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Nowadays, Lithium-ion batteries (LIBs) have dominated the power source market in a variety of applications. Lithium cobalt oxide (LiCoO2) is one of the most common cathode materials for LIBs in consumer electronics. The recycling of LIBs is important because cobalt is an expensive element that is dependent on foreign sources for production. Lithium-ion batteries need to be recycled and disposed properly when they reach the end of life (EOL) to avoid negative environmental impact. This project focuses on recycling cathode material (LiCoO2) by direct method. Two automation stages, tape peeling stage and unrolling stage, are designed for disassembling prismatic winding cores. Different sintering conditions (e.g., temperature, sintering atmosphere, the amount of lithium addition) are investigated to recycle EOL cathode materials. The results show that the capacity of the recycled cathode materials increases with increasing temperature. The extra Li addition leads to worse cycling performance. In addition, the sintering atmosphere has little influence on small- scale sintering. Also, most of directly recycled cathode materials have better electrochemical (EC) performance than commercial LiCoO2 (LCO) from Sigma, especially when cycling with 4.45V cutoff voltage. / Master of Science / Nowadays, Lithium-ion batteries (LIBs) have dominated the power source market in a variety of applications. A LIB contains an anode, a cathode and electrolyte. The cathode material is the most valuable component in the LIB. Lithium cobalt oxide (LiCoO2) is one of the most common cathode materials for LIBs in consumer electronics. The recycling of LIBs is important because cobalt is an expensive element that is dependent on foreign sources for production. Lithium-ion batteries need to be recycled and disposed properly when they reach end of life (EOL) to avoid negative environmental impact. The direct recycling is a cost effective and energy conservative method which can be divided into two steps: retrieving the cathode materials from EOL LIBs and regenerating the cathode materials. This project focuses on recycling LiCoO2 by direct method. Two automation modules, tape peeling stage and unrolling stage, are designed for a disassembling line which is the automation line to collect the cathodes materials. The EOL cathode materials is lithium deficient (Li1-xCoO2). To regenerate the EOL cathode materials, lithium is added into structure of cathode materials which is called the re-lithiation process. The different sintering conditions (e.g., temperature, sintering atmosphere, the amount of lithium addition) are investigated for the re-lithiation process. The results show that the capacity of the recycled cathode materials increases with increasing temperature. The extra Li addition in iv Li1-xCoO2 leads to worse cycling performance. In addition, sintering atmosphere has little influence on small- scale sintering. Most of directly recycled cathode materials have better electrochemical (EC) performance than commercial LiCoO2, especially when cycling with 4.45V cutoff voltage.

"A ¡°mixed cathodes¡± LIB recycling process was first proposed and developed in the CR3 center at Worcester Polytechnic Institute. This process can efficiently and economically recover all the valuable metal elements in LIB waste. In the end of the recovery process, lithium, nickel, manganese, and cobalt ions will be recovered in the leaching solution. The objective of this work is to utilize the leaching solution to synthesis NixMnyCoz(OH)2 precursors and their corresponding LiNixMnyCozO2 cathode materials. The synthesized cathode materials can be used to build new LIBs, allowing the overall process to be a ¡°closed loop¡±. "

