Resources Recycling (자원리싸이클링)

The Korean Institute of Resources Recycling (한국자원리싸이클링학회)
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Lithium Recovery from NCM Lithium Ion Battery by Hydrogen Reduction Followed by Water Leaching

NCM계 리튬이온 배터리 양극재의 수소환원과 수침출에 의한 리튬 회수

  • So-Yeong Lee (School of Materials Science and Engineering, Kyungpook National University) ;
  • So-Yeon Lee (L&F Co., Ltd) ;
  • Dae-Hyeon Lee (Korea Zinc) ;
  • Ho-Sang Sohn (School of Materials Science and Engineering, Kyungpook National University)
  • Received : 2023.11.29
  • Accepted : 2024.01.02
  • Published : 2024.02.28
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Abstract

The demand for electric vehicles powered by lithium-ion batteries is continuously increasing. Recovery of valuable metals from waste lithium-ion batteries will be necessary in the future. This research investigated the effect of reaction temperature on the lithium recovery ratio from hydrogen reduction followed by water leaching from lithium-ion battery NCM-based cathode materials. As the reaction temperature increased, the weight loss ratio observed after initiation increased rapidly owing to hydrogen reduction of NiO and CoO; at the same time, the H2O amount generated increased. Above 602 ℃, the anode materials Ni and Co were reduced and existed in the metallic phases. As the hydrogen reduction temperature was increased, the Li recovery ratio also increased; at 704 ℃ and above, the Li recovery ratio reached a maximum of approximately 92%. Therefore, it is expected that Li can be selectively recovered by hydrogen reduction as a waste lithium-ion battery pretreatment, and the residue can be reprocessed to efficiently separate and recover valuable metals.

전기차용 리튬이온배터리의 수요가 증가함에 따라 향후 발생할 폐리튬이온배터리 중의 유가금속 회수가 필요하다. 본 연구에서는 리튬이온배터리의 NCM계 양극재를 수소환원과 수침출에 의해 리튬을 수산화리튬으로 회수할 때의 회수율에 미치는 반응온도의 영향을 조사하였다. 반응온도가 상승함에 따라 수소에 의한 NiO, CoO의 환원에 의해 무게 감소율이 반응초기부터 급격하게 증가하였으며 동시에 H2O 발생량도 증가하였다. 602 ℃ 이상에서는 양극재 중의 Ni, Co가 전부 환원되어 금속상으로 존재하였다. 그리고 수소환원 온도의 상승과 함께 Li 회수률도 증가하였으나 704 ℃ 이상에서는 약 92 % 이상의 유사한 수준을 나타내었다. 따라서 폐Li이온 배터리의 전처리로 수소환원하는 것에 의해 리튬만 사전에 회수하고 잔사를 재처리하면 효율적으로 유가금속을 분리하여 회수할 수 있을 것으로 기대된다.

Keywords

Acknowledgement

이 논문은 2023학년도 경북대학교 연구년 교수 연구비에 의하여 연구되었음.

References

  1. Ho-Sang Sohn, 2022 : Extractive Metallurgy of Lithium, Resources Recycling, 31(3), pp.3-15. https://doi.org/10.7844/kirr.2022.31.3.3
  2. Nayaka, G. P., Pai, K. V., Santhosh, G., et al., 2016 : Recovery of cobalt as cobalt oxalate from spent lithium ion batteries by using glycine as leaching agent, Journal of Environmental Chemical Engineering, 4(2), pp.2378-2383. https://doi.org/10.1016/j.jece.2016.04.016
  3. Huang, Z., Liu, F., Makuza, B., et al., 2022 : Metal Reclamation from Spent Lithium-Ion Battery Cathode Materials: Directional Conversion of Metals Based on Hydrogen Reduction, ACS Sustainable Chemistry & Engineering, 10(2), pp.756-765. https://doi.org/10.1021/acssuschemeng.1c05721
  4. Liu, F., Peng, C., Ma, Q., et al., 2021 : Selective lithium recovery and integrated preparation of high-purity lithium hydroxide products from spent lithium-ion batteries, Separation and Purification Technology, 259, 118181, pp.1-9. https://doi.org/10.1016/j.seppur.2020.118181
  5. Hong, S. J., Kim, H. J., Son, S. R., et al., 2021 : Method of recycling active metal of lithium secondary battery, KR10-2021-0101647.
  6. Park, S. J., Park, J. S., Lee, M. G., et al., 2019 : Manufacturing method of lithium hydroxide monohydrate using waste cathode material of lithium ion secondary battery, KR10-2019-0119329.
  7. Lee, So-Yeon, Lee, Dae-Hyeon, Lee, So-Yeong, et al., 2022 : Lithium Recovery from NCM Lithium-ion Battery by Carbonation Roasting with Graphite Followed by Water Leaching, Resources Recycling, 31(4), pp.26-33. https://doi.org/10.7844/kirr.2022.31.4.26
  8. Kim, D. W., Jang, S. T. and Baek, K. M., 2013 : Recovery of Lithium and Leaching Behavior of NCM Powder by Hydrogen Reductive Treatment from NCM System Li-ion Battery Scraps, J. of Korean Inst. of Resources Recycling, 22(3), pp.43-49. https://doi.org/10.7844/kirr.2013.22.3.43
  9. Lee, Dae-Hyeon, Lee, So-Yeon, Lee, So-Yeong, et al., 2022 : Lithium Recovery from NCM Lithium Ion Battery by Carbonation Roasting Followed by Water Leaching, Korean J. Met. Mater., 60(10), pp.744-750. https://doi.org/10.3365/KJMM.2022.60.10.744