Review

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Recycling of Lithium-Ion Batteries—Current State of the

Art, Circular Economy, and Next Generation Recycling
Jonas Neumann, Martina Petranikova, Marcel Meeus, Jorge D. Gamarra, Reza Younesi,
Martin Winter, and Sascha Nowak*

the lithium-ion battery (LIB), as an estab-

Being successfully introduced into the market only 30 years ago, lithium-ion lished technology, is a promising candidate
batteries have become state-of-the-art power sources for portable electronic for the energy-storage of the future.[1] Con-
devices and the most promising candidate for energy storage in stationary or sequently, LIBs are already the first choice
for energy storage in modern day portable
electric vehicle applications. This widespread use in a multitude of indus- consumer electronics like laptops, smart-
trial and private applications leads to the need for recycling and reutilization phones, or tablets. Furthermore, as the most
of their constituent components. Improving the “recycling technology” of attractive battery technology for pure and
lithium ion batteries is a continuous effort and recycling is far from maturity hybrid electric vehicles, as well as a strong
today. The complexity of lithium ion batteries with varying active and inac- candidate for stationary storage solutions,
there is a widespread use of LIBs in private
tive material chemistries interferes with the desire to establish one robust
and industrial applications.[2–4] This broad
recycling procedure for all kinds of lithium ion batteries. Therefore, the distribution goes hand in hand with the
current state of the art needs to be analyzed, improved, and adapted for the need for recycling. Partially, this necessity
coming cell chemistries and components. This paper provides an overview is economically driven by the value of the
of regulations and new battery directive demands. It covers current practices applied metals, which is significant given
in material collection, sorting, transportation, handling, and recycling. Future the high Ni, Cu, or Co contents. Spent LIBs
usually contain 5–20% cobalt (Co), 5–10%
generations of batteries will further increase the diversity of cell chemistry nickel (Ni), 5–7% lithium (Li), 5–10% other
and components. Therefore, this paper presents predictions related to the metals (copper (Cu), aluminum (Al), iron
challenges of future battery recycling with regard to battery materials and (Fe), etc.), 15% organic compounds, and 7%
chemical composition, and discusses future approaches to battery recycling. plastics.[5,6] Currently, the market is domi-
nated by LiPF6-based organic solvent electro-
lytes due to the excellent properties of LiPF6
1. Introduction regarding ion conductivity, supporting solid electrolyte interphase
(SEI) formation at the anode, and protection of the Al current
Increasing energy demands, due to the world population growth, collector at cathode.[7–12] Additionally, the state-of-the-art LIB cell
as well as the changing lifestyle and the depleting fossil-fuel consists of a graphite anode, and in most cases a layered lithium
resources are creating a dependence on renewable energy sources. metal oxide (LiMO2, M =, e.g., Co, Ni, Mn, Al) with varying metal
One problem of renewable energy is the unsteady electricity gen- contents or a lithium transition metal phosphate as a cathode.[13–19]
eration. Accordingly, surplus energy must be stored in order to There are also a variety of non-Li chemistries currently inves-
compensate for fluctuations in the power supply. Due to its high tigated, including batteries based on naturally highly abun-
energy density, high specific energy and good recharge capability, dant elements such as sodium, zinc, magnesium, calcium,

J. Neumann, M. Winter, S. Nowak M. Petranikova

University of Münster Chalmers University of Technology
MEET Battery Research Center Department of Chemistry and Chemical Engineering
Corrensstraße 46, 48149 Münster, Germany Industrial Material Recycling
E-mail: [email protected] Kemivägen 4, Gothenburg 41296, Sweden
M. Meeus
European Materials Industrial Research Initiative- EMIRI
The ORCID identification number(s) for the author(s) of this article Rue de Ransbeek 310, Brussels B-1120, Belgium
can be found under https://doi.org/10.1002/aenm.202102917.
J. D. Gamarra, R. Younesi
Department of Chemistry-The Ångström Laboratory
© 2022 The Authors. Advanced Energy Materials published by Wiley- Uppsala University
VCH GmbH. This is an open access article under the terms of the Uppsala 75121, Sweden
Creative Commons Attribution License, which permits use, distribution M. Winter
and reproduction in any medium, provided the original work is prop- Helmholtz-Institute Münster
erly cited. IEK-12
Forschungszentrum Jülich
DOI: 10.1002/aenm.202102917 Corrensstraße 46, 48149 Münster, Germany

