Removal of polyvinylidene fluoride binder and other organics for enhancing the leaching efficiency of lithium and cobalt from black mass

The agglomeration and encapsulation of recoverable materials of interest (e.g. metals and graphite) as a result of the presence of polyvinylidene fluoride (PVDF) in spent lithium-ion batteries (LIBs) with mixed chemistries (black mass) lower the extraction efficiency of metals. In this study, organic solvents and alkaline solutions were used as non-toxic reagents to investigate the removal of a PVDF binder from a black mass. The results demonstrated that 33.1%, 31.4%, and 31.4% of the PVDF were removed using dimethylformamide (DMF), dimethylacetamide (DMAc), and dimethyl sulfoxide (DMSO) at 150, 160, and 180 °C, respectively. Under these conditions, the peel-off efficiencies for DMF, DMAc, and DMSO were 92.9%, 85.3%, and approximately 92.9%, respectively. Using tetrabutylammonium bromide (TBAB) as a catalyst and 5 M sodium hydroxide (NaOH) at room temperature (RT- 21 °C-23 °C), 50.3% of PVDF and other organic compounds were eliminated. The removal efficiency was enhanced to approximately 60.5% when the temperature was raised to 80 °C using NaOH. Using 5 M potassium hydroxide at RT in a TBAB-containing solution, ca. 32.8% removal efficiency was obtained; raising the temperature to 80 °C further enhanced the removal efficiency to almost 52.7%. The peel-off efficiency was 100% for both alkaline solutions. Lithium extraction increased from 47.2% to 78.7% following treatment with DMSO and to 90.1% following treatment with NaOH via leaching black mass (2 M sulfuric acid, solid-to-liquid ratio (S/L): 100 g L-1 at 50 °C, for 1 h without a reducing agent) before and after removal of the PVDF binder. Cobalt's recovery went from 28.5% to 61.3% with DMSO treatment to 74.4% with NaOH treatment.