an official journal of: published by:
an official journal of: published by:
Editor in Chief: RAFFAELLO COSSU
Home

 

GO TO

LI-ION BATTERY RECYCLING AT PILOT SCALE: DEMONSTRATING THE RESYNTHESIS ROUTE ALSO FOR NMC-LFP MIXED BLACK MASS

  • Francesca Pagnanelli - Department of Chemistry, “Sapienza” University of Rome, Italy - Ecorecycling s.r.l., Italy
  • Pietro Altimari - Department of Chemistry, “Sapienza” University of Rome, Italy
  • Pier Giorgio Schiavi - Department of Chemistry, “Sapienza” University of Rome, Italy
  • Ludovica D'Annibale - Department of Chemistry, “Sapienza” University of Rome, Italy
  • Alyssa Mancini - Department of Chemistry, “Sapienza” University of Rome, Italy
  • Marco Colasanti - Department of Chemistry, “Sapienza” University of Rome, Italy
  • Emanuela Moscardini - Eco Recycling s.r.l., Italy
  • Lorenzo Toro - Eco Recycling s.r.l., Italy
  • Ludovica Baldassari - Eco Recycling s.r.l., Italy
  • Luigi Toro - Eco Recycling s.r.l., Italy

DOI 10.31025/2611-4135/2024.19412

Access restricted to subscribed members only

Released under All rights reserved

Copyright: © 2024 CISA Publisher

Abstract

The hydrometallurgical recycling of end-of-life Li-ion batteries constitutes a sustainable path for the integral recovery of battery components. However, the heterogeneity of electrode materials constitutes a limitation for process optimization that must provide robust and flexible strategies. In this work, the preliminary results obtained as part of the demonstration activities of the LIFE DRONE project are reported with particular attention to the possibility of integrating the recycling process based on the resynthesis of NMC (Nickel Manganese Cobalt) cathodes with the treatment of mixed black mass also containing LFP (Lithium Ferrous Phosphate) electrodic powders. The experimental results obtained highlight the possibility of leaching NMC black mass in the absence of hydrogen peroxide when NMC-LFP mixtures are used with almost quantitative extraction yields of metals. In particular, working without H2O2 at 60°C for 3 h the following yields of extraction were obtained: 89% for Ni, 69% for Mn, 89% for Co, 91% for Li, 90% for Fe, 100% for P, 56% for Al and 32% for Cu. Furthermore, the experimental data showed that by varying the pH of the leach liquor, it is possible to separate selectively iron phosphate by quantitative precipitation (100% for Fe, 100% for P and 60% for Al) before proceeding with NMC resynthesis.

Keywords

Editorial History

  • Received: 23 Apr 2024
  • Revised: 20 Jun 2024
  • Accepted: 12 Jul 2024
  • Available online: 17 Sep 2024

References

Abo Atia, T., Elia, G., Hahn, R., Altimari, P., Pagnanelli, F., 2019. Closed-loop hydrometallurgical treatment of end-of-life lithium ion batteries: Towards zero-waste process and metal recycling in advanced batteries. Journal of Energy Chemistry, 35, 220-227.
DOI 10.1016/j.jechem.2019.03.022

Domingues, A.M., Gabbay de Souza, R., Ometto, A.R., Silva, J.R.A., 2023. Life cycle assesment of scenarios for end-of-life management of lithium-ion batteries from smartphones and laptops Detritus, 25, 33-53
DOI 10.31025/2611-4135/2023.18329

EU Regulation 2023/1542 of the European Parliament and of the Council of 12 July 2023 concerning batteries and waste batteries, http://data.europa.eu/eli/reg/2023/1542/oj

Gerold, E., Lerchbammer, R., Antrekowitsch, H., 2022. Parameter Study on the Recycling of LFP Cathode Material Using Hydrometallurgical Methods. Metals 12, 1706.
DOI 10.3390/met12101706

Li, H., Xing, S., Liu, Y., Li, F., Guo, H., Kuang, G., 2017. Recovery of Lithium, Iron, and Phosphorus from Spent LiFePO4 Batteries Using Stoichiometric Sulfuric Acid Leaching System. ACS Sus.Chem.Eng. 5, 8017- 8024
DOI 10.1021/acssuschemeng.7b01594