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etc. Among these non-Li batteries, the sodium ion technology the treatment of EOL products to the producer. In general, a
as the most similar to the commercial LIBs is considered as distinction is made between physical and financial respon-
a drop-in solution.[20] However, from a recycling perspective, sibilities.[42,43] Physical responsibility refers to ensuring the
such battery chemistries with low-cost elements are of little eco- treatment of waste products, including collection, transport,
nomic interest. Therefore, the recycling of such batteries must sorting, reuse, recycling, and disposal.[42] These tasks can usu-
be supported by legislation. ally be delegated to third parties.[42–44] The financial responsi-
Battery recycling is encouraged by the legislation through bility relates to the financing of the aforementioned activities
different directives, mainly because of risks to human health and allows producers to internalize the costs of waste treat-
or the environment deriving from hazardous battery constitu- ment and incorporate them into their prices.[42,43] Regulations
ents.[21–26] Recycling processes are the only option to re-intro- regarding the treatment of EOL batteries vary from country to
duce end-of-life (EOL) batteries and their components into country. In the following, the legislation in three of the largest
the economic cycle, reducing the need for primary raw mate- battery markets, EU, USA, and China, is presented (Table 1).
rials[27,28] and promoting an improved acceptance of pure and
hybrid electric vehicles. However, the complexity of an LIB with
its diverse components, cell chemistries, and aging mecha- 2.1.1. EU
nisms offers certain challenges for recycling.[29,30].In addition
the varying lifetimes for batteries in different applications (cell In the EU, present regulations include the Battery Directive
phones: about 2  years, other consumer electronics 3–4  years (Directive 2006/66/EC) and the Waste Electrical and Electronic
and electric vehicles >10  years) produce a mixed upcoming Equipment (WEEE) Directive (Directive 2012/19/EU). These
stream of spent batteries.[31] Beyond this, the development of policies include a physical and financial EPR. Member countries
next generation batteries leads to even more complex mixtures are required to set up collection schemes for end-of-life portable
of battery scrap, increasing the need for universal and flexible batteries in the form of collection points located in the vicinity
recycling processes.[32–35] Furthermore, in contrast to the lead of end-users. The costs for collection, treatment, recycling, and
acid battery, only high amounts of metals such as nickel or disposal must be financed by the battery producers. Producers
cobalt provide financial viability for LIB recycling.[36] And last, and distributors are further required to take back portable, auto-
so far no standardizations for cell designs of LIBs exists.[37] motive, and industrial batteries (including electric vehicle (EV)
Nevertheless, recycling processes are used to handle the batteries) free of charge. Industrial, automotive, and collected
upcoming stream of spent batteries. Today, mainly pyro- and portable waste batteries must undergo treatment and recy-
hydrometallurgical processes, or a combination of both, are cling using the best available techniques to protect health and
