Lithium-Ion Battery Recycling

A special issue of Batteries (ISSN 2313-0105). This special issue belongs to the section "Battery Processing, Manufacturing and Recycling".

Deadline for manuscript submissions: 5 August 2024 | Viewed by 5276

Special Issue Editors


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Guest Editor
Electrification and Energy Infrastructures Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
Interests: lithium-ion battery recycling; battery manufacturing.
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Guest Editor
Key Laboratory of Multifunctional Nanomaterials and Smart Systems, Advanced Materials Division, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou 215123, China
Interests: recycling spent lithium-ion batteries; nanomaterials synthesis for energy storage and conversion; smart materials synthesis and application

Special Issue Information

Dear Colleagues,

Lithium-ion batteries are widely used in a variety of consumer and industrial applications, including smartphones, laptops, electric vehicles, and renewable energy storage systems. As the demand for these batteries continues to grow, so does the need for effective recycling methods to manage the end-of-life batteries. Lithium-ion battery recycling involves the recovery and re-use of the valuable materials contained in the batteries, reducing the need for new resources and minimizing the environmental impact of discarded batteries. This Special Issue invites researchers to contribute original research/review/perspective articles on the development of advanced technologies for lithium-ion battery recycling. Topics of interest include, but are not limited to:

  • Direct recycling (e.g., direct recycling and upcycling of cathodes, advanced separation methods, anode recycling, electrolyte recovery);
  • Hydrometallurgy;
  • Pyrometallurgy;
  • Life cycle assessment and environmental impacts of recycling;
  • New designs and materials to facilitate recycling;
  • Recycling manufacturing scraps.

Dr. Yaocai Bai
Dr. Panpan Xu
Guest Editors

Manuscript Submission Information

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Keywords

  • recycling
  • direct recycling
  • lithium-ion batteries
  • upcycling
  • hydrometallurgy
  • cathode
  • graphite

Published Papers (3 papers)

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Research

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12 pages, 3960 KiB  
Article
Efficient Leaching of Metal Ions from Spent Li-Ion Battery Combined Electrode Coatings Using Hydroxy Acid Mixtures and Regeneration of Lithium Nickel Manganese Cobalt Oxide
by Ananda S. Amarasekara, Deping Wang and Ambar B. Shrestha
Batteries 2024, 10(6), 170; https://doi.org/10.3390/batteries10060170 - 21 May 2024
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Abstract
Extensive use of Li-ion batteries in electric vehicles, electronics, and other energy storage applications has resulted in a need to recycle valuable metals Li, Mn, Ni, and Co in these devices. In this work, an aqueous mixture of glycolic and lactic acid is [...] Read more.
Extensive use of Li-ion batteries in electric vehicles, electronics, and other energy storage applications has resulted in a need to recycle valuable metals Li, Mn, Ni, and Co in these devices. In this work, an aqueous mixture of glycolic and lactic acid is shown as an excellent leaching agent to recover these critical metals from spent Li-ion laptop batteries combined with cathode and anode coatings without adding hydrogen peroxide or other reducing agents. An aqueous acid mixture of 0.15 M in glycolic and 0.35 M in lactic acid showed the highest leaching efficiencies of 100, 100, 100, and 89% for Li, Ni, Mn, and Co, respectively, in an experiment at 120 °C for 6 h. Subsequently, the chelate solution was evaporated to give a mixed metal-hydroxy acid chelate gel. Pyrolysis of the dried chelate gel at 800 °C for 15 h could be used to burn off hydroxy acids, regenerating lithium nickel manganese cobalt oxide, and the novel method presented to avoid the precipitation of metals as hydroxide or carbonates. The Li, Ni, Mn, and Co ratio of regenerated lithium nickel manganese cobalt oxide is comparable to this metal ratio in pyrolyzed electrode coating and showed similar powder X-ray diffractograms, suggesting the suitability of α-hydroxy carboxylic acid mixtures as leaching agents and ligands in regeneration of mixed metal oxide via pyrolysis of the dried chelate gel. Full article
(This article belongs to the Special Issue Lithium-Ion Battery Recycling)
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15 pages, 3237 KiB  
Article
Sequential Recovery of Critical Metals from Leached Liquor of Processed Spent Lithium-Ion Batteries
by Ayorinde Emmanuel Ajiboye and Trevor L. Dzwiniel
Batteries 2023, 9(11), 549; https://doi.org/10.3390/batteries9110549 - 9 Nov 2023
Viewed by 1857
Abstract
The processing and extraction of critical metals from black mass is important to battery recycling. Separation and recovery of critical metals (Co, Ni, Li, and Mn) from other metal impurities must yield purified metal salts, while avoiding substantial losses of critical metals. Solvent [...] Read more.
The processing and extraction of critical metals from black mass is important to battery recycling. Separation and recovery of critical metals (Co, Ni, Li, and Mn) from other metal impurities must yield purified metal salts, while avoiding substantial losses of critical metals. Solvent extraction in batch experiments were conducted using mixed metal sulphates obtained from the leach liquor obtained from spent and shredded lithium-ion batteries. Selective extraction of Mn2+, Fe3+, Al3+ and Cu2+ from simulated and real leached mixed metals solution was carried out using di-2-ethylhexylphophoric acid (D2EPHA) and Cyanex-272 at varying pH. Further experiments with the preferred extractant (D2EPHA) were performed under different conditions: changing the concentration of extractant, organic to aqueous ratio, and varying the diluents. At optimum conditions (40% v/v D2EPHA in kerosene, pH 2.5, O:A = 1:1, 25 °C, and 20 min), 85% Mn2+, 98% Al3+, 100% Fe3+, and 43% Cu2+ were extracted with losses of only trace amounts (<5.0%) of Co2+, Ni2+, and Li+. The order of extraction efficiency for the diluents was found to be kerosene > Exxal-10 >>> dichloromethane (CH2Cl2) > toluene. Four stages of stripping of metals loaded on D2EPHA were performed as co-extracted metal impurities were selectively stripped, and a purified MnSO4 solution was produced. Spent extractant was regenerated after Fe3+ and Al3+ were completely stripped using 1.0 M oxalic acid (C2H2O4). Full article
(This article belongs to the Special Issue Lithium-Ion Battery Recycling)
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Review

