Effective Recycling of the Whole Cathode in Spent Lithium Ion Batteries: From the Widely Used Oxides to High-Energy/Stable Phosphates

With the rapidly increasing use of lithium ion batteries (LIBs), the corresponding spent materials will eventually lead to severe environment pollution and resource waste if they cannot be recycled through a suitable way. Herein, a new and effective strategy is proposed to directly recycle the whole oxide cathode in the spent LIBs to prepare the next generation high-performance phosphate cathode materials for LIBs. In the present case, a high voltage/energy and long life LiFe0.6Mn0.4PO4/C (LFMP/C) composite has been prepared successfully by reusing the whole LiMn2O4 cathode as the main raw material. When used in LIBs, the LFMP/C delivers a high capacity of 141.3 mAh/g at 0.1 C and 104.9 mAh/g at a high rate of 10 C, and exhibits a long cycle life, e.g., 86.4% capacity retention over 400 cycles at 1 C. For the presently proposed reuse strategy, not only have all metallic elements on the cathodes of spent LIBs including Li and Mn been 100% recycled, but organic binder and conductive additive can also be directly employed as the precursor to construct conductive carbon network for performance enhancement. This strategy is highly green and universal, and can be easily extended to recycle other whole oxide cathodes, such as from the market-dominant LiCoO2 cathode to high-voltage LiCoPO4 material.