According to the International Energy Agency, the global Electric Vehicle (EV) sales are experiencing approximately 24% annual growth and the total market could reach 4 million in 2020 and 21.5 million by 2030. However, the mass production of lithium-ion batteries (LIBs) to power EV creates concerns over environmental impacts and the long-term sustainability of critical elements for producing the major battery components. Although much investment has been made, it is still imperative to develop an effective LIB production and recycling process. This dissertation demonstrates a green and sustainable paradigm for LIBs where the batteries are manufactured and direct recycled to form a closed loop. The water-based cathode electrode delivers comparable cycle life and rate performance to the ones from the conventional organic solvent-based process. The direct recycling process has the advantages to regenerate the cathode material from electrode instead of decomposing into elements. Utilization of a water-soluble binder enables separating the cathode compound from spent electrodes using water, which is then successfully regenerated to deliver comparable electrochemical performance to the pristine one. When scaled up, the degraded cathode material can be directly regenerated by an optimized relithiation thermal synthesis (RTS) method to resynthesize the homogeneous cathode powder of high quality. The key factors and sintering procedures are studied to ensure the performance of the product. The pilot scale test successfully scales up to Kg-level with recycled output materials delivering good electrochemical performance. To automate the direct recycling process and improve the efficiency, machine learning and sensors are utilized in a novel battery disassembly platform. It can classify different batteries based on their types and sizes. The processing temperature is instantly monitored using thermal imager, and the prediction model is trained to give the prediction for measures taken by a closed loop control system. Furthermore, the image recognition is employed for quality control after the cutting process and the defect can be mitigated to ensure effective dismantling of End-of-life (EOL) batteries. The integration of machine learning techniques makes the elaborate dismantling process safer and more efficient. / Doctor of Philosophy / According to the International Energy Agency, the global Electric Vehicle (EV) sales are experiencing approximately 24% annual growth and the total market could reach 4 million in 2020 and 21.5 million by 2030. However, the mass production of lithium-ion batteries (LIBs) to power EV creates concerns over environmental impacts and the long-term sustainability of critical elements for producing the major battery components. In this work, a green and sustainable manufacturing and recycling paradigm for LIBs is ushered and scaled up to pilot-scale test. Compared with the electrodes produced by conventional organic solvent-based process, the water-based electrodes can deliver comparable battery performance, meanwhile reduce the cost as well as the pollution to environment. The spent batteries are successfully regenerated to form the closed loop system with minimal external toxic solvent used. At pilot-scale, Kg-level battery material can be directly regenerated to deliver high-quality cathode powder. It provides the guidance of design parameters for large-scale battery recycling in industry. To automate the direct recycling process and improve the efficiency, machine learning and sensors are utilized in a novel battery disassembly platform. The integration of machine learning techniques makes the elaborate dismantling process safer and more efficient.

End-of-life lithium-ion batteries retired from portable electronics, electric vehicles (EVs), and power grids need to be properly recycled to save rare earth metals and avoid any hazardous threats to the environment. The recycling process of a Lithium-ion Battery Cell/Module includes storage, transportation, deactivation, disassembly, and material recovery. This study focused on the disassembly step and proposed a systematic method to recover cathode active coating, which is considered the most valuable component of a LIB, from end-of-life LIB pouch cells. A semi-destructive disassembly sequence is developed according to the internal structure of the LIB cell. A fully automated disassembly line aiming at extracting cathode electrodes is designed, modeled, prototyped, and demonstrated based on the disassembly sequence. In order to further obtain the coating material, the extracted cathode electrodes are treated with the organic solvent method and the relationship between process parameters and cathode coating separation yield is numerically studied with the help of Design of Experiment (DOE). Regression models are then fitted from the DOE result to predict the cathode coating separation yield according to combinations of the process parameters. The single cell material separation methodology developed in this study plays an important role in the industrial application of the direct recycling method that may dominate the battery recycling market due to its environmental friendly technology and high recovery rate regardless of element type in the short future. / Doctor of Philosophy / The bursting demand of lithium-ion batteries from portable electronics, electric vehicles, and power grids in the past few years not only facilitate the booming of the lithium-ion battery market, but also put forward serious global concerns: Where should these batteries go at their end-of life and how should they be treated in a safe and harmless manner. As a metal enriched "city mine", end-of-life LIBs are expected to be properly stored, transported, deactivated, disassembled, and recovered with sufficient safety precautions to prevent fire, explosion or any hazardous emissions. This study focuses on the disassembly procedure and emphasized automated battery disassembly techniques and the improving of material separation efficiency. A disassembly sequence of the pouch cell is scheduled and optimized for the first time. To realize the scheduled sequence, a fully automated pouch cell disassembly system is designed to achieve semi-destructive disassembly of z-folded pouch cells. Fixtures, transporters and end-effectors were prototyped and assembled into the modularized disassembly line which extracts cathode electrodes as final product. Cathode electrodes as the most valuable component in a LIB then need to go through multiple chemical-mechanical treatments to future separate cathode coating and Al current collector. This study utilized DOEs to optimize the operating parameters of the material separation process for Lithium cobalt oxide (LCO) coating and Lithium iron phosphate (LFP) coating. Regression models are successfully established for yield prediction with certain levels of control factors.

