Selective Extraction of Lithium from Li Batteries by Leaching the Black Mass in Oxalic Acid

In this work, a method for leaching black mass from spent Li batteries using oxalic acid was developed and experimentally verified with the objective of selectively separating lithium and cobalt. Oxalic acid proved to be an efficient and selective leaching agent. Under 1 M C2H2O4, 120 min, L:S = 20, 80 °C and 300 rpm, a lithium yield of 90% was achieved, while cobalt dissolution remained low at 1.57%. Subsequently, cobalt spontaneously precipitated from the leachate within several hours, and the solid phase was fully separated after 24 h. The leachate contained minor amounts of accompanying metals, with dissolution yields of 0.5% Mn, 8% Fe and 1.4% Cu. These impurities were removed from the leachate by controlled pH adjustment using NaOH at ambient temperature and 450 rpm, with complete precipitation at pH 12. This procedure generated a purified lithium-rich leachate, which was converted into lithium oxalate by crystallisation at 105 °C. Subsequent calcination of the resulting solid at 450 °C for 30 min produced Li2CO3 with a purity of 91%. Based on the experimental findings, a conceptual technological process for selective lithium leaching using oxalic acid was proposed, demonstrating the potential of this method for sustainable lithium recovery.