Separation and Regeneration of LiNi_1/3Co_1/3Mn_1/3O₂ Materials from Spent Lithium-Ion Batteries: A Facile Process

Abstract

In this paper, a potential method for the closed-loop recovery and regeneration of cathode materials from spent lithiumion batteries (LIBs) is developed to greatly simplify the regeneration process, which successfully removes metal impurities from spent LIBs and synthesis of layered oxide Li-Ni 1/3 Co 1/3 Mn 1/3 O 2 materials. First, the valuable metals (Ni, Co, Mn, and Li) in spent LIB materials are transformed into watersoluble ions based on the synergy between DL-malic acid and glucose. Subsequently, the residual Fe impurities are successfully decreased from the leaching solution by oxidation-precipitation. Prior to the synthesis process, valuable metal ions are immediately precipitated using oxalic acid as a precipitant from the leaching solution into Ni 1/3 Co 1/3 Mn 1/3 C 2 O 4 •nH 2 O with extremely uniform size particles. Furthermore, the LiNi 1/3 Co 1/3 Mn 1/3 O 2 materials with an excellent crystal structure are successfully synthesized by adding Li 2 CO 3 as the lithium source after roasting at 500 °C for 4 h and then at 950 °C for 12 h. The regenerated LiNi 1/3 Co 1/3 Mn 1/3 O 2 materials demonstrate reliable electrochemical performance. This work clarifies a potential method for the closed-loop recovery resource sustainability of spent LIB materials.