Priority Extraction of Li+ and Sequential Recovery of Divalent Metals from Retired LiNixCoyMn1–x–yO2 Batteries Using GIS Zeolite

Abstract

The shortage of lithium resources and the accumulation of retired batteries are strategic issues that need to be addressed urgently. Here, we propose an innovative and efficient strategy for the preferential extraction of Li⁺, followed by the sequential recovery of Mn²⁺ and Co²⁺, utilizing GIS zeolite from battery leachate. Li⁺ ions were preferentially exchanged, achieving a 95% recovery rate at 0 °C; subsequently, 94% of Mn²⁺ and 97% of Co²⁺ were recovered by increasing the temperature to 40 and 60 °C; meanwhile, 90% of Ni²⁺ remains in solution. The fastest kinetic rate of Li⁺ in GIS zeolite and its efficient extraction at low temperatures were verified through ion exchange processes; at higher temperatures, the adsorption capacity and selectivity of GIS zeolite for Co²⁺ and Mn²⁺ increased. We found the diffusion rate of Li⁺ in GIS zeolite to be over 2.5 times faster than that of Mn²⁺, Co²⁺, and Ni²⁺, which all have the same rate by molecular dynamics simulations. The ion exchange of Mn²⁺, Co²⁺, and Ni²⁺ was an endothermic reaction, with the ΔH⁰ and ΔG⁰ following the order Mn²⁺ < Co²⁺ < Ni²⁺ by thermodynamic calculations. The regeneration ability of GIS zeolite indicated its promising industrial application prospects.