Efficient Removal of Fluorine from Leachate of Spent Lithium Iron Phosphate Calcine by Porous Zirconium-Based Adsorbent

During the recycling process of spent lithium-ion batteries (LIBs), there is a large number of fluoride ions in the leaching solution. These fluoride ions not only affect the quality of lithium products, but they also have adverse effects on the environment. Therefore, the efficient and deep removal of the characteristic pollutant fluoride ions is currently a hot topic in the field of recycling spent LIBs. In this study, a porous zirconium-based adsorbent was prepared and its adsorptive properties were characterized. Due to the excellent affinity between zirconium and fluorine, the zirconium-based adsorbent exhibited excellent adsorption performance in the leaching solution of spent lithium iron phosphate (SLFP) batteries. Under the optimal adsorption conditions, the adsorption capacity reached 113.78 mg/g, and it surpassed most commercial adsorbents. The zirconium-based adsorbent followed the Langmuir isotherm model for fluoride adsorption with correlation coefficients consistently exceeding 0.95, and exhibited pseudo-second-order kinetics, demonstrating goodness-of-fit values above 0.998. The negative Gibbs free energy change thermodynamically confirms the spontaneous nature of the adsorption process. The structure of the adsorbent before and after adsorption was characterized, and the adsorption mechanism was elaborated in detail. Furthermore, the influence of the coexistence of different anions on the adsorption of fluoride ions by zirconium-based adsorbent was studied in a real leaching solution from SLFP calcine. This study provides a feasible approach to deep defluoridation for leachate from spent LIBs, and has the advantages of simple operation and high adsorption capacity.