Recycling for Recovery of Critical Metals from LiCoO2 Cathode Material Through Methanesulfonic Acid‑Citric Acid Organic Leaching System - Mining, Metallurgy & Exploration (2023)

Growing demand for valuable battery materials and environmental issues from battery disposal make the recycling of spent lithium-ion batteries (LIBs) essential. Specifically, the green approaches using organic reagents have garnered many attentions for battery recycling. In this study, a synergetic organic leaching system using methanesulfonic acid (MSA) of strong organic acid and citric acid (CA) with good chelating ability was investigated to extract valuable metals from LiCoO2. Hydrogen peroxide was used as a reducing agent to enhance leaching kinetics. Cobalt extraction of 98% and lithium extraction of 97 % were achieved in the optimized condition; 2.4M MSA, 1.6M CA, 1.0 vol% H2O2, S/L ratio 80 g/L, 85 °C, and 1 h. The optimal leaching condition of the MSA-CA mixed leaching system exhibited good applicability to various cathode scraps, such as LiCoO2, LiNixMnyCo1- x-yO2, and LiNixCoyO2. The dissolved Co and Li ions in the MSA-CA leachate were selectively recovered with high recovery efficiencies of 99 % and 97 % as Co3O4 and Li3PO4, respectively. The recovered Co3O4 and Li3PO4 were utilized to regenerate cathode materials. LiCoO2 and LiFePO4 were also synthesized through a solid-state reaction and hydrothermal method. The recycling process based on the MSA-CA-H2O2 synergetic leaching system was proposed, and it might be applied as a green and economical organic leaching system for the recycling of various types of spent LIBs.