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.

Due to the increasing demand for battery raw materials such as cobalt, nickel, manganese, and lithium, the extraction of these metals not only from primary, but also from secondary sources like spent lithium-ion batteries (LIBs) is becoming increasingly important. One possible approach for an optimized recovery of valuable metals from spent LIBs is a combined pyro- and hydrometallurgical process. According to the pyrometallurgical process route, in this paper, a suitable slag design for the generation of slag enriched by lithium and mixed cobalt, nickel, and copper alloy as intermediate products in a laboratory electric arc furnace was investigated. Smelting experiments were carried out using pyrolyzed pelletized black mass, copper(II) oxide, and different quartz additions as a flux to investigate the influence on lithium-slagging. With the proposed smelting operation, lithium could be enriched with a maximum yield of 82.4% in the slag, whereas the yield for cobalt, nickel, and copper in the metal alloy was 81.6%, 93.3%, and 90.7% respectively. The slag obtained from the melting process is investigated by chemical and mineralogical characterization techniques. Hydrometallurgical treatment to recover lithium is carried out with the slag and presented in part 2.

The objective of this study is to describe primary lithium production and to summarize the methods for combined mechanical and hydrometallurgical recycling of lithium-ion batteries (LIBs). This study also aims to draw attention to the problem of lithium losses, which occur in individual recycling steps. The first step of hydrometallurgical treatment is leaching, which is an effective method capable of transferring over 99% of the present metals to the leach solutions. Extraction of metals after leaching can be conducted using various methods, with precipitation being the most commonly used. The precipitation of other metals can result in the co-precipitation of lithium, causing total lithium losses up to 30%. To prevent such losses, solvent extraction methods are used to selectively remove elements, such as Co, Ni, Al, and Mn. Solvent extraction (SX) is highly effective, reducing the losses to 3% per extraction stage and reducing overall lithium losses to 15%. After the refining, lithium is precipitated as lithium carbonate. High lithium carbonate solubility (1.5 g/L) and high liquid to solid leaching ratios require costly and avoidable operations to be implemented in order to enhance lithium concentration. Therefore, it is suggested that more studies should focus on multistage leaching with lower L/S ratios.

The production of ferroalloys and alloys like ferronickel, ferrochromium, ferromanganese, silicomanganese, ferrosilicon and silicon is commonly carried out in submerged arc furnaces. Submerged arc furnaces are also used to upgrade ilmenite by producing pig iron and a titania-rich slag. Metal containing resources are smelted in this furnace type using fossil carbon as a reducing agent, which is responsible for a large amount of direct CO₂ emissions in those processes. Instead, renewable bio-based carbon could be a viable direct replacement of fossil carbon currently investigated by research institutions and companies to lower the CO₂ footprint of produced alloys. A second option could be the usage of hydrogen. However, hydrogen has the disadvantages that current production facilities relying on solid reducing agents need to be adjusted. Furthermore, hydrogen reduction of ignoble metals like chromium, manganese and silicon is only possible at very low H₂O/H₂ partial pressure ratios. The present article is a comprehensive review of the research carried out regarding the utilization of bio-based carbon for the processing of the mentioned products. Starting with the potential impact of the ferroalloy industry on greenhouse gas emissions, followed by a general description of bio-based reducing agents and unit operations covered by this review, each following chapter presents current research carried out to produce each metal. Most studies focused on pre-reduction or solid-state reduction except the silicon industry, which instead had a strong focus on smelting up to an industrial-scale and the design of bio-based carbon for submerged arc furnace processes. Those results might be transferable to other submerged arc furnace processes as well and could help to accelerate research to produce other metals. Deviations between the amount of research and scale of tests for the same unit operation but different metal resources were identified and closer cooperation could be helpful to transfer knowledge from one area to another. Life cycle assessment to produce ferronickel and silicon already revealed the potential of bio-based reducing agents in terms of greenhouse gas emissions, but was not carried out for other metals until now.

Due to the increasing demand for battery raw materials, such as cobalt, nickel, manganese, and lithium, the extraction of these metals, not only from primary, but also from secondary sources, is becoming increasingly important. Spent lithium-ion batteries (LIBs) represent a potential source of raw materials. One possible approach for an optimized recovery of valuable metals from spent LIBs is a combined pyro- and hydrometallurgical process. The generation of mixed cobalt, nickel, and copper alloy and lithium slag as intermediate products in an electric arc furnace is investigated in part 1. Hydrometallurgical recovery of lithium from the Li slag is investigated in part 2 of this article. Kinetic study has shown that the leaching of slag in H₂SO₄ takes place according to the 3-dimensional diffusion model and the activation energy is 22–24 kJ/mol. Leaching of the silicon from slag is causing formation of gels, which complicates filtration and further recovery of lithium from solutions. The thermodynamic study presented in the work describes the reasons for the formation of gels and the possibilities of their prevention by SiO₂ precipitation. Based on these findings, the Li slag was treated by the dry digestion (DD) method followed by dissolution in water. The silicon leaching efficiency was significantly reduced from 50% in the direct leaching experiment to 5% in the DD experiment followed by dissolution, while the high leaching efficiency of lithium was maintained. The study takes into account the preparation of solutions for the future trouble-free acquisition of marketable products from solutions.

A continuously growing demand for valuable non-ferrous metals and therefore an increase in their prices at the metal exchanges makes it necessary and profitable to investigate alternative metal resources. Polymetallic deep-sea nodules contain cobalt, copper, manganese, molybdenum and nickel, and are highly abundant on the sea floor. Developing a metallurgical process to recover the metal content from manganese nodules can close the predicted supply gap of critical metals like cobalt. This paper investigated a potential extraction process for valuable metals from manganese nodules supplied by the German Federal Institute for Geosciences and Natural Resources. The samples originated from the German license area of the Clarion-Clipperton Zone in the Pacific Ocean. Due to a low concentration of valuable metals in nodules, a pyrometallurgical enrichment step was carried out to separate cobalt, copper, molybdenum and nickel in a metallic phase. The manganese was discarded in the slag and recovered in a second smelting step as ferromanganese. To aid the experiments, FactSage^TM was used for thermodynamic modeling of the smelting steps. To increase metal yields and to alter the composition of the metal alloys, different fluxes were investigated. The final slag after two reduction steps were heavy-metal free and a utilization as a mineral product was desired to ensure a zero-waste process.