Sustainable recovery of cobalt and lithium from lithium-ion battery cathode material by combining sulfate leachates and aqueous biphasic systems based on tetrabutylphosphonium-ionic liquids

• Published in: Separation and purification technology 2024-11, Vol.348, p.127707, Article 127707
• Main Authors: Mušović, Jasmina, Tekić, Danijela, Marić, Slađana, Jocić, Ana, Stanković, Dalibor, Dimitrijević, Aleksandra
• Format: Article
• Language: English
• Subjects: Aqueous biphasic system; Cathode material; Cobalt; Ionic liquid; Li-ion battery; Lithium; Metals recovery; Separation; Sustainable extraction; Tetrabutylphosphonium ILs
• ISSN: 1383-5866
• DOI: 10.1016/j.seppur.2024.127707

[Display omitted] •Novel [TBP]-ionic liquids with different anions were used for ABS formation in combination with ammonium-sulfate.•Partition studies showed that [TBP][DTPA]/(NH4)2SO4 ABS demonstrates the highest extraction efficiencies for Co, Ni, and Mn.•The optimized ABS was applied for the recovery of valuable metals from the cathode of the LCO battery from sulfate leachate.•Co and Li extraction and separation from the leaching solution of spent LIB was achieved.•A sustainable and efficient integrated extraction platform for separation and concentration of Co and Li from spent battery was proposed. The consistent expansion of the lithium-ion battery (LIB) market, coupled with their relatively brief lifespan, necessitates the development of efficient and sustainable LIB recycling strategies. Recycling is crucial not only for the recovery of critical metals like Co(II) and Li(I) from the cathode material as a secondary resource but also from an environmental perspective. This study explores the use of a series of aqueous biphasic systems (ABS) with synthesized tetrabutylphosphonium ionic liquids (ILs) and ammonium sulfate as extraction platforms for metals from LIB cathode. Firstly, liquid–liquid equilibrium phase diagrams for each ABS were established, and partitioning experiments were conducted to assess the Co(II), Ni(II), Mn(II), and Li(I) recovery efficiencies. We observed distinct partitioning behaviors for the metals, with tetrabutylphosphonium diethylenetriaminepentaacetate, [TBP][DTPA], showing recovery efficiencies exceeding 98% for Co(II), Ni(II), and Mn(II). At the same time, Li(I) was predominantly retained in the aqueous salt-rich phase. By fine-tuning ABS operational parameters such as pH, temperature, system composition, and phase ratio, we identified optimal conditions for extracting metals from the cathode material of lithium-cobalt-oxide (LCO) batteries using sulfate lixiviate. Introducing [TBP][DTPA] after the leaching process induced ABS, achieving remarkable recovery efficiency over 95% for Co(II) in the IL-rich phase, with all Li(I) remaining in the lower phase. Cobalt was subsequently extracted using oxalic acid to precipitate as Co-oxalate from concentrate, while Li(I) was isolated from the aqueous phase using ammonium carbonate. After the “cleaning” of the IL-rich phase, the [TBP][DTPA] was recovered and reused in four consecutive cycles, with small detected losses on the recovery efficiency of Co(II) and Li(I). Therefore, our