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Industrial Recycling of Lithium-Ion Batteries—A Critical Review of Metallurgical Process Routes

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Industrial Recycling of Lithium-Ion Batteries—A Critical Review of Metallurgical Process Routes metals Review Industrial Recycling of Lithium-Ion Batteries—A Critical Review of Metallurgical Process Routes Lisa Brückner 1,* , Julia Frank 2 and Tobias Elwert 3 1 Department of Mineral and Waste Processing, Institute of Mineral and Waste Processing, Waste Disposal and Geomechanics, Clausthal University of Technology, Walther-Nernst-Str. 9, 38678 Clausthal-Zellerfeld, Germany 2 Northvolt Zwei GmbH & CO. KG, Frankfurter Straße 4, 38122 Braunschweig, Germany; [email protected] 3 New Energy Vehicle Research Centre, Qingdao University, Ningxia Road No. 308, Qingdao 266071, China; [email protected] * Correspondence: [email protected]; Tel.: +49-532-372-2633 Received: 20 July 2020; Accepted: 14 August 2020; Published: 18 August 2020 Abstract: Research for the recycling of lithium-ion batteries (LIBs) started about 15 years ago. In recent years, several processes have been realized in small-scale industrial plants in Europe, which can be classified into two major process routes. The first one combines pyrometallurgy with subsequent hydrometallurgy, while the second one combines mechanical processing, often after thermal pre-treatment, with metallurgical processing. Both process routes have a series of advantages and disadvantages with respect to legislative and health, safety and environmental requirements, possible recovery rates of the components, process robustness, and economic factors. This review critically discusses the current status of development, focusing on the metallurgical processing of LIB modules and cells. Although the main metallurgical process routes are defined, some issues remain unsolved. Most process routes achieve high yields for the valuable metals cobalt, copper, and nickel. In comparison, lithium is only recovered in few processes and with a lower yield, albeit a high economic value. The recovery of the low value components graphite, manganese, and electrolyte solvents is technically feasible but economically challenging. The handling of organic and halogenic components causes technical difficulties and high costs in all process routes. Therefore, further improvements need to be achieved to close the LIB loop before high amounts of LIB scrap return. Keywords: lithium-ion battery; recycling; lithium; cobalt; nickel; manganese; graphite; mechanical processing; pyrometallurgy; thermal treatment; pyrolysis; hydrometallurgy 1. Introduction Renewable energy sources have the potential to end the era of fossil fuels. Electrochemical storage systems, especially lithium-ion batteries (LIBs), are an important technology for the success of this transition. This is due to their sum of positive properties such as their high energy density and low self-discharge [1]. On the production site, the growing application of LIBs leads to high investments in research and development with a focus on questions such as optimized cell production or optimized active materials. These developments are accompanied by a critical discussion regarding the security of the necessary raw material supply, the environmental and social impact of the raw material production, and the responsible recycling of end-of-life batteries [2–5]. Beside base metals such as iron (Fe), aluminum (Al), copper (Cu), manganese (Mn), and nickel (Ni), LIBs also contain minor metals such as cobalt (Co) and lithium (Li) as well as graphite. The production of some of these raw materials Metals 2020, 10, 1107; doi:10.3390/met10081107 www.mdpi.com/journal/metals Metals 2020, 10, 1107 2 of 29 Metals 2020, 10, x FOR PEER REVIEW 2 of 31 canExamples be connected are the toappearance severe ecological of child and labor social in artisanal impacts. Co Examples mining and are the influence appearance of ofLi childproduction labor inon artisanal the water Co balance mining in and desert the influenceareas [6,7]. of Furtherm Li productionore, in on the the case water of balancesome raw in materials, desert areas a small [6,7]. Furthermore,number of producers in the case dominate of some the raw markets. materials, This a small is especially number true of producers for Co and dominate graphite the [8]. markets. In view Thisof these is especially developments, true for the Co recycling and graphite of LIBs [8 is]. a In key view factor of theseto manage developments, the transition the toward recycling renewable of LIBs isenergies a key factor in a sustainable to manage theway. transition However, toward LIB recy renewablecling is energiesa challenging in a sustainable task due to way. their However, complex LIBmaterial recycling composition is a challenging and their task electrical due to their and complex chemical material energy