Organics removal combined with in situ thermal-reduction for enhancing the liberation and metallurgy efficiency of LiCoO2 derived from spent lithium-ion batteries

Abstract

Liberation and reduction of cathode material are the necessary procedures for improving the recycling efficiency of cathode material derived from spent lithium-ion batteries. In this research work, a pyrolysis technology was utilized to remove the organic binder and enhance liberation of electrode materials. At the same time, pyrolysis treatment can facilitate the thermal-reduction of Co3+ in LiCoO2 to Co2+ with surface organics, which lays a foundation for the subsequent reductant-free acid leaching. Results indicate that the crystal structure of pure LiCoO2 is not changed at a pyrolysis temperature of 600 °C, but LiCoO2 transforms to CoO, Li2CO3, LiF, and Li2O under the reduction action of HF, pyrolytic carbon, and additive carbon black. Water-impact crushing is synchronized with water-leaching to separate electrode materials from aluminum foil and recover Li element. Afterwards, reductant-free acid leaching technology can be utilized to recycle Li and Co from spent LiCoO2 batteries. Recovery efficiency of Li element in water-leaching process was up to 92.17% while the remaining 7.83% of Li and all Co elements were recovered during reductant-free acid leaching process. Based on the foundation analysis, the green chemical process for recovering valuable metals from spent lithium-ion batteries was proposed.