Maryanne Hoffmann Cardoso

The rapid increase in electric vehicles has increased the generation of spent lithium-ion batteries (LIBs) and the need for efficient lithium recovery technologies. This study compared two distinct sulfation roasting routes, using sodium sulfate (Na₂SO₄) at 750 °C and sulfuric acid (H₂SO₄) at 550 °C, applied to black mass derived from lithium iron phosphate (LFP) and lithium nickel manganese cobalt oxide (NCM) batteries. Metal extraction efficiencies were determined by inductively coupled plasma optical emission spectrometry, while reaction products were identified by X-ray diffraction analysis. Sulfation roasting using Na₂SO₄ resulted in low lithium recovery for both materials, with maximum extractions of 5.7% for LFP and 24.5% for NCM. In contrast, H₂SO₄-assisted roasting achieved high lithium recovery from NCM black mass, reaching 90.8%, 91.5%, and 88.5% at 45, 90, and 180 min at 550 °C, respectively, with lithium predominantly converted into water-soluble lithium sulfate. Lithium extraction from LFP black mass remained below 13% under all conditions. Statistical analysis confirmed that lithium recovery at 45 min was equivalent to longer residence times, while prolonged roasting increased manganese coextraction and altered cobalt and nickel behavior. Overall, sulfuric acid-assisted sulfation roasting is an efficient and energy-favorable route for lithium recovery from NCM black mass, whereas sulfation roasting is unsuitable for LFP materials, under the tested conditions. The results highlight the importance of cathode chemistry segregation and demonstrate the feasibility of reducing processing time without compromising lithium recovery.

Recent increases in the demand for automotive lithium-ion batteries (LIBs) have led to higher needs for critical materials like lithium, cobalt, nickel, and graphite. Consequently, recovering materials from spent batteries has gained importance. This study aimed to (1) develop a mechanical pretreatment method for separating and concentrating materials from spent NCM₈₁₁ cells and (2) evaluate the economic, environmental, and shortage potentials of these fractions. The pretreatment involved grinding and granulometric separation, producing six particle-size fractions. The main novelty of the study was the assessment to identify the particle size fractions which are priorities for recycling for decision-making by recycling companies, optimizing their resources and efforts. Analysis showed that the finest fraction (n < 0.5 mm) had 85% of lithium, 77.4% of cobalt, 75.1% of manganese, and 68.5% of nickel. This fraction represented 40.4% of the processed mass and had the highest economic value (USD 3669/ton NCM cell). This fraction was also prioritized for recycling due to its superior environmental impact (103,788 kg CO₂-eq/ton NCM cell) and scarcity considerations. Furthermore, the black mass of NCM was the priority for recycling and had greater economic, environmental, and supply risk potential than the black mass of LFP cells.

Recent increases in the demand for automotive lithium-ion batteries (LIBs) have led to higher needs for critical materials like lithium, cobalt, nickel, and graphite. Consequently, recovering materials from spent batteries has gained importance. This study aimed to (1) develop a mechanical pre-treatment method for separating and concentrating materials from spent NCM622 cells, and (2) evaluate the economic, environmental, and scarcity potentials of these fractions. The pre-treatment involved grinding and granulometric separation, producing six particle-size fractions. Analysis showed that the finest fraction (n < 0.5 mm) had 85% of lithium, 77.4% of cobalt, 75.1% of manganese, and 68.5% of nickel. This fraction represented 40.4% of the processed mass and had the highest economic value (USD 3,669/ton NCM cell). This fraction was also prioritized for recycling due to its superior environmental and scarcity considerations.