Cradle-to-cradle recycling of spent NMC batteries with emphasis on novel Co2+/Ni2+ separation from HCl leached solution and synthesis of new ternary precursor
- Authors
- Ilyas, Sadia; Srivastava, Rajiv Ranjan; Kim, Hyunjung
- Issue Date
- Feb-2023
- Publisher
- Institution of Chemical Engineers
- Keywords
- Cathode precursor synthesis; Critical raw materials; Resources recycling; Spent Li-ion batteries
- Citation
- Process Safety and Environmental Protection, v.170, pp.584 - 595
- Indexed
- SCOPUS
- Journal Title
- Process Safety and Environmental Protection
- Volume
- 170
- Start Page
- 584
- End Page
- 595
- URI
- https://scholarworks.bwise.kr/hanyang/handle/2021.sw.hanyang/182167
- DOI
- 10.1016/j.psep.2022.12.045
- ISSN
- 0957-5820
- Abstract
- Herein, a cradle-to-cradle recycling of post-consumer NMC batteries has been demonstrated with a focused separation of cobalt over nickel by applying the ionic liquid, trihexyl(tetradecyl)phosphonium bis-2,4,4-(trimethylpentyl)phosphinate. At the optimized condition of: 0.8 mol·L−1 ionic liquid, 3.0 mol·L−1 Cl− ions, equilibrium pH value ∼5.0, and organic-to-aqueous ratio 2/3, > 99% cobalt was extracted in the organic phase with a separation factor of 1097. Approximately 99% cobalt from the loaded organic was stripped back in 2.0 mol·L−1 HCl solution, yielding high-pure CoCl2·xH2O crystals after crystallizing the stripped solution. Subsequently, ∼99% of nickel from the Co-depleted raffinate was extracted over lithium using 0.32 mol·L−1 acetophenone at an organic-to-aqueous ratio of 1 and equilibrium pH ∼5.3. Nickel stripped in 2.0 mol·L−1 H2SO4 was crystallized to yield high-pure NiSO4·6H2O crystals. Further, Li-bearing raffinate was subjected to carbonate precipitation at a higher pH (∼12) and CO32−:Li+ ratio of 1.2. All the recycled products were further employed to the stepwise synthesis of a new ternary precursor, exhibiting similar electrochemical behaviour (with 149 mAh·g−1 capacity) and found compatible with the precursor prepared using virgin materials. The sustainable process index value determined to be 0.0006 cap·t−1 for the overall recycling process indicated that the process is suitable for sustainable development.
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