This paper defines terms such as "recycling rate" that enable the characterization of flows of battery materials and expands the terminology to accommodate the description of complex product recycling. It also estimates the maximum percentage of U.S. demand for critical elements that could be satisfied by recycling as demand continues to grow, and it defines and estimates the recycling rate for lithium-ion batteries. Finally, it clarifies the role of manufacturing scrap as the domestic U.S. supply chain is built up. It concludes that recycling will be important in the long term, but growth still requires that new material be extracted to supply additional material.

The market dynamics, and their impact on a future circular economy for lithium-ion batteries (LIB), are presented in this roadmap, with safety as an integral consideration throughout the life cycle. At the point of end-of-life (EOL), there is a range of potential options—remanufacturing, reuse and recycling. Diagnostics play a significant role in evaluating the state-of-health and condition of batteries, and improvements to diagnostic techniques are evaluated. At present, manual disassembly dominates EOL disposal, however, given the volumes of future batteries that are to be anticipated, automated approaches to the dismantling of EOL battery packs will be key. The first stage in recycling after the removal of the cells is the initial cell-breaking or opening step. Approaches to this are reviewed, contrasting shredding and cell disassembly as two alternative approaches. Design for recycling is one approach that could assist in easier disassembly of cells, and new approaches to cell design that could enable the circular economy of LIBs are reviewed. After disassembly, subsequent separation of the black mass is performed before further concentration of components. There are a plethora of alternative approaches for recovering materials; this roadmap sets out the future directions for a range of approaches including pyrometallurgy, hydrometallurgy, short-loop, direct, and the biological recovery of LIB materials. Furthermore, anode, lithium, electrolyte, binder and plastics recovery are considered in order to maximise the proportion of materials recovered, minimise waste and point the way towards zero-waste recycling. The life-cycle implications of a circular economy are discussed considering the overall system of LIB recycling, and also directly investigating the different recycling methods. The legal and regulatory perspectives are also considered. Finally, with a view to the future, approaches for next-generation battery chemistries and recycling are evaluated, identifying gaps for research. This review takes the form of a series of short reviews, with each section written independently by a diverse international authorship of experts on the topic. Collectively, these reviews form a comprehensive picture of the current state of the art in LIB recycling, and how these technologies are expected to develop in the future.

Many countries have started their transition to a net-zero economy. Lithium-ion batteries (LIBs) play an ever-increasing role towards this transition as a rechargeable energy storage medium. Initially, LIBs were developed for consumer electronics and portable devices but have seen dramatic growth in their use in electric vehicles (EVs) and via the gradual uptake in battery energy storage systems (BESSs) over the last decade. As such, critical metals (Li, Co, Ni, and Mn) and chemicals (polymers, electrolytes, Cu, Al, PVDF, LiPF6, LiBF4, and graphite) needed for LIBs are currently in great demand and are susceptible to global supply shortages. Dramatic increases in raw material prices, coupled with predicted exponential growth in global demand (e.g., United States graphite demand from 2022 7000 t to ~145,000 t), means that LIBs will not be sustainable if only sourced from raw materials. LIBs degrade over time. When their performance can no longer meet the requirement of their intended application (e.g., EVs in the 8–12 year range), opportunities exist to extract and recover battery materials for re-use in new batteries or to supply other industrial chemical sectors. This paper compares the challenges, barriers, opportunities, and successes of the United States of America and Australia as they transition to renewable energy storage and develop a battery supply chain to support a circular economy around LIBs.

The grey dashed line in Fig. 1a has been replaced.-The sentence "As a result of the potentially fast growing LFP industry, light-duty EVs alone could consume as much phosphorus as is currently produced for industrial purposes globally in as little as 15-20 years from now (Fig. 1a)." in the main text has been replaced with "As a result of the potentially fast growing LFP industry, light-duty EVs alone could consume as much phosphorus as is currently produced for industrial purposes globally in as little as 20-25 years from now (Fig. 1a).

Having transformed our way of life, rechargeable batteries are poised for exponential growth over the coming decade, notably due to the wider adoption of electric vehicles. An international expert panel proposes a combination of vision, innovation and practice for feasible pathways toward sustainable batteries.

Although the US has minimal reserves of the raw materials needed to make EV batteries, EOL material can contribute to domestic supply. However, this valuable resource will be exported if it is not economical to recycle it here. Hydrometallurgical recycling plants are being built now, with the expectation that they will be profitable, but profits will decline with cobalt content. By the time that happens, direct recycling will be sufficiently developed to take up the slack. Both processes will then be available to upgrade recovered materials to more up-to-date chemistries, securing a domestic supply of these materials.

