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Recycling and Reuse of End-of-Life Lithium-Ion Batteries: Challenges and Strategies
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Recycling and Reuse of End-of-Life Lithium-Ion Batteries: Challenges and Strategies

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

Deadline for manuscript submissions: 25 October 2024 | Viewed by 13504

Special Issue Editors

Dr. Chiara Ferrara

E-Mail Website
Guest Editor
Department of Materials Science, University of Milano-Bicocca, Via Roberto Cozzi, 55, 20125 Milano, MI, Italy
Interests: lithium- and sodium-ion battery materials; lithium-ion battery recycling; energy storage materials and devices
Prof. Dr. Elza Bontempi

E-Mail Website
Guest Editor
INSTM and Chemistry for Technologies Laboratory, Department of Mechanical and Industrial Engineering, University of Brescia, Via Branze 38, 25123 Brescia, Italy
Interests: spent lithium-ion batteries; raw materials recovery
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Lithium-ion batteries (LIBs) are electrochemical energy storage devices that have revolutionized our daily life since their commercialization, enabling the diffusion of portable devices and boosting the market of electric vehicles. Associated with their widespread application in several sectors, the inevitable consequence is an ever-growing volume of end-of-life lithium-ion batteries, which poses urgent challenges for the proper management of waste. Indeed, LIBs are complex and compact objects, containing a wide range of different materials (metal foils and wires, plastic cases and separators, oxide powders, organic solvents, salts, etc.). Moreover, the essential components of the batteries contain valuable critical raw materials, such as lithium, cobalt, and nickel; the recovery of such elements has the potential to form the basis of a beneficial circular economy scheme. Today, the available industrial technologies for LIB recycling are not able to satisfy the requirements for environmental sustainability and do not allow for the recovery of all the valuable elements; efforts are needed to identify new solutions in the complex sequence of steps following the disposal of waste LIBs, including proper sorting, discharging, dismantling, reuse, or recycling.

In this Special Issue, we present contributions addressing, but not limited to, these major topics, defining protocols and strategies, highlighting challenges, and identifying possible routes for the management of the various aspects involved in the recycling and reuse of lithium-ion batteries. The wide spectrum of topics and approaches considered here is necessary to fully address such a complex challenge. 

  • Protocols for pre-treatments, cell discharge, and cell disassembly at laboratory and industrial scale;
  • Protocols for the robust and fast analysis of the state of health and charge of the battery;
  • Processes and materials for the degradation of battery components (cathode, anode, electrolytes, and current collectors);
  • Processes and materials for the recovery of critical/strategical raw materials through the isolation of target elements via separation, precipitation, and filtration;
  • Upcycling and recycling of different components of waste lithium-ion batteries (cathode, anode, electrolytes, and current collectors);
  • Regeneration and healing of degraded battery components (cathode, anode, electrolytes, and current collectors) for their direct recycling;
  • Assessment of the environmental and economical sustainability of all the above-mentioned aspects;
  • New perspectives on the development of new-generation lithium-ion battery materials and design to enable easy recycling.

Dr. Chiara Ferrara
Prof. Dr. Elza Bontempi
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Batteries is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • end-of-life lithium-ion batteries
  • recycling
  • critical and strategical raw materials
  • second life
  • circular economy
  • sustainability

Published Papers (6 papers)