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This report explores simultaneous crystallization in multicomponent solutions to intensification of metal recovery in lithium-ion batteries. The main focus is to evaluate and compare the efficiency of sodium hydroxide and sodium carbonate as precipitating agents in recovering cobalt, nickel, manganese and lithium. To be able to do this, 15 different metal systems were precipitated with these two precipitating agents at 8 and 12 molar equivalent. The samples were then analyzed through ICP-OES, XRD, gravimetric analysis, and SEM-EDX. The results showed that the precipitation efficiency of the transition metals cobalt, nickel and manganese, in all the system was 98% or more. Lithium precipitated only with carbonate. In the system with four metals and 12 molar equivalents carbonate lithium 78% was precipitated. The results indicate that higher concentration of carbonate leads to higher precipitation efficiency. A way to likely reach a higher effective concentration is to first neutralize the solution with sodium hydroxide and then precipitate it with carbonate.

<p dir="ltr">Vehicle electrification has been proposed as one of the most important technologies for the future of sustainable energy and climate change mitigation. These electric vehicles (EVs) are predominantly powered by lithium-ion batteries (LIBs) which contain critical materials — lithium (Li), cobalt (Co), nickel (Ni), manganese (Mn), and graphite — that are in short supply. Maximizing resource efficiency through material recovery is crucial for a circular economy and the long-term financial, environmental, and social sustainability of the EV industry.</p><p><br></p><p dir="ltr">Heavily influenced by technology, business, and policy, the EV ecosystem must balance the interests of multiple stakeholders. There is a system-of-systems dependency between the circular business model employed; the process, scale, and impact of operations; and the overall economy of the operating environment. However, these linkages are highly dependent on the technological process for material recovery. Given that proof-of-concept research methodologies in the academy are typically low-complexity technologies (low-tech) and at a low technological readiness level (TRL), economies of scale, environmental impacts, and policy implications are not readily deduced.</p><p><br></p><p dir="ltr">Two practical low-tech and low TRL methods for cathode material recovery and cell reattachment for extended battery usage were developed as proofs-of-concept. One theoretical approach for cell removal using heat application was also explored. Given that artisanal mining plays a significant role in the upstream battery material supply chain and is often carried out on a small scale with common tools, safe manual disassembly processes through low-tech, low TRL methods for environmentally friendly battery material recovery could be influential in the downstream management of end-of-life (EOL) EVs.</p><p><br></p><p dir="ltr">Another recommendation is to treat lithium-ion batteries and current recycling methods as transitory technologies, thus encouraging investments in low-tech methods as part of effective business practices today. Vertical integration and supply chain partnerships by companies to recover legacy batteries could be more beneficial in the short term than investing large amounts of capital in new recycling facilities of whose features they are unsure. Higher-complexity and TRL methods can be developed as part of new growth engines for future businesses.</p><p dir="ltr">Finally, the major policy observation is the recognition that state level involvement in setting up appealing environments for private companies is a major contributor to attracting investments for local economic growth, thus necessitating the need for stronger multistakeholder engagement and collaboration in workforce development and environmental safety. Without adequate workforce development and retention programs, companies will struggle to meet and keep the labor requirements necessary to take advantage of tax credits, which could hinder their desire to set up shop in certain states.</p>

Data visualisation can provide a user-friendly way to observe and understand data. It can make is easier to make well-informed decision and communicate findings in data. This study aims to research how to effectively structure and visualize a complex data sets in order to improve a battery discharge process. By implementing a dashboard and visualising a data set from electrical battery discharging, the following objectives are considered; analyse and identify which parameters and variables are most important in the battery discharging process. Analyse how data transformation and cleaning can support data visualisations. Define an interface that visualises the trends, anomalies and correlations of the data set. Evaluate how the visual representation is perceived by users in the battery recycling process?The study followed the User Centered Design method, which consist of five phases that are iterated. During the phases Identify needs and Specify context of use six stake holder interviews was held, theses were analysed through an Affinity diagram and Personas. In the phase Specify requirements requirements are established by conducting a user journey mapping. The data and insights from the previous phases was turned into ideas and solutions in the phase Produce design solutions. In total three low-fidelity and one high-fidelity prototype were created, as well as one implemented solution. In the last phase Evaluate design the design solutions were tested though, interviews, usability test and a survey. The result of the study strengthens the theory that data visualisations can be used to provide insights. The findings show that visualisation to some extent could help detect abnormalities, patterns and correlation between variables, which could be useful in improving a process.

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