composition content leading and theirto various electrical health, and chemicalsafety, and energy environmental content leading (HSE) to risks various [9]. health, safety, and environmental (HSE) risks [9]. InIn orderorder to to ensureensure aa closedclosed looploop forfor LIBsLIBs (see(see FigureFigure1 1),), extensive extensive research research activities activities started started about about 1515 yearsyears ago.ago. SeveralSeveral eeffortsfforts ledled toto thethe developmentdevelopment ofof didifferentfferent recyclingrecycling processes,processes, whichwhich havehave beenbeen realizedrealized inin aa fewfew pioneeringpioneering industrialindustrial plants.plants. AllAll thesethese processprocess routesroutes areare characterizedcharacterized byby longlong andand complexcomplex process process chains chains and useand a combinationuse a combination of mechanical of andmechanical/or thermal and/or and/or pyrometallurgicalthermal and/or andpyrometallurgical hydrometallurgical and hydrometallurgical unit operations [10]. unit operations [10]. Cathode Active Lithium-Ion Metal Mining Material Battery and Refining Production Production Scrap Scrap Metal Battery Life Refining Collection Metal Discussed in and Extraction this Review Dismantling Figure 1. Closed loop for battery materials. Figure 1. Closed loop for battery materials. This paper reviews and discusses the current status of industrial metallurgical processes from This paper reviews and discusses the current status of industrial metallurgical processes from a a European perspective. In contrast to existing reviews [11–17], which often focus on research at European perspective. In contrast to existing reviews [11–17], which often focus on research at a lower a lower technology readiness level and specific process technologies, this review emphasizes the technology readiness level and specific process technologies, this review emphasizes the complex complex dependencies between legal framework, economic conditions, and technical boundaries dependencies between legal framework, economic conditions, and technical boundaries of industrial of industrial process routes. The focus here lays on the metal extraction and metal refining from process routes. The focus here lays on the metal extraction and metal refining from battery battery cells/modules. Pre-treatment (discharging and dismantling of battery systems) is not covered cells/modules. Pre-treatment (discharging and dismantling of battery systems) is not covered in this in this review. For further details on this subject, see [10,11]. Products of metal refining are metal salts, review. For further details on this subject, see [10,11]. Products of metal refining are metal salts, compounds, or the respective metals, e.g., cathodes that can be used in different industries depending compounds, or the respective metals, e.g., cathodes that can be used in different industries depending on the final quality. on the final quality. In the following, after a background on current and future LIBs as well as legislation is given in In the following, after a background on current and future LIBs as well as legislation is given in Section2, the currently pursued industrial recycling routes are presented in Section3. In Section4, Section 2, the currently pursued industrial recycling routes are presented in Section 3. In Section 4, the recycling processes are critically discussed with respect to legislation, recovery rate, process the recycling processes are critically discussed with respect to legislation, recovery rate, process robustness, economics, and HSE. Section5 summarizes the main conclusions and gives an outlook robustness, economics, and HSE. Section 5 summarizes the main conclusions and gives an outlook regarding the upcoming developments. regarding the upcoming developments. 2. Background 2. Background The LIB technology has reached a wide acceptance since its introduction and is applied in a growingThe LIB number technology of applications. has reached First,a wide it wasacceptance widely since applied its introduction in batteries forand mobile is applied phones in a andgrowing laptops, number followed of applications. by pedelecs and First, power it was tools. widely Nowadays, applied LIBs in capturebatteries the for markets mobile for phones stationary and storagelaptops, systems followed and by electricpedelecs vehicles and power (xEVs) tools. [1]. Nowadays, Table1 summarizes LIBs capture the characteristicsthe markets for of stationary LIBs in distoragefferent systems applications. and electric vehicles (xEVs) [1]. Table 1 summarizes the characteristics of LIBs in different applications. Metals 2020, 10, 1107 3 of 29 Metals 2020, 10, x FOR PEER REVIEW 3 of 31 TableTable 1. 1.Characteristics Characteristics of of lithium-ion lithium-ion batteries batteries (LIBs) (LIBs) used used in in battery battery electric
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