The ReCell Center was established by the US Department of Energy’s Vehicle Technologies Office to develop a practical process for recycling of lithium-ion batteries. But if a recycling process is actually going to be adopted by industry, it must be economical. And since a main motivation for electric vehicles is environmental, the process must be “green” as well. Therefore, early in their development, ReCell processes are subjected to careful technical and economic analysis, using our publicly available and award-winning EverBatt model, to verify that they will be economical and environmentally friendly. This presentation will describe processes under development and illustrate the use of technical and economic analysis to evaluate them and compare them to alternatives.

The expected rapid growth in electric vehicle deployment will inevitably be followed by a corresponding rise in the supply of end-of-life vehicles and their lithium-ion batteries (LIBs). The batteries may be reused, but will eventually be spent and provide a potential domestic resource that can help supply materials for future battery production. However, commercial recycling processes depend on profits from recovery of cobalt, use of which is being reduced in new cathode chemistries. The U.S. Department of Energy, therefore, established the ReCell Center in early 2019 to develop robust LIB recycling technology that would be economical even for batteries that contain no cobalt. The central feature of the technology is recovery of the cathode material with its unique crystalline cathode morphology intact in order to retain its value and functionality. Other materials are recovered as well in order to maximize revenues and minimize waste-handling costs. Analysis and modeling serve to evaluate and compare process options so that we can identify those that will be most economical while still minimizing energy use and environmental impacts. This paper provides background and describes highlights of the center's first 2 years of operation.

Rapid growth in the market for electric vehicles is imperative, to meet global targets for reducing greenhouse gas emissions, to improve air quality in urban centres and to meet the needs of consumers, with whom electric vehicles are increasingly popular. However, growing numbers of electric vehicles present a serious waste-management challenge for recyclers at end-of-life. Nevertheless, spent batteries may also present an opportunity as manufacturers require access to strategic elements and critical materials for key components in electric-vehicle manufacture: recycled lithium-ion batteries from electric vehicles could provide a valuable secondary source of materials. Here we outline and evaluate the current range of approaches to electric-vehicle lithium-ion battery recycling and re-use, and highlight areas for future progress.

Product design is an important factor which can control the efficiency and economics of a recycling flowsheet.

Recycling is not an objective in itself, but for the benefits it can bring, including reductions in life-cycle costs, energy use and environmental impacts, and dependence on scarce or imported materials. Because the options available now for recycling of lithium-ion batteries are not optimal, the U.S. Department of Energy announced its Battery Recycling R&D Center (and the Recycling Prize) in January 2019 to develop an economical recycling process by the time large volumes of batteries from electric vehicles and other uses reach end of life. The ReCell center is based at lead-lab Argonne National Laboratory, and includes partner labs Oak Ridge and NREL, and several universities.Even batteries that find second use will eventually need to be recycled. However, by then the material could be a 20 year-old formulation with little residual value from its structure or contained elements. In particular, cathodes are evolving towards formulations containing reduced quantities of cobalt (the valuable element sought in most current recycling operations), reducing the incentive for recycling with standard pyrometallurgical or hydrometallurgical methods.Many R&D questions focus on recovering usable cathode, which is the most valuable form of recoverable material. How can the cathode get separated from the other cell components and restored to full functionality? Can we separate one cathode type from another? Can we modify the cathode composition or morphology to update it for reuse? Can other materials be recovered as well? This presentation will describe progress that has been made to address these questions during the ReCell centeru2019s first year of operation.

The world is shifting to electric vehicles to mitigate climate change. Here, we quantify the future demand for key battery materials, considering potential electric vehicle fleet and battery chemistry developments as well as second-use and recycling of electric vehicle batteries. We find that in a lithium nickel cobalt manganese oxide dominated battery scenario, demand is estimated to increase by factors of 18–20 for lithium, 17–19 for cobalt, 28–31 for nickel, and 15–20 for most other materials from 2020 to 2050, requiring a drastic expansion of lithium, cobalt, and nickel supply chains and likely additional resource discovery. However, uncertainties are large. Key factors are the development of the electric vehicles fleet and battery capacity requirements per vehicle. If other battery chemistries were used at large scale, e.g. lithium iron phosphate or novel lithium-sulphur or lithium-air batteries, the demand for cobalt and nickel would be substantially smaller. Closed-loop recycling plays a minor, but increasingly important role for reducing primary material demand until 2050, however, advances in recycling are necessary to economically recover battery-grade materials from end-of-life batteries. Second-use of electric vehicles batteries further delays recycling potentials.