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Research

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15 pages, 13651 KiB  
Article
Electric Vehicle Battery Disassembly Using Interfacing Toolbox for Robotic Arms
by Alireza Rastegarpanah, Carmelo Mineo, Cesar Alan Contreras, Ali Aflakian, Giovanni Paragliola and Rustam Stolkin
Batteries 2024, 10(5), 147; https://doi.org/10.3390/batteries10050147 (registering DOI) - 27 Apr 2024
Viewed by 72
Abstract
This paper showcases the integration of the Interfacing Toolbox for Robotic Arms (ITRA) with our newly developed hybrid Visual Servoing (VS) methods to automate the disassembly of electric vehicle batteries, thereby advancing sustainability and fostering a circular economy. ITRA enhances collaboration between industrial [...] Read more.
This paper showcases the integration of the Interfacing Toolbox for Robotic Arms (ITRA) with our newly developed hybrid Visual Servoing (VS) methods to automate the disassembly of electric vehicle batteries, thereby advancing sustainability and fostering a circular economy. ITRA enhances collaboration between industrial robotic arms, server computers, sensors, and actuators, meeting the intricate demands of robotic disassembly, including the essential real-time tracking of components and robotic arms. We demonstrate the effectiveness of our hybrid VS approach, combined with ITRA, in the context of Electric Vehicle (EV) battery disassembly across two robotic testbeds. The first employs a KUKA KR10 robot for precision tasks, while the second utilizes a KUKA KR500 for operations needing higher payload capacity. Conducted in T1 (Manual Reduced Velocity) mode, our experiments underscore a swift communication protocol that links low-level and high-level control systems, thus enabling rapid object detection and tracking. This allows for the efficient completion of disassembly tasks, such as removing the EV battery’s top case in 27 s and disassembling a stack of modules in 32 s. The demonstrated success of our framework highlights its extensive applicability in robotic manufacturing sectors that demand precision and adaptability, including medical robotics, extreme environments, aerospace, and construction. Full article
(This article belongs to the Special Issue Recycling and Reuse of End-of-Life Lithium-Ion Batteries: Challenges and Strategies)
14 pages, 2280 KiB  
Article
Advances in the Separation of Graphite from Lithium Iron Phosphate from End-of-Life Batteries Shredded Fine Fraction Using Simple Froth Flotation
by Olivier Renier, Andrea Pellini and Jeroen Spooren
Batteries 2023, 9(12), 589; https://doi.org/10.3390/batteries9120589 - 13 Dec 2023
Cited by 1 | Viewed by 2227
Abstract
Olivine-type lithium iron phosphate (LiFePO4, LFP) lithium-ion batteries (LIBs) have become a popular choice for electric vehicles (EVs) and stationary energy storage systems. In the context of recycling, this study addresses the complex challenge of separating black mass of spent LFP [...] Read more.
Olivine-type lithium iron phosphate (LiFePO4, LFP) lithium-ion batteries (LIBs) have become a popular choice for electric vehicles (EVs) and stationary energy storage systems. In the context of recycling, this study addresses the complex challenge of separating black mass of spent LFP batteries from its main composing materials to allow for direct recycling. In this study, 71% copper and 81% aluminium foil impurities were removed by sieving black mass to <250 µm. Next, the application of froth flotation as a separation technique was explored, examining the influence of chemical agents, pre-treatment, and multi-step processes. Frother agent addition improved material recovery in the froth, while collector addition influenced the separation efficiency and enhanced graphite recovery. Pre-treatment, particularly sonication, was found to break down agglomerates and further improve separation. Multi-step flotation increased the purity of recovered fractions. The optimized process for a black mass < 250 µm, involving sonication pre-treatment and double flotation, resulted in enriched carbonaceous material (80.3 mol%) in froth fractions and high LFP concentration (81.9 mol%) in tailings fractions. The recovered spent LFP cathode material contained 37.20 wt% Fe2P2O7, a degradation product of LiFePO4. This research offers valuable insights for the development of efficient battery recycling methods for LFP batteries. Full article
(This article belongs to the Special Issue Recycling and Reuse of End-of-Life Lithium-Ion Batteries: Challenges and Strategies)
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17 pages, 1567 KiB  
Article
State of Health Assessment of Spent Lithium–Ion Batteries Based on Voltage Integral during the Constant Current Charge
by Ote Amuta and Julia Kowal
Batteries 2023, 9(11), 537; https://doi.org/10.3390/batteries9110537 - 28 Oct 2023
Viewed by 1545
Abstract
Lithium–ion batteries (LIBs) are used in many personal electronic devices (PED) and energy-demanding applications such as electric vehicles. After their first use, rather than dispose of them for recycling, some may still have reasonable capacity and can be used in secondary applications. The [...] Read more.
Lithium–ion batteries (LIBs) are used in many personal electronic devices (PED) and energy-demanding applications such as electric vehicles. After their first use, rather than dispose of them for recycling, some may still have reasonable capacity and can be used in secondary applications. The current test methods to assess them are either slow, complex or expensive. The voltage integral during the constant current (CC) charge of the same model of LIBs strongly correlates with the state of health (SOH) and is faster than a full capacity check. Compared to the filtering requirement in the incremental capacity (IC) and differential voltage (DV) or the complex analysis in the electrochemical impedance spectrum (EIS), the voltage integral offers a simple integration method, just like the simple capacity Coulomb’s counter that is installed in many BMS for estimating the SOC of LIBs. By obtaining the voltage integral of a relatively new cell and an old cell of the same model with known SOH at a given ambient temperature and CC charge, the SOH of other similar cells can be easily estimated by finding their voltage integrals. Full article
(This article belongs to the Special Issue Recycling and Reuse of End-of-Life Lithium-Ion Batteries: Challenges and Strategies)
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16 pages, 7195 KiB  
Article
The Investigation of Triple-Lithiated Transition Metal Oxides Synthesized from the Spent LiCoO2
by Alexandra Kosenko, Konstantin Pushnitsa, Vladislav Chernyavsky, Pavel Novikov and Anatoliy A. Popovich
Batteries 2023, 9(8), 423; https://doi.org/10.3390/batteries9080423 - 12 Aug 2023
Viewed by 1014
Abstract
The environmentally friendly closed cycle of the regeneration process of spent LiCoO2 was successfully developed and the following synthesis of triple-lithiated transition metal oxides was carried out. A hydrometallurgy recycling route with the usage of 1.5 mol/L of malic acid and 3 [...] Read more.
The environmentally friendly closed cycle of the regeneration process of spent LiCoO2 was successfully developed and the following synthesis of triple-lithiated transition metal oxides was carried out. A hydrometallurgy recycling route with the usage of 1.5 mol/L of malic acid and 3 vol.% of H2O2 as a leaching solution for cobalt extraction was chosen. The efficiency of the cobalt extraction reached 95%. The obtained material was investigated using an X-ray diffraction analysis and the EDX and SEM methods. The electrochemical behavior of the synthesized NCM111 was analyzed and compared to the commercially available material of the same type. The material demonstrated a specific discharge capacity on the first cycle of 163.7 mAh/g. The cyclic resource of the material turned out to be unsatisfactory. In addition, perspective cathode materials, such as NCM622 and NCM811, were obtained. The synthesized materials were analyzed using XRD, SEM, EDX, charge–discharge and cycle life tests, and the CVA and EIS methods. The initial specific discharge capacities of the NCM622 and NCM811 were 168 and 187 mAh/g, respectively. On the fifth cycle, the NCM622 demonstrated an increasing capacity—to 179 mAh/g, unlike NCM811, as the capacity of this material decreased to 141 mAh/g. Full article
(This article belongs to the Special Issue Recycling and Reuse of End-of-Life Lithium-Ion Batteries: Challenges and Strategies)
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Review

