Comparative study on the leaching behavior of lithium-ion battery black mass using sulfuric and organic acids combined with hydrogen peroxide

• Various acids with H 2 O 2 were conducted for black mass leaching process. • H 2 O 2 improved Co, Ni, Mn leaching and reduced Fe dissolution. • 1 M H 2 SO 4 + H 2 O 2 gave highest leaching for Li, Ni, Co, and Cu. • Strong chelation by organic acids hindered metal precipitation. • Organic acid may improve eco-friendly metal recovery from waste. The black mass obtained from spent lithium-ion batteries offers a promising opportunity to establish a sustainable supply chain for critical battery materials, such as lithium, cobalt, manganese, and nickel. Battery recycling provides an effective solution for substantially reducing environmental waste. This study examines the physicochemical properties and leaching behavior of lithium-ion battery black mass using various acids (sulfuric, malic, acetic, citric, and butyric acids) in combination with hydrogen peroxide (H 2 O 2 ) as a reductant. Physicochemical analyses using powder X-ray diffraction and inductively coupled plasma-optical emission spectroscopy indicated that the black mass originated primarily from the NMC622-type or nickel-rich cathode materials. Leaching experiments revealed that 1 M sulfuric acid combined with H 2 O 2 yielded the highest extraction efficiencies, achieving Li (62.2 %), Cu (53.5 %), Fe (26.9 %), Al (46.5 %), Ni (55.1 %), Co (50.6 %), and Mn (36.7 %). Although organic acids generally exhibit lower extraction efficiencies, citric and malic acids perform better than acetic and butyric acids because of their greater capacity to form stable chelate complexes with metal ions. However, strong chelate formation with citric and malic acids limits selective precipitation during subsequent pH adjustment. In contrast, despite their lower overall leaching efficiencies, the use of acetic and butyric acids provided enhanced selectivity for the precipitation of Co, Cu, and Ni at pH 8 and Mn at pH 9 while significantly reducing lithium co-precipitation. These results highlight that the careful selection of acids combined with the reductive action of H 2 O 2 is essential for optimizing the selective recovery of valuable metals from battery black mass.

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Publication Details

Journal
Separation and Purification Technology
Published
2025-06-13
DOI
https://doi.org/10.1016/j.seppur.2025.133991
Citations
10
Primary Topic
Extraction and Separation Processes
Type
article
Field-Weighted Citation Impact
7.13

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article

Comparative study on the leaching behavior of lithium-ion battery black mass using sulfuric and organic acids combined with hydrogen peroxide

Yeomin Yoon, Seokyoon Moon, Hojung Rho, Weon‐Sik Chae et al.
10 citations
Separation and Purification Technology
Extraction and Separation Processes
7.13
article

Comparative study on the leaching behavior of lithium-ion battery black mass using sulfuric and organic acids combined with hydrogen peroxide

Yeomin Yoon, Seokyoon Moon, Hojung Rho, Weon‐Sik Chae, Byung‐Moon Jun
article en
10 citations

Abstract

• Various acids with H 2 O 2 were conducted for black mass leaching process. • H 2 O 2 improved Co, Ni, Mn leaching and reduced Fe dissolution. • 1 M H 2 SO 4 + H 2 O 2 gave highest leaching for Li, Ni, Co, and Cu. • Strong chelation by organic acids hindered metal precipitation. • Organic acid may improve eco-friendly metal recovery from waste. The black mass obtained from spent lithium-ion batteries offers a promising opportunity to establish a sustainable supply chain for critical battery materials, such as lithium, cobalt, manganese, and nickel. Battery recycling provides an effective solution for substantially reducing environmental waste. This study examines the physicochemical properties and leaching behavior of lithium-ion battery black mass using various acids (sulfuric, malic, acetic, citric, and butyric acids) in combination with hydrogen peroxide (H 2 O 2 ) as a reductant. Physicochemical analyses using powder X-ray diffraction and inductively coupled plasma-optical emission spectroscopy indicated that the black mass originated primarily from the NMC622-type or nickel-rich cathode materials. Leaching experiments revealed that 1 M sulfuric acid combined with H 2 O 2 yielded the highest extraction efficiencies, achieving Li (62.2 %), Cu (53.5 %), Fe (26.9 %), Al (46.5 %), Ni (55.1 %), Co (50.6 %), and Mn (36.7 %). Although organic acids generally exhibit lower extraction efficiencies, citric and malic acids perform better than acetic and butyric acids because of their greater capacity to form stable chelate complexes with metal ions. However, strong chelate formation with citric and malic acids limits selective precipitation during subsequent pH adjustment. In contrast, despite their lower overall leaching efficiencies, the use of acetic and butyric acids provided enhanced selectivity for the precipitation of Co, Cu, and Ni at pH 8 and Mn at pH 9 while significantly reducing lithium co-precipitation. These results highlight that the careful selection of acids combined with the reductive action of H 2 O 2 is essential for optimizing the selective recovery of valuable metals from battery black mass.

Separation and Purification TechnologyVol. 376
Seoul National University of Science and Technology (KR), Ewha Womans University (KR), Korea Institute of Civil Engineering and Building Technology (KR), Kyung Hee University (KR)
Korea Institute of Construction Technology, National Research Foundation of Korea
Clean water and sanitation
Openalex Percentile: Top 2%
Extraction and Separation Processes
7.13
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