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20 pages, 3351 KiB  
Review
Direct Recycling Technology for Spent Lithium-Ion Batteries: Limitations of Current Implementation
by Anna Pražanová, Zbyněk Plachý, Jan Kočí, Michael Fridrich and Vaclav Knap
Batteries 2024, 10(3), 81; https://doi.org/10.3390/batteries10030081 - 28 Feb 2024
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Abstract
The significant deployment of lithium-ion batteries (LIBs) within a wide application field covering small consumer electronics, light and heavy means of transport, such as e-bikes, e-scooters, and electric vehicles (EVs), or energy storage stationary systems will inevitably lead to generating notable amounts of [...] Read more.
The significant deployment of lithium-ion batteries (LIBs) within a wide application field covering small consumer electronics, light and heavy means of transport, such as e-bikes, e-scooters, and electric vehicles (EVs), or energy storage stationary systems will inevitably lead to generating notable amounts of spent batteries in the coming years. Considering the environmental perspective, material resource sustainability, and terms of the circular economy, recycling represents a highly prospective strategy for LIB end-of-life (EOL) management. In contrast with traditional, large-scale, implemented recycling methods, such as pyrometallurgy or hydrometallurgy, direct recycling technology constitutes a promising solution for LIB EOL treatment with outstanding environmental benefits, including reduction of energy consumption and emission footprint, and weighty economic viability. This work comprehensively assesses the limitations and challenges of state-of-the-art, implemented direct recycling methods for spent LIB cathode and anode material treatment. The introduced approaches include solid-state sintering, electrochemical relithiation in organic and aqueous electrolytes, and ionothermal, solution, and eutectic relithiation methods. Since most direct recycling techniques are still being developed and implemented primarily on a laboratory scale, this review identifies and discusses potential areas for optimization to facilitate forthcoming large-scale industrial implementation. Full article
(This article belongs to the Special Issue Lithium-Ion Battery Recycling)
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Planned Papers

The below list represents only planned manuscripts. Some of these manuscripts have not been received by the Editorial Office yet. Papers submitted to MDPI journals are subject to peer-review.

Title: A Mini Review of Electrochemical Recovery for Lithium Ion Batteries
Authors: Yaocai Bai*, Lu Yu, Ilias Belharouak
Affiliation: Oak Ridge National Laboratory

Title: An acid/alkali-free hydrothermal method for selectively recycling lithium from spent cathode materials with glucose
Authors: Xinyu Bian, Ahui Zhu, Kai Zhu, Shubin Wang
Affiliation: Harbin Engineering University
Abstract: In recent years, the rapid growth in the use of lithium-ion batteries (LIBs) and the scarcity of lithium resources have led to an explosion in the demand of Li resources. The selective extraction of lithium from spent lithium-ion batteries (sLIBs) has received increasing attention. Herein, we proposed an acid/alkali-free selective process to recycle spent LiCoO2 cathode materials via using glucose as a leaching reagent and a reducing agent to leach LiCoO2 cathode materials. Li can be leached selectively and Co precipitates as CoO precipitates. The leaching efficiencies of Li (99.57 %) and Co (3.08 %) can be achieved under the condition of 180 ℃ and leaching for 24 h. And the CoO residues can be covert to carbon coated Co3O4. As-prepared carbon coated Co3O4 demonstrates a capacity of 1476 mAh g-1 at 0.1 A g-1. Meanwhile, a capacity of 885 mAh g-1 at 0.5 A g-1 can be maintained after 500 cycles, suggesting a stable cycling performance.This work suggests an innovative idea for preferentially extracting lithium from spent LiCoO2 batteries, which provides a new idea for the recycling of sLIBs batteries.