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40 pages, 10284 KiB  
Review
A Review of the Technical Challenges and Solutions in Maximising the Potential Use of Second Life Batteries from Electric Vehicles
by Farhad Salek, Shahaboddin Resalati, Meisam Babaie, Paul Henshall, Denise Morrey and Lei Yao
Batteries 2024, 10(3), 79; https://doi.org/10.3390/batteries10030079 - 27 Feb 2024
Cited by 2 | Viewed by 1564
Abstract
The increasing number of electric vehicles (EVs) on the roads has led to a rise in the number of batteries reaching the end of their first life. Such batteries, however, still have a capacity of 75–80% remaining, creating an opportunity for a second [...] Read more.
The increasing number of electric vehicles (EVs) on the roads has led to a rise in the number of batteries reaching the end of their first life. Such batteries, however, still have a capacity of 75–80% remaining, creating an opportunity for a second life in less power-intensive applications. Utilising these second-life batteries (SLBs) requires specific preparation, including grading the batteries based on their State of Health (SoH); repackaging, considering the end-use requirements; and the development of an accurate battery-management system (BMS) based on validated theoretical models. In this paper, we conduct a technical review of mathematical modelling and experimental analyses of SLBs to address existing challenges in BMS development. Our review reveals that most of the recent research focuses on environmental and economic aspects rather than technical challenges. The review suggests the use of equivalent-circuit models with 2RCs and 3RCs, which exhibit good accuracy for estimating the performance of lithium-ion batteries during their second life. Furthermore, electrochemical impedance spectroscopy (EIS) tests provide valuable information about the SLBs’ degradation history and conditions. For addressing calendar-ageing mechanisms, electrochemical models are suggested over empirical models due to their effectiveness and efficiency. Additionally, generating cycle-ageing test profiles based on real application scenarios using synthetic load data is recommended for reliable predictions. Artificial intelligence algorithms show promise in predicting SLB cycle-ageing fading parameters, offering significant time-saving benefits for lab testing. Our study emphasises the importance of focusing on technical challenges to facilitate the effective utilisation of SLBs in stationary applications, such as building energy-storage systems and EV charging stations. Full article
(This article belongs to the Special Issue Recycling and Reuse of End-of-Life Lithium-Ion Batteries: Challenges and Strategies)
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30 pages, 6366 KiB  
Review
A Review of Lithium-Ion Battery Recycling: Technologies, Sustainability, and Open Issues
by Alessandra Zanoletti, Eleonora Carena, Chiara Ferrara and Elza Bontempi
Batteries 2024, 10(1), 38; https://doi.org/10.3390/batteries10010038 - 22 Jan 2024
Cited by 1 | Viewed by 6024
Abstract
Lithium-ion batteries (LIBs) are a widely used energy storage technology as they possess high energy density and are characterized by the reversible intercalation/deintercalation of Li ions between electrodes. The rapid development of LIBs has led to increased production efficiency and lower costs for [...] Read more.
Lithium-ion batteries (LIBs) are a widely used energy storage technology as they possess high energy density and are characterized by the reversible intercalation/deintercalation of Li ions between electrodes. The rapid development of LIBs has led to increased production efficiency and lower costs for manufacturers, resulting in a growing demand for batteries and their application across various industries, particularly in different types of vehicles. In order to meet the demand for LIBs while minimizing climate-impacting emissions, the reuse, recycling, and repurposing of LIBs is a critical step toward achieving a sustainable battery economy. This paper provides a comprehensive review of lithium-ion battery recycling, covering topics such as current recycling technologies, technological advancements, policy gaps, design strategies, funding for pilot projects, and a comprehensive strategy for battery recycling. Additionally, this paper emphasizes the challenges associated with developing LIB recycling and the opportunities arising from these challenges, such as the potential for innovation and the creation of a more sustainable and circular economy. The environmental implications of LIB recycling are also evaluated with methodologies able to provide a sustainability analysis of the selected technology. This paper aims to enhance the comprehension of these trade-offs and encourage discussion on determining the “best” recycling route when targets are in conflict. Full article
(This article belongs to the Special Issue Recycling and Reuse of End-of-Life Lithium-Ion Batteries: Challenges and Strategies)
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