High-Yield One-Pot Recovery and Characterization of Nanostructured Cobalt Oxalate from Spent Lithium-Ion Batteries and Successive Re-Synthesis of LiCoO2

Abstract

A complete recycling process for the cathode material of spent lithium-ion batteries is demonstrated with a simple two-step process comprised of one-pot cobalt recovery to nanostructured materials and single step synthesis of LiCoO2. For the facile and efficient recovery of cobalt, we employ malic acid as a leaching agent and oxalic acid as a precipitating agent, resulting in nanostructured cobalt oxalate. X-ray diffraction and Fourier transform infrared spectroscopy (FT-IR) analysis clearly show that cobalt species are simultaneously leached and precipitated as cobalt oxalate with a high yield of 99.28%, and this material can then be used as a reactant for the synthesis of LiCoO2 for use as a cathode material. In addition to its advantages in simplifying the process, the proposed method allows for not only enhancing the efficiency of cobalt recovery, but also enabling reaction without a reducing agent, H2O2. Through successive single-step reaction of the obtained cobalt oxalate without any purification process, LiCoO2 is also successfully synthesized. The effect of the annealing temperature during synthesis on the nanostructure and charge–discharge properties is also investigated. Half-cell tests with recycled LiCoO2 exhibit a high discharge capacity (131 mA·h·g−1) and 93% charge–discharge efficiency.

Keywords

• cobalt recovery
• nanostructured cobalt oxalate
• spent Li-ion batteries
• one-pot process
• lithium cobalt oxide