Dissolution of Spent Lithium‐Ion Battery Cathode Materials: Overlooked Significance of Aluminum Impurities

Abstract Impurities are pivotal in determining the quality of the critical metal products derived from spent lithium‐ion batteries (LIBs), but there is a lack of understanding of their potential impacts. The mechanisms by which Aluminium (Al) impurities permeate the active crystals of spent ternary...

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Main Authors: Kang Liu, Yuying Zhang, Mengmeng Wang, Xiaohong Zhu, Roya Maboudian, Daniel C.W. Tsang
Format: Article
Language:English
Published: Wiley 2025-06-01
Series:Advanced Science
Subjects:
Online Access:https://doi.org/10.1002/advs.202417737
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author Kang Liu
Yuying Zhang
Mengmeng Wang
Xiaohong Zhu
Roya Maboudian
Daniel C.W. Tsang
author_facet Kang Liu
Yuying Zhang
Mengmeng Wang
Xiaohong Zhu
Roya Maboudian
Daniel C.W. Tsang
author_sort Kang Liu
collection DOAJ
description Abstract Impurities are pivotal in determining the quality of the critical metal products derived from spent lithium‐ion batteries (LIBs), but there is a lack of understanding of their potential impacts. The mechanisms by which Aluminium (Al) impurities permeate the active crystals of spent ternary nickel─cobalt─manganese oxide (NCM) cathode materials and interact with critical metal sites are elucidated. During frictional contact, the substitution of transition metals by Al impurities disrupts the bonding between critical metals and oxygen, leading to the formation of more stable Al─O covalent bonds. Al can preferentially substitute for Co, altering the local coordination and electronic structure of transition metals. Owing to the strong interaction of Al─O, the Fermi level shifts downward, thus increasing the stabilization of lattice oxygen in the NCM cathode materials and consequently delaying the dissolution of NCM cathode materials. In different extraction environments, the invasion of Al retards the release of lattice oxygen and inhibits the dissolution of NCM in formic acid but enhances those in ammonia solution and shows mixed results in deep eutectic solvents. These crucial findings will help to elucidate the mechanisms of Al impurities in the recycling industry chain of retired LIBs, thereby enhancing the recovery of high‐quality critical metal products.
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publishDate 2025-06-01
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series Advanced Science
spelling doaj-art-71e090c99d4b4b92af08064526d2c5de2025-08-20T03:26:10ZengWileyAdvanced Science2198-38442025-06-011221n/an/a10.1002/advs.202417737Dissolution of Spent Lithium‐Ion Battery Cathode Materials: Overlooked Significance of Aluminum ImpuritiesKang Liu0Yuying Zhang1Mengmeng Wang2Xiaohong Zhu3Roya Maboudian4Daniel C.W. Tsang5Department of Civil and Environmental Engineering The Hong Kong University of Science and Technology Clear Water Bay Hong Kong 999077 ChinaDepartment of Civil and Environmental Engineering The Hong Kong University of Science and Technology Clear Water Bay Hong Kong 999077 ChinaDepartment of Civil and Environmental Engineering The Hong Kong University of Science and Technology Clear Water Bay Hong Kong 999077 ChinaDepartment of Civil and Environmental Engineering University of California Berkeley Berkeley CA 94720 USADepartment of Chemical and Biomolecular Engineering University of California Berkeley Berkeley CA 94720 USADepartment of Civil and Environmental Engineering The Hong Kong University of Science and Technology Clear Water Bay Hong Kong 999077 ChinaAbstract Impurities are pivotal in determining the quality of the critical metal products derived from spent lithium‐ion batteries (LIBs), but there is a lack of understanding of their potential impacts. The mechanisms by which Aluminium (Al) impurities permeate the active crystals of spent ternary nickel─cobalt─manganese oxide (NCM) cathode materials and interact with critical metal sites are elucidated. During frictional contact, the substitution of transition metals by Al impurities disrupts the bonding between critical metals and oxygen, leading to the formation of more stable Al─O covalent bonds. Al can preferentially substitute for Co, altering the local coordination and electronic structure of transition metals. Owing to the strong interaction of Al─O, the Fermi level shifts downward, thus increasing the stabilization of lattice oxygen in the NCM cathode materials and consequently delaying the dissolution of NCM cathode materials. In different extraction environments, the invasion of Al retards the release of lattice oxygen and inhibits the dissolution of NCM in formic acid but enhances those in ammonia solution and shows mixed results in deep eutectic solvents. These crucial findings will help to elucidate the mechanisms of Al impurities in the recycling industry chain of retired LIBs, thereby enhancing the recovery of high‐quality critical metal products.https://doi.org/10.1002/advs.202417737aluminum interactionscritical mineral extractionelectric vehicle batteryhydrometallurgical dissolutionmetal‐oxygen bondingsustainable waste management
spellingShingle Kang Liu
Yuying Zhang
Mengmeng Wang
Xiaohong Zhu
Roya Maboudian
Daniel C.W. Tsang
Dissolution of Spent Lithium‐Ion Battery Cathode Materials: Overlooked Significance of Aluminum Impurities
Advanced Science
aluminum interactions
critical mineral extraction
electric vehicle battery
hydrometallurgical dissolution
metal‐oxygen bonding
sustainable waste management
title Dissolution of Spent Lithium‐Ion Battery Cathode Materials: Overlooked Significance of Aluminum Impurities
title_full Dissolution of Spent Lithium‐Ion Battery Cathode Materials: Overlooked Significance of Aluminum Impurities
title_fullStr Dissolution of Spent Lithium‐Ion Battery Cathode Materials: Overlooked Significance of Aluminum Impurities
title_full_unstemmed Dissolution of Spent Lithium‐Ion Battery Cathode Materials: Overlooked Significance of Aluminum Impurities
title_short Dissolution of Spent Lithium‐Ion Battery Cathode Materials: Overlooked Significance of Aluminum Impurities
title_sort dissolution of spent lithium ion battery cathode materials overlooked significance of aluminum impurities
topic aluminum interactions
critical mineral extraction
electric vehicle battery
hydrometallurgical dissolution
metal‐oxygen bonding
sustainable waste management
url https://doi.org/10.1002/advs.202417737
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AT mengmengwang dissolutionofspentlithiumionbatterycathodematerialsoverlookedsignificanceofaluminumimpurities
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