applied to process current cell chemistries.[32,38,39] Yet, a closed the environment before residual compounds can be landfilled
loop in view of a holistic circular economy is not achieved, or incinerated. In order to maximize the separate collection
since several components like anode, electrolyte or binder are of spent batteries from mixed municipal waste, the directives
still not, or only recently subject to recycling. However, activi- set minimum collection targets and recycling efficiencies for
ties in this area are increasing, so that potential methods and member states. The collection rate is calculated by dividing the
processes for the recycling of these components are emerging. mass of portable waste batteries collected in one year by the
In contrast to this, the recycling of next generation batteries is average annual mass of portable batteries placed on the market
neither focused by industry nor by research activities. Only less in the previous three years. The minimum collection rates were
than a handful studies have been published recently so far.[40,41] set at 25% by 2012 and 45% by 2016. For Pb–acid, Ni–Cd, and
In this review, we provide an overview about the current other battery types, the directive sets recycling efficiency targets
state of the art in LIB recycling, addressing topics like regula- of 65%, 75%, and 50% by average weight, respectively.[44,45]
tions (EU, China, and USA), handling, transport, and current In a revision report from 2019, the European Commis-
technologies which are applied during recycling in research sion evaluated the effectiveness of the 2006 Battery Directive.
and industry. In addition, a critical assessment on the dif- According to the report, most countries achieved the collection
ferent types of next generation cell chemistries (batteries of the target of 25% by 2012. However, only 14 member states have
future) and emerging recycling approaches such as design for reached the subsequent target of 45% by 2016. In total, 56.7% of
recycling and direct recycling are given. all waste portable batteries are not collected annually and about
35  000 tons end up in municipal waste streams. The report
concludes that the current collection targets are not sufficient
2. Regulatory Framework and further targets should be defined for the future. Another
concern is that collection targets have so far only been defined
2.1. Recycling Regulations for waste portable batteries and not for automotive and indus-
trial batteries (including EV batteries).[45] Another statement
Legislation plays an important role in controlling the recycling from the European Association of National Collection Systems
of any waste material. By setting targets for collection rates for Batteries (Eucobat) describes the collection rate calculation
and recycling efficiencies, and regulating disposal responsibili- as inappropriate. Accordingly, the calculation does not consider
ties and safety requirements, government authorities can con- the varying lifetimes for different battery types, as well as pos-
tribute to the establishment of an effective circular economy. sible battery exports, and is therefore not realistic. As a solu-
An important concept in this regard is the extended producer tion, the calculation of collection rates based on the battery cells
responsibility (EPR), which assigns the responsibility for available for collection is proposed.[46]

