Recycling of mixed lithium-ion battery cathode materials with spent lead-acid battery electrolyte with the assistance of thermodynamic simulations

Abstract

Based on the concept of recycling waste with waste, the mixed cathode materials of spent lithium-ion batteries were recycled with waste electrolyte from spent lead–acid batteries. With the assistance of thermodynamic simulations, the optimized recycling path of the mixed cathode materials was proposed and tested. A higher overall recycling ratio of valuable metals, that is, 94.9% of lithium, 94.5% of cobalt, 94.4% of nickel, and 95.5% of manganese, was achieved by replacing the oxalates/carbonates used in the precipitation process with sulfides and reducing the solubility of lithium carbonate in the lithium precipitation step at room temperature with ethanol. A higher ethanol-to-water ratio yielded a higher precipitation ratio of lithium until the ratio reached 5:1. High-purity lithium carbonate and cobalt (99.9%) were recovered as nanoparticles and nanoribbons, respectively, through precipitation using carbon dioxide in a solution with a 4:1 ethanol-to-water ratio and electrodeposition at E = −0.4 V in a traditional three-electrode system. Furthermore, the poisonous heavy metal (lead) was separated and stabilized as lead sulfide.