Low-temperature chlorination roasting technology for the simultaneous recovery of valuable metals from spent LiCoO<sub>2</sub> cathode material

Junjie Shi; Changle Hou; Jingjing Dong; Dong Chen; Jianzhong Li

doi:10.1007/s12613-024-2898-4

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Junjie Shi, Changle Hou, Jingjing Dong, Dong Chen, and Jianzhong Li, Low-temperature chlorination roasting technology for the simultaneous recovery of valuable metals from spent LiCoO₂ cathode material, Int. J. Miner. Metall. Mater.,(2025). https://doi.org/10.1007/s12613-024-2898-4

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Junjie Shi, Changle Hou, Jingjing Dong, Dong Chen, and Jianzhong Li, Low-temperature chlorination roasting technology for the simultaneous recovery of valuable metals from spent LiCoO2 cathode material, Int. J. Miner. Metall. Mater.,(2025). https://doi.org/10.1007/s12613-024-2898-4

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Research Article

Low-temperature chlorination roasting technology for the simultaneous recovery of valuable metals from spent LiCoO₂ cathode material

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Corresponding author:
Junjie Shi E-mail: junjieshi@126.com
Received: 27 December 2023; Revised: 28 March 2024; Accepted: 1 April 2024; Available online: 2 April 2024

Abstract

Abstract

With the continuous increase in the disposal volume of spent lithium-ion batteries (LIBs), properly recycling spent LIBs has become essential for the advancement of the circular economy. This study presents a systematic analysis of the chlorination roasting kinetics and proposes a new two-step chlorination roasting process that integrates thermodynamics for the recycling of LIB cathode materials. The activation energy for the chloride reaction was 88.41 kJ/mol according to thermogravimetric analysis–derivative thermogravimetry data obtained by using model-free, model-fitting, and Z(α) function (α is conversion rate). Results indicated that the reaction was dominated by the first-order (F1) model when the conversion rate was less than or equal to 0.5 and shifted to the second-order (F2) model when the conversion rate exceeded 0.5. Optimal conditions were determined by thoroughly investigating the effects of roasting temperature, roasting time, and the mass ratio of NH₄Cl to LiCoO₂. Under the optimal conditions, namely 400°C, 20 min, and NH₄Cl/LiCoO₂ mass ratio of 3:1, the leaching efficiency of Li and Co reached 99.43% and 99.05%, respectively. Analysis of the roasted products revealed that valuable metals in LiCoO₂ transformed into CoCl₂ and LiCl. Furthermore, the reaction mechanism was elucidated, providing insights for the establishment of a novel low-temperature chlorination roasting technology based on a crystal structure perspective. This technology can guide the development of LIB recycling processes with low energy consumption, low secondary pollution, high recovery efficiency, and high added value.
- spent lithium-ion battery;
- thermodynamics;
- chlorination roasting;
- kinetics;
- circular economy

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