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Table 1.  Selection of the most important federal policies regarding the recycling and treatment of EOL batteries in the EU, USA, and China.

Year EU USA China

1995 Universal Waste Rule as part of the Resource Law of the People´s Republic of China on the Prevention and
Conservation and Recovery Act (RCRA) Control of Solid Waste Pollution
1996 Mercury-Containing and Rechargeable Battery
Management Act (Battery Act)
2006 Battery Directive (Directive 2006/66/EC)
2012 Waste Electrical and Electronic Equipment (WEEE) Notice of the State Council on Issuing the Planning for the
Directive (Directive 2012/19/EU) Development of the Energy-Saving and New Energy Automobile
Industry
2014 Guiding Opinions of the General Office of the State Council
on Accelerating Promoting and Application of New-Energy
Automobiles
2016 Policy on Pollution Prevention Techniques of Waste Batteries
Implementation Plan of the Extended Producer Responsibility
System
2018 Interim Measures for the Management of Power Battery
Recovery and Utilization of New Energy Vehicles
2020 Proposal for a regulation of the European Parlia-
ment and of the Council concerning batteries and
waste batteries, repealing Directive 2006/66/EC and
amending Regulation (EU) No 2019/1020

As part of the European Green Deal, in 2020 a legisla- mercury-containing battery types, and requires the Environ-
tive proposal was submitted by the European Commission to mental Protection Agency (EPA) to establish a public education
replace the 2006 Battery Directive. The proposed regulations program on battery recycling, proper handling, and disposal of
considerably exceed previous legislation in many respects and used batteries. Moreover, the Universal Waste Rule, as part of the
are intended to support the development of the EU toward a Resource Conservation and Recovery Act (RCRA) from 1995, is
modern, resource-efficient, and competitive economy. Accord- made effective for all 50 states.[47] The Universal Waste Rule pro-
ingly, new collection targets for waste portable batteries hibits the disposal of certain hazardous wastes and sets standards
(excluding batteries for light means of transport, e.g., e-bikes) for the collection, storage, and transportation of these wastes.[48]
are 45% by 2023, 65% by 2025, and 70% by 2030. The proposal In addition to the Battery Act, some U.S. states have enacted
does not include collection targets for industrial, automotive, further legislation on battery recycling. In 25 states, regula-
and EV batteries, but sets a legal framework for the establish- tions that are more specific apply to the recycling of lead acid
ment of appropriate collection schemes for these battery types. batteries. In most of these states, landfilling or incineration of
In addition, the proposal is called for a revision of the collection lead acid batteries is prohibited, and consumers are required to
targets in 2030, including the consideration of adjusting the cal- dispose such batteries separately from mixed municipal wastes.
culation method for collection rates to be based on the waste Furthermore, retailers are required to take back lead acid bat-
batteries available for collection. New targets for recycling effi- teries in certain quantities and deliver them to manufacturers
ciencies are 65% for LIBs and 75% for Pb-acid batteries by 2025. or permitted secondary treatment facilities. Only four states,
Moreover, target material recovery rates of 95 % for cobalt, 95% namely California, Minnesota, New York and Puerto Rico, have
for copper, 95% for lead, 95% for nickel, and  70% for lithium also introduced regulations for the collection and recycling of
by 2030 have been defined. Further requirements include LIBs.[49–52] For example, the Rechargeable Battery Recycling Act
extended battery labelling, a battery passport for batteries with of 2006 introduced the EPR in California. Thus, producers are
capacities above 2  kWh, minimum contents of recycled mate- required to internalize the costs for handling, recycling and
rials in new industrial and automotive batteries, minimum per- safe, environmentally sound disposal of used rechargeable bat-
formance and durability requirements, and more.[44] teries. In addition, retailers are required to take back used bat-
teries free of charge, the content of hazardous substances in
rechargeable batteries should be reduced, batteries should be
2.1.2. USA designed for longer life and reusability, and consumers must be
provided with comprehensive information on battery recycling.
The only federal policy in the U.S. regarding battery recycling is
the Battery Act of 1996, which primarily focuses on facilitating the
recycling of nickel–cadmium (Ni–Cd) and small sealed lead-acid 2.1.3. China
(SSLA) rechargeable batteries, as well as phasing out the use of
mercury in batteries. The directive includes a national standardi- In China, first legislation regarding battery products were
zation of labelling requirements, the prohibition of selling certain introduced in 1995. Initially, the regulations mainly focused