LIFELIBAT project: Recycling of primary LIthium BATtery by mechanical and hydrometallurgical operations” Life LiBat - LIFE16 ENV/IT/000389 (https://www.lifelibat.eu/it)

LIFE DRONE project: Direct pROduction of New Electrode materials from battery recycling (ENV/IT/000520) (www.lifedrone.eu)

Pagnanelli, F., Moscardini, E., Altimari, P., Abo Atia, T., Toro, L., 2016. Cobalt products from real waste fractions of end of life lithium ion batteries. Waste Manag. 51, 214-221.
DOI 10.1016/j.wasman.2015.11.003

Pagnanelli, F., Schiavi, P.G., Altimari, P., Beolchini, F., Amato, A., Coletta, J., Forte, F., Moscardini, E., Toro, L., 2023. Economic and Environmental Sustainability of an Innovative Cryo-Mechano-Hydrometallurgical Process Validated at Pilot Scale for the Recycling of Li Batteries. Metals, 13, 497.
DOI 10.3390/met13030497

Park, S., Kim, D., Ku, H., Jo, M., Kim, S., Song, J., Yu, J., Kwon, K., 2019. The effect of Fe as an impurity element for sustainable resynthesis of Li(Ni1/3Co1/3Mn1/3)O2 cathode material from spent lithium-ion batteries. Electrochimica Acta 296, 814-822,
DOI 10.1016/j.electacta.2018.11.001

Sa, Q., Heelan, J.A., Lu, Y., Apelian, D., Wang, Y., 2015. Copper Impurity Effects on LiNi1/3Mn1/3Co1/3O2 Cathode Material ACS Applied Materials & Interfaces 7 (37), 20585-20590.
DOI 10.1021/acsami.5b04426

Schiavi, P.G., Branchi, M., Casalese, E., Altimari, P., Navarra, M.A., Pagnanelli, F., 2021. Resynthesis of NMC111 cathodic material from real waste lithium ion batteries. CET, 86, 463 – 468
DOI 10.3303/CET2186078

Song, S.L., Liu, R.Q., Sun, M.M. et al. 2023 Hydrometallurgical recovery of lithium carbonate and iron phosphate from blended cathode materials of spent lithium-ion battery. Rare Met.
DOI 10.1007/s12598-023-02493-9

Wang, M., Liu, K., Dutta, S., Alessi, D.S., Rinklebe, J., Ok, Y.S., Tsang, D.C.W., 2022. Recycling of lithium iron phosphate batteries: Status, technologies, challenges, and prospects, Renewable and Sustainable Energy Reviews, 163, 112515.
DOI 10.1016/j.rser.2022.112515

Xu, Y., Zhang, B., Ge, Z., Zhang, S., Song, B., Tian, Y., Deng, W., Zou, G., Hou, H., Ji, X., 2024. Advances and perspectives towards spent LiFePO4 battery recycling. Journal of Cleaner Production, 434, 140077.
DOI 10.1016/j.jclepro.2023.140077

Zhang, R., Zheng, Y., Yao, Z., Vanaphuti, P., Ma, X., Bong, S., Chen, M., Liu, Y., Cheng, F., Yang, Z., Wang, Y., 2020. Systematic Study of Al Impurity for NCM622 Cathode Materials. ACS Sustainable Chemistry & Engineering 8 (26), 9875-9884
DOI 10.1021/acssuschemeng.0c02965

Zhang, R., Meng, Z., Ma, X., Chen, M., Chen, B., Zheng, Y., Yao, Z., Vanaphuti, P. Bong, S., Yang, Z., Wang, Y., 2020. Understanding fundamental effects of Cu impurity in different forms for recovered LiNi0.6Co0.2Mn0.2O2 cathode materials. Nano Energy 78, 105214
DOI 10.1016/j.nanoen.2020.105214

Zhao, Y., Yuan, X., Jiang, L., Wen, J., Wang, H., Guan, R., Zhang, J., Zeng, G., 2020. Regeneration and reutilization of cathode materials from spent lithium-ion batteries. Chemical Engineering Journal, 383, 123089
DOI 10.1016/j.cej.2019.123089

Zheng, R., Zhao, L., Wang, W., Liu, Y., Ma, Q., Mu, D., Li, R., Dai, C., 2016. Optimized Li and Fe recovery from spent lithium-ion batteries via a solution-precipitation method. RSC Adv. 6, 49
DOI 10.1039/C6RA05477C

Related Contents