Recycling of spent lithium-ion batteries (LIBs) is an urgent need to address their environmental and global sustainability issues. Here, we report an efficient and environmentally benign LIB regeneration method based on defect- targeted healing, which represents a paradigm-shift LIB recycling strategy. Specifically, by combining lowtemperature aqueous solution relithiation and rapid post-annealing, we demonstrate successful direct regeneration of spent LiFePO4 (LFP) cathodes, one of the most important materials for EVs and grid storage applications. We show revitalization of composition, structure, and electrochemical performance of LFP with various degradation conditions to the same levels as the pristine LFP. Life-cycle analysis of different LIB recycling processes shows that this defect-targeted direct reycling approach can significantly reduce energy usage and greenhouse gas (GHG) emissions, leading to more economic and environmental benefits compared with today's hydrometallurgical and pyrometallurgical methods.

Direct recycling of lithium-ion is a promising method for manufacturing sustainability. It is more efficient than classical methods because it recovers the functional cathode particle without decomposition into substituent elements or dissolution and precipitation of the whole particle. This case study of cathode-healing™ applied to a battery recall demonstrates an industrial model for recycling of lithium-ion, be it consumer electronic or electric vehicle (EV) batteries. The comprehensive process includes extraction of electrolyte with carbon dioxide, industrial shredding, electrode harvesting, froth flotation, cathode-healing™ and finally, building new cells with recycled cathode and anode. The final products demonstrated useful capability in the first full cells made from direct recycled cathodes and anodes from an industrial source. The lessons learned on recycling the prototypical chemistry are preliminarily applied to EV relevant chemistries.

The number of plug-in electric vehicles sold in the U.S. has grown from 52,500 units in 2012 to over 160,000 vehicles sold in 2016; that is over a 300% increase in just four years. These vehicles’ batteries are going to reach auto dismantlers after approximately 10 years and require proper end-of-life processing, but the current solutions are not cost-effective. Argonne National Laboratory has developed a model that evaluates every stage of a battery’s life from material acquisition through recycling to provide a total cost and environmental impact. This allows for a direct comparison of virgin batteries to batteries with recycled content.

In light of the increasing penetration of electric vehicles (EVs) in the global vehicle market, understanding the environmental impacts of lithium-ion batteries (LIBs) that characterize the EVs is key to sustainable EV deployment. This study analyzes the cradle-to-gate total energy use, greenhouse gas emissions, SOx, NOx, PM10 emissions, and water consumption associated with current industrial production of lithium nickel manganese cobalt oxide (NMC) batteries, with the battery life cycle analysis (LCA) module in the Greenhouse Gases, Regulated Emissions, and Energy Use in Transportation (GREET) model, which was recently updated with primary data collected from large-scale commercial battery material producers and automotive LIB manufacturers. The results show that active cathode material, aluminum, and energy use for cell production are the major contributors to the energy and environmental impacts of NMC batteries. However, this study also notes that the impacts could change significantly, depending on where in the world the battery is produced, and where the materials are sourced. In an effort to harmonize existing LCAs of automotive LIBs and guide future research, this study also lays out differences in life cycle inventories (LCIs) for key battery materials among existing LIB LCA studies, and identifies knowledge gaps.

The rapidly growing fleet of electric vehicles contributes to transforming transport but presents challenges for managing spent lithium-ion batteries in the coming decades. Recently in Joule, Chen et al. reviewed the advantages and limitations of existing lithium-ion-battery recycling processes. To scale rapidly, recycling must be profitable, even for low-cobalt batteries.

The electric vehicle and energy storage industries will generate over one-million tons per annum of lithium-ion for recycling in the next decade. There are significant technology gaps in the recovery of lithium-ion battery materials that threaten the sustainability of these industries. Cathode healing is introduced here as a new approach to produce low cost (i.e. < $10/kg), recycled, battery grade electrode material. The soft-chemical treatment non-destructively recycles cathodes. Two examples are shown in this work: LiNi0.5Co0.2Mn0.3O2 and LiNi0.6Co 0.2Mn0.2O2 (NCM 523 and NCM 622). The cathodes were harvested from end-of-life cells and further processed with cathode-healing methods to reproduce recycled electrodes with performance equivalent to the original manufactured baseline material. The so-called healed cathodes were built into 2Ah test cells and compared side-by-side with the baseline. Healed NCM 523 performed like the baseline, recording over 2,100 charge-discharge cycles to reach 80% of original capacity. The cathode healing process was modified to fully recover end-of-life NCM 622. Powder X-ray diffraction and X-ray photoelectron spectroscopy data support the lithium capacity measurements with structural models. These analyses show that cathode healing reverses cation mixing by oxidizing nickel to reproduce well-ordered, high-capacity material. These examples show the technical feasibility and low-cost opportunity for cathode healing to enable sustainability in the electric vehicle and energy storage industries.