Copper-Mediated Leaching of LiNi0.65Co0.25Mn0.10O2 in H3PO4: Thermodynamics, Structural Evolution, and Redox Mechanism

Đorđević, Ivan; Medić, Dragana; Gajić, Nataša; Nujkić, Maja; Nedelkovski, Vladan; Stanković, Sonja; Cvetković, Aleksandar

doi:10.3390/molecules31091502

Article Restricted access M21

molecules-31-01502-v2.pdf (14.38MB)

2026

Đorđević, Ivan
Medić, Dragana
Gajić, Nataša
Nujkić, Maja
Nedelkovski, Vladan
Stanković, Sonja
Cvetković, Aleksandar

MDPI

Molecules

1502

English

M21 - Paper in a top international journal

This study investigates the leaching behavior of the LiNi0.65Co0.25Mn0.10O2 cathode material in a phosphoric acid medium, with metallic copper recycled from spent battery components serving as a reducing agent. The aim was to develop an efficient approach for the recovery of Li, Ni, Co, and Mn while providing a mechanistic understanding. Leaching experiments were performed by varying key parameters, including copper addition, acid concentration (0.2–0.8 mol·L−1), cathode mass (0.2–1.0 g), stirring rate (0–600 rpm), and temperature (35–80 ◦C). Thermodynamic analysis, supported by Pourbaix and species distribution diagrams, was used to interpret metal behavior. The results show that lithium is readily dissolved, whereas the extraction of Ni, Co, and Mn depends on the presence of copper, which enables their reduction and dissolution. Optimal conditions (0.4 mol·L−1 H3PO4, 0.2 g Cu, 600 rpm, 80 ◦C) enabled rapid extraction, exceeding 90% within 30 min, while near-complete extraction (~100%, 99%, 99%, and 97% for Li, Ni, Co, and Mn) was achieved after 60 min. Structural analysis revealed a transformation from the layered structure to spinel-like intermediates, followed by their dissolution and formation of copper phosphate phases. The proposed system represents an efficient approach for the sustainable recycling of NMC cathodes.

lithium-ion batteries, NMC cathode, phosphoric acid leaching, copper-assisted leaching, battery recycling

DOI

10.3390/molecules31091502

ISSN

1420-3049

URI

https://repozitorijum.tfbor.bg.ac.rs/handle/...

Scopus Web of Science OpenCitations OpenAlex

dc.creator	Đorđević, Ivan
dc.creator	Medić, Dragana
dc.creator	Gajić, Nataša
dc.creator	Nujkić, Maja
dc.creator	Nedelkovski, Vladan
dc.creator	Stanković, Sonja
dc.creator	Cvetković, Aleksandar
dc.title	Copper-Mediated Leaching of LiNi0.65Co0.25Mn0.10O2 in H3PO4: Thermodynamics, Structural Evolution, and Redox Mechanism
dc.date.issued	2026
dc.publisher	MDPI
dc.identifier.doi	10.3390/molecules31091502
dc.identifier.issn	1420-3049
dc.type	article
dc.source	Molecules
dc.citation.volume	31
dc.citation.issue	9
dc.citation.spage	1502
dc.language.iso	en
dc.type.version	publishedVersion
dc.citation.rank	M21
dc.citation.ifactor	5.5
dc.subject	lithium-ion batteries
dc.subject	NMC cathode
dc.subject	phosphoric acid leaching
dc.subject	copper-assisted leaching
dc.subject	battery recycling
dc.description.abstract	This study investigates the leaching behavior of the LiNi0.65Co0.25Mn0.10O2 cathode material in a phosphoric acid medium, with metallic copper recycled from spent battery components serving as a reducing agent. The aim was to develop an efficient approach for the recovery of Li, Ni, Co, and Mn while providing a mechanistic understanding. Leaching experiments were performed by varying key parameters, including copper addition, acid concentration (0.2–0.8 mol·L−1), cathode mass (0.2–1.0 g), stirring rate (0–600 rpm), and temperature (35–80 ◦C). Thermodynamic analysis, supported by Pourbaix and species distribution diagrams, was used to interpret metal behavior. The results show that lithium is readily dissolved, whereas the extraction of Ni, Co, and Mn depends on the presence of copper, which enables their reduction and dissolution. Optimal conditions (0.4 mol·L−1 H3PO4, 0.2 g Cu, 600 rpm, 80 ◦C) enabled rapid extraction, exceeding 90% within 30 min, while near-complete extraction (~100%, 99%, 99%, and 97% for Li, Ni, Co, and Mn) was achieved after 60 min. Structural analysis revealed a transformation from the layered structure to spinel-like intermediates, followed by their dissolution and formation of copper phosphate phases. The proposed system represents an efficient approach for the sustainable recycling of NMC cathodes.
dc.rights.license	CC-BY
dc.rights.uri	https://creativecommons.org/licenses/by/4.0/
dc.date.accessioned	2026-10-29T10:25:50Z
dc.description.provenance	Submitted by dmedic@tfbor.bg.ac.rs on 2026-10-29 09:56:25.82612, with 2 file(s). Approved by Милица Ницуловић (mniculovic@tfbor.bg.ac.rs) on 2026-10-29T10:25:50Z.
dc.identifier.uri	https://repozitorijum.tfbor.bg.ac.rs/handle/123456789/6181


Copper-Mediated Leaching of LiNi0.65Co0.25Mn0.10O2 in H3PO4: Thermodynamics, Structural Evolution, and Redox Mechanism	16


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