A novel integrated approach for selective separation and recovery of critical metals from ground cathode-anode mixtures of spent li-ion batteries

The growing demand for sustainable management of spent Li-ion batteries has necessitated efficient recovery processes for valuable elements. Conventional recycling of Li-ion batteries still relies on separate anode and cathode processing lines and high-temperature steps that inflate cost and carbon footprint. This study overcome these limitations with a single-line, room-temperature hydrometallurgical flowsheet that treats a ground, unsorted mixture of cathode and anode materials. A dilute H₂SO₄ + H₂O₂ leach operated at 25 °C dissolves valuable metals, eliminating the thermal energy demand of roast-leach routes. Copper is first cemented (85 % recovery at Fe/Cu = 1.2), and Fe Al hydroxides are precipitated at pH 5.5. The clarified leachate then enters a tailored solvent-extraction step: Mn is selectively extracted with 15 % saponified D2EHPA at pH 3 and stripped with 0.2 M H₂SO₄ (92 % recovery); Co and Ni are subsequently split with Cyanex 272 at pH 4.5 (91 % and 88 % recovery, respectively), while Li remains in the raffinate for downstream recovery. The integrated sequence delivers Cu, Fe, Al, Mn, Co, Ni and Li streams, using mild conditions and low residence times. By recovering all critical metals from a single mixed feed, the process eliminates costly pre-sorting and duplicate lines, reduces chemical inventory compared with multi-acid schemes, and cuts energy consumption relative to pyrometallurgical or hybrid schemes. These attributes position the flowsheet as a scalable, environmentally benign alternative for industrial Li-ion battery recycling and provide a robust baseline for future optimization. • Low-temperature flowsheet recovers >90 % Li, Co, Ni, Mn, and Cu from spent NMC EV batteries. • Sequential Cu/Fe/Al removal enables Co, Ni & Mn separation without pyrometallurgy. • Saponified D2EHPA yields 92 % selective Mn extraction at pH 3. • Reagent-efficient route converts LIB waste into high-purity metal feedstocks.

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Publication Details

Journal
Journal of Energy Storage
Published
2025-06-06
DOI
https://doi.org/10.1016/j.est.2025.117373
Citations
4
Primary Topic
Extraction and Separation Processes
Type
article
Field-Weighted Citation Impact
2.85
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article

A novel integrated approach for selective separation and recovery of critical metals from ground cathode-anode mixtures of spent li-ion batteries

Francesco Vegliò, Valentina Innocenzi, Zhitong Yao, Pietro Romano et al.
4 citations
Journal of Energy Storage
Extraction and Separation Processes
2.85
article

A novel integrated approach for selective separation and recovery of critical metals from ground cathode-anode mixtures of spent li-ion batteries

Francesco Vegliò, Valentina Innocenzi, Zhitong Yao, Pietro Romano, Tasaddaq Younas, Hossein Shalchian
article en
4 citations

Abstract

The growing demand for sustainable management of spent Li-ion batteries has necessitated efficient recovery processes for valuable elements. Conventional recycling of Li-ion batteries still relies on separate anode and cathode processing lines and high-temperature steps that inflate cost and carbon footprint. This study overcome these limitations with a single-line, room-temperature hydrometallurgical flowsheet that treats a ground, unsorted mixture of cathode and anode materials. A dilute H₂SO₄ + H₂O₂ leach operated at 25 °C dissolves valuable metals, eliminating the thermal energy demand of roast-leach routes. Copper is first cemented (85 % recovery at Fe/Cu = 1.2), and Fe Al hydroxides are precipitated at pH 5.5. The clarified leachate then enters a tailored solvent-extraction step: Mn is selectively extracted with 15 % saponified D2EHPA at pH 3 and stripped with 0.2 M H₂SO₄ (92 % recovery); Co and Ni are subsequently split with Cyanex 272 at pH 4.5 (91 % and 88 % recovery, respectively), while Li remains in the raffinate for downstream recovery. The integrated sequence delivers Cu, Fe, Al, Mn, Co, Ni and Li streams, using mild conditions and low residence times. By recovering all critical metals from a single mixed feed, the process eliminates costly pre-sorting and duplicate lines, reduces chemical inventory compared with multi-acid schemes, and cuts energy consumption relative to pyrometallurgical or hybrid schemes. These attributes position the flowsheet as a scalable, environmentally benign alternative for industrial Li-ion battery recycling and provide a robust baseline for future optimization. • Low-temperature flowsheet recovers >90 % Li, Co, Ni, Mn, and Cu from spent NMC EV batteries. • Sequential Cu/Fe/Al removal enables Co, Ni & Mn separation without pyrometallurgy. • Saponified D2EHPA yields 92 % selective Mn extraction at pH 3. • Reagent-efficient route converts LIB waste into high-purity metal feedstocks.

Journal of Energy StorageVol. 129
University of L'Aquila (IT), Hangzhou Dianzi University (CN)
Openalex Percentile: Top 9%
Extraction and Separation Processes
2.85
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