Sustainable waste management & valorisation within the circular economy era: Closed-loop recycling of lithium iron phosphate cathodic powders via citric acid leaching

Lithium recovery from Lithium-ion batteries requires hydrometallurgy but up-to-date technologies aren’t economically viable for Lithium-Iron-Phosphate (LFP) batteries. Selective leaching (specifically targeting Lithium and based on mild organic acids and low temperatures) is attracting attention because of decreased environmental impacts compared to conventional hydrometallurgy. This study analysed the technical and economic performances of selective leaching with 6%vv. H2O2 and citric acid (0.25-1 M, 25 °C, 1 h, 70 g/l) compared with conventional leaching with an inorganic acid (H2SO4 1 M, 40 °C, 2 h, 50 g/l) and an organic acid (citric acid 1 M, 25 °C, 1 h, 70 g/l) to recycle end of life LFP cathodes. After conventional leaching, chemical precipitation allowed to recover in multiple steps Li, Fe and P salts, while selective leaching allowed to recover Fe and P, in the leaching residues and required chemical precipitation only for lithium recovery. Conventional leaching with 1 M acids achieved leaching efficiencies equal to 95 ± 2% for Li, 98 ± 8% for Fe, 96 ± 3% for P with sulfuric acid and 83 ± 0.8% for Li, 8 ± 1% for Fe, 12 ± 5% for P with citric acid. Decreasing citric acid’s concentration from 1 to 0.25 M didn’t substantially change leaching efficiency. Selective leaching with citric acid has higher recovery efficiency (82 ± 6% for Fe, 74 ± 8% for P, 29 ± 5% for Li) than conventional leaching with sulfuric acid (69 ± 15% for Fe, 70 ± 18% for P, and 21 ± 2% for Li). Also, impurities’ amounts were lower with citric acid (335 ± 19 mg/kg of S) than with sulfuric acid (8104 ± 2403 mg/kg of S). In overall, the operative costs associated to 0.25 M citric acid route (3.17€/kg) were lower compared to 1 M sulfuric acid (3.52€/kg). In conclusion, citric acid could be a viable option to lower LFP batteries’ recycling costs, and it should be further explored prioritizing Lithium recovery and purity of recovered materials.