Lithium-Ion Battery Recycling

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

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

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: Comparison of element extraction behavior in pyrometallurgical treatment of spent lithium-ion batteries
Authors: Namho Koo1, Byungseon Kim1, Hong-in Kim2, Kyungjung Kwon1
Affiliation: 1 Department of Energy & Mineral Resources Engineering, Sejong University, Seoul 05006, Republic of Korea 2 Convergence Research Center for Development of Mineral Resources, Korea Institute of Geoscience and Mineral Resources, Daejeon 34132, Republic of Korea
Abstract: A growing demand for lithium-ion batteries (LIBs) has led to an increase in spent batteries. Consequently, recycling spent LIBs is crucial to prevent environmental pollution and recover valuable metals. Conventional methods for recycling spent LIBs include pyrometallurgy and hydrometallurgy. Among many hydrometallurgical techniques for LIB recycling, solvent extraction can selectively extract and concentrate valuable metals in the leachate of spent LIBs. Meanwhile, spent LIBs underwent through pyrometallurgical treatment generate so-called a ‘black alloy’ of Ni, Co, Cu, and so on. These elements in the black alloy need to be separated in the leachate of the alloy by solvent extraction. However, there have been few studies on extracting valuable metals for the black alloy to the best of our knowledge. A difference in the elemental composition between conventional black mass and black alloy makes it necessary to examine the extraction behavior of black alloy composition and optimize the process to recover valuable metals. In this paper, four types of organic extractants are used to extract valuable metals from the leachate: di-(2ethylhexyl) phosphoric acid (D2EHPA), bis-(2,4,4-trimethylpentyl) phosphinic acid (Cyanex272), 2-ethylhexyl phosphonic acid mono-2-ethylhexyl ester (PC88A), and 2-ethyl-2-methylheptanoic acid (Versatic 10). In conclusion, some impurities in the alloy exhibit a higher concentration than black mass, and the extraction behavior of various metals such as Ni, Co, Mn, Cu, Zn, Ca, and Mg are compared. It is confirmed that D2EHPA is useful for extracting Mn, and Cyanex272 is effective for extracting Co in the black alloy composition.