic Recovery of Spent Lithium‐Ion Batteries by Flash Joule Heating
Shichen Xu, Justin Sharp, Qiming Liu, Jaeho Shin, Haoxin Ye, K. Yang, Shihui Chen, Karla Silva, Ralph Abdel Nour, Carter Kittrell, Haojie Zhu, Bowen Li, Khalil JeBailey, Carolyn Teng, Boris I. Yakobson, Yufeng Zhao, James M. Tour
Abstract
The rising demand for lithium-ion batteries (LIBs) highlights the urgent need for sustainable recycling technologies. Existing pyrometallurgy and hydrometallurgy methods can recover valuable metals but suffer from high energy costs and wastewater generation. Here, a selective flash Joule heating chlorination and oxidation (FJH-ClO) strategy is presented for the efficient separation of metals from spent batteries. In this process, cathode metals are first chlorinated for 60 s, after which the transition metal chlorides are oxidized to oxides, enabling lithium to be separated from transition metals due to their different aqueous solubility. This approach applies not only to the recovery of metals from lithium cobalt oxide (LCO), lithium iron phosphate (LFP), and lithium manganese iron phosphate (LMFP) cathode materials, but also to the anodic graphite, all from the black mass. The recovered graphite exhibits purity of ≈100% with a yield of 85%, Co at 99% purity and 97% yield, and Li at 99% purity with a 92% yield. Gram-scale experiments confirm the scalability of the method, maintaining high efficiency and selectivity. Life-cycle assessment and technoeconomic analysis reveal that the FJH-ClO process substantially reduces energy consumption, operation time, and reagent consumption, while lowering operating costs by up to 92%, compared to conventional approaches.