Title: Upcycling of spent lithium ion battery mateirals
Authors: Xiangjun Liu, Guiling Wang, Panpan Xu,* Jiangtao Di, Qingwen Li
Affiliation: Suzhou Institute of Nano-tech and Nano-bionics

Title: Use of waste SNCR catalyst powder to produce Li4Ti5O12 anode material for lithium ion battery
Authors: Yenchun Liu
Affiliation: Graduate School of OptoMechatronics and Materials, WuFeng University, Chiayi 62153, Taiwan
Abstract: The titanium dioxide (TiO2) content in waste selective non-catalytic reduction (SNCR) catalyst powder is recycled using acid and is then baked, filtered, hydrolyzed and calcined to form TiO2 powder. The powder is structurally uniform with a particle size of 26 - 250 nm. The TiO2 powder is reacted with Li2CO3 to produce Li4Ti5O12 as an anode material for lithium ion batteries. Unreacted TiO2 is observed in the Li4Ti5O12 powder following sintering at 700°C for 12 hr. However, for higher sintering temperatures in the range of 800~900°C, the TiO2 disappears and is replaced by pure Li4Ti5O12 phase with a particle size of approximately 50 nm. The elemental composition of the Li4Ti5O12 powder is determined via energy dispersive spectroscopy (EDS) and inductively coupled plasma mass spectrometry (ICP-MS). Moreover, the crystalline phase is determined via X-ray diffraction (XRD). Finally, the surface morphology is observed using field emission scanning electron microscopy (FESEM). The Li4Ti5O12 powder is assembled into a button-type battery and subjected to cyclic charge-discharge tests. The maximum discharge capacity is found to be 152.66 mAh/g, and is obtained using the Li4Ti5O12 powder sintered at 850°C. The capacity retention performance (>95%) of this powder.

Title: Deep eutectic solvents (DES) assisted extraction of valuable metals from spent LiMnO2 cathode materials of Lithium-ion batteries
Authors: Jasreen Kaur Jasmel Singh; Masud Rana; Young-Tae Jo; Jeong-Hun Park*
Affiliation: Department of Environment and Energy Engineering, Chonnam National University, 77 Yongbong-ro, Buk-gu, Gwangju 61186, Republic of Korea
Abstract: As the world moves towards more sustainable modes of energy usages, rechargeable batteries typically lithium-ion batteries (LIBs) are widely used as energy storage. LIBs are favorable as it has great energy density which allows them to be lightweight. One of the main usages of LIBs is in the automotive field. It is expected that the demand of LIBs used in electric vehicles to be increase to 1.5 million metric tons per year by 2030 [1]. Hence, great emphasis and need will be placed on the recycling process of the lithium-ion batteries themself. The recycling process of these batteries should support a sustainable and circular economy. In this paper, it is aimed at using the idea of green chemistry of deep eutectic solvent (DES) to extract valuable metals of lithium (Li) and manganese (Mn) from spent Lithium Manganese batteries (LiMnO). DES will be used as a leachate to extract the valuable metals whereby it will be tested against the leaching efficiency, molar ratio, temperature, solid liquid ratio, time, presence of reducing agent. The leaching efficiency of Mn was found to be more than 90% leaching efficiency with operating parameters of DES 1:2 molar ratio, 1.5 of S/L ratio at 50C with optimum time of 1.5hr and under the present of glucose as reducing agent. (Li leaching efficiency with optimum parameters will be added later). XDR analysis of the black powder used before and after leaching were taken as well as the after leaching SEM images for the recovered products. The obtained results from this research shows that this DES mixture of ChCl:Latic Acid is able to leached out the Li and Mn from the spent lithium-ion batteries.

Title: Extraction Strategies from Black Alloy Leachate: A Comparative Study of Solvent Extractants
Authors: Namho Koo; Byungseon Kim; Hong-In Kim; Kyungjung Kwon
Affiliation: Korea Institute of Geoscience and Mineral Resources
Abstract: Recycling spent lithium-ion batteries (LIBs) is crucial to prevent environmental pollution and recover valuable metals. Traditional methods for recycling spent LIBs include hydrometallurgy and pyrometallurgy. Among these methods, solvent extraction can selectively extract valuable metals in spent LIB leachate. Meanwhile, spent LIBs underwent through pyrometallurgical treatment generate so-called a ‘black alloy’ of Ni, Co, Cu, and so on. These elements in black alloy need to be separated by solvent extraction and there have been few studies on extracting valuable metals for black alloy. Therefore, it is necessary to examine the extraction behavior of elements in black alloy and optimize the solvent extraction process to recover valuable metals. In this paper, four types of organic extractants are used to extract metals from simulated black alloy leachate: di-(2ethylhexyl) phosphoric acid (D2EHPA), bis-(2,4,4-trimethylpentyl) phosphinic acid (Cyanex272), 2-ethylhexyl phosphonic acid mono-2-ethylhexyl ester (PC88A), and neodecanoic acid (Versatic acid 10). Based on the pH isotherms, D2EHPA would be the most reasonable for Mn extraction and impurity removal. Cyanex 272 would be more suitable for Co separation than PC88A, and Versatic acid 10 is preferred for Cu extraction over other metals. In conclusion, the optimal combination of extractants is suggested for the recovery of valuable metals.

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