Two-step leaching of spent lithium-ion batteries and effective regeneration of critical metals and graphitic carbon employing hexuronic acid

Abstract

Recovering precious metal ions like Co, Li, Mn, and Ni from discarded lithium-ion batteries (LIBs) has significant environmental and economic benefits. Also, graphite will be in high demand in the coming years due to the development of LIBs for use in electric vehicles (EVs) and the need for it for electrodes in a variety of energy storage devices. However, it has been overlooked during the recycling of used LIBs, which resulted in resource waste and environmental pollution. In this work, a comprehensive and environmentally friendly approach for recycling critical metals as well as graphitic carbon from discarded LIBs was proposed. To optimize the leaching process, various leaching parameters were investigated by employing hexuronic acid or ascorbic acid. The feed sample was analyzed using XRD, SEM-EDS, and a Laser Scattering Particle Size Distribution Analyzer to determine the phases, morphology, and particle size. 100% of Li and 99.5% of Co were leached at the optimum conditions of 0.8 mol L⁻¹ ascorbic acid, a particle size of −25 μm, 70 °C, 60 min of leaching time, and 50 g L⁻¹ of S/L ratio. A detailed study of the leaching kinetics was carried out. The leaching process was found to be well-fitted with the surface chemical reaction model based on the findings of temperature, acid concentration, and particle size variations. To obtain pure graphitic carbon after the initial leaching, the leached residue was subjected to further leaching with various acids (HCl, H₂SO₄, and HNO₃). The Raman spectra, XRD, TGA, and SEM-EDS analysis of the leached residues following the two-step leaching process were examined to exemplify the quality of the graphitic carbon.