Efficient separation and stepwise recovery of lithium and transition metals from spent ternary lithium-ion batteries powders

Release time:2026-04-10

Impact Factor:13.2

DOI number:10.1016/j.cej.2025.16732

Journal:CHEMICAL ENGINEERING JOURNAL

Key Words:Spent lithium-ion batteries； Black powders recycling； Reductive-sulfation roasting； Lithium selective extraction； Lithium phosphate； Ni-Co-Mn acid leaching

Abstract:A process based on carbon-sulfur collaborative roasting was developed for the gradual separation and efficient recovery of Li and transition metals (TMs) from spent ternary lithium-ion batteries (LIBs) powders. The phase transformation behavior of valuable metals during roasting were elucidated through thermodynamic simulations and multiscale product characterization. Under optimized roasting conditions (600 degrees C, n(H2SO4),n(Li) = 0.5, 120 min), similar to 90 % Li and similar to 16 % Mn were converted into water-soluble Li2SO4 and MnSO4, while residual TMs formed acid-soluble oxides (NiO)(0.75)(MnO)(0.25) and CoO. LiF was not converted into water-soluble Li salts and remained in the water-leaching residue. Subsequent acid leaching (2 mol/L H2SO4, 60 degrees C, 120 min, 5 mL/g) achieved similar to 96 % Mn and similar to 100 % Li, Ni and Co recovery. A novel extractant, p-tert-octyl phenyl phosphate (PTOPP), was employed to selectively extract >99 % Mn2+ and deeply remove impurities (Al3+, Cu2+) from the water-leaching solution. PTOPP exhibited superior extraction performance compared to P204 under non-saponification conditions. Finally, spherical Li3PO4 particles with 99.94 % purity was precipitated from the purified raffinate (alpha(Na3PO4) = 1.1, 90 degrees C, 60 min). This process provides a promising and sustainable strategy for the recycling of spent ternary LIBs.

Indexed by:Journal paper

Document Code:167321

Discipline:Engineering

First-Level Discipline:Metallurgical Engineering

Document Type:J

Volume:522

Translation or Not:no

Date of Publication:2025-10-15

Included Journals:SCI、EI、SSCI