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on phasing out batteries containing mercury and cadmium. composition.[54–57] Three of the main markets for LIBs are con-
Later, increasing attention was given to the recycling and proper sumer electronics, stationary battery energy storage (SBES),
disposal of lead-acid batteries.[53] However, until the 2010s, and EVs.[55,58,59] While the consumer electronics market (cell
there was a significant lack of regulation governing the collec- phones, portable computers, medical devices, power tools,
tion and treatment of waste LIBs.[42,53] With the Notice of the etc.) is mature, the EV market in particular is expected to be
State Council on Issuing the Planning for the Development the main driver for an increasing LIB demand.[58–60] Since these
of the Energy-Saving and New Energy Automobile Industry markets show significant differences, it is necessary to establish
from 2012 and the Guiding Opinions of the General Office different types of collection systems. The smaller household
of the State Council on Accelerating Promoting and Applica- batteries from electronic devices can be collected in containers
tion of New-Energy Automobiles from 2014, the State Council at retail partner and manufacturer locations, whereas the col-
set the foundation for establishing a system for collection and lection of larger modules from EVs and SBES devices requires
treatment of waste EV batteries, including the development disassembly and must be performed by trained personnel.[61]
of technical standards and management rules as well as their The availability of EOL batteries is especially important in
enforcement. Subsequently, in 2016, the Policy on Pollution Pre- this context. Consumer electronics currently account for a large
vention Techniques of Waste Batteries by the Ministry of Eco- share of the LIB market. Batteries from this segment have life-
logical and Environment (MEE) and the Implementation Plan times of approx. 3–10 years, depending on the type of device.[62]
of the Extended Producer Responsibility System by the General The service life is usually much shorter, but the widespread
Office of the State Commission (GOSC) were issued. These pol- storage of devices after their use, often referred to as hiberna-
icies specify the development of standards related to pollution tion, leads to an extension of the overall lifetime. The lifetime
prevention and the collection, transportation, storage, utiliza- of EV batteries is often warranted by car manufacturers for a
tion, and disposal of waste LIBs. Furthermore, the development minimum of 8  years or 100  000  miles/160  000  km (e.g., Tesla
of a monitoring system for waste batteries is encouraged, an Model 3 Standard Range, VW eGolf, Nissan Leaf, BMW i3).
EPR is introduced for EV and battery manufacturers and spe- The accurate prediction of the EV battery life is difficult because
cific recycling targets of 40% by 2020 and 50% by 2025 for many factors, such as the battery type, the number of cycles,
major waste products, including LIBs are set. With the Interim the charging conditions and the annual driving distance must
Measures for the Management of Power Battery Recovery and be considered.[63,64] For example, using predictive models, Yang
Utilization of New Energy Vehicles issued in 2018, the Ministry et  al. have estimated EV battery lifetimes of 5–13  years under
of Industry and Information Technology (MIIT) and six other average driving conditions in different U.S. states. Consid-
ministries and commissions consolidated existing regulations. ering a second-life application of retired EV batteries in SBES
Along with several subsequent guidelines, the Interim Meas- systems, the total battery lifetime could be increased to about
ures provide an overall policy framework for today’s battery 15–25 years depending on the application. Due to this long bat-
recycling industry in China. The key elements of this policy tery life and the immaturity of the EV sector, waste streams
framework are: a) encouragement of manufacturers to design from consumer electronics are an important near-term source
batteries for easy disassembly; b) obligation of manufacturers for battery recycling.[60,65]. Currently, only a small portion of the
to provide the technical information necessary for EOL battery electronic waste generated each year is collected and properly
treatment; c) promotion of cascaded application and second recycled.[66] According to the Global E-Waste Monitor 2020, the
life of EOL batteries; d) responsibility of EV and battery pro- rate of collected and recycled e-waste is 42.5% in Europe, 11.4%
ducers for battery waste treatment, based on the EPR concept; in Asia, 9.4% in the Americas, 8.8% in Oceania, and 0.9% in
e) responsibility of cascaded application companies, EV makers Africa. Overall, 17.4% of the e-waste generated worldwide is
and battery producers for establishing waste battery collection documented to be collected and recycled.[66] Among the largest
outlets; f) material recovery targets of 98% for nickel, cobalt, and generators of e-waste, Asia leads with 24.9  Mt, followed by
manganese, 85% for lithium, and 97% for rare earth and other Europe with 12.0 Mt and North America with 7.7 Mt. To ensure
metals. Further specification of the financing mechanisms for effective battery recycling, it is therefore necessary to maximize
waste battery treatment is not included in the policies.[42,53] the collection rate for spent batteries and e-waste and thus opti-
mally use available resources. Furthermore, suitable structures
for the collection and recycling of larger battery modules should
2.2. Material Collection and Sorting be installed at an early stage in order to prepare for the rapidly
growing EV and SBES markets.
The establishment of an efficient collection system for EOL bat- In addition to the heterogeneity regarding different module
teries is a key element in a successful recycling strategy. The sizes and fundamentally different cell chemistries, such as Pb–
collection rate determines the number of spent batteries that acid, Ni–Cd, and Ni–metal hydride, LIBs also significantly vary
enter the recycling stream and is therefore decisive for the for similar applications within the same market segments.[54,57]
extent of economic and ecological output of the overall recy- Due to continuous development, changing performance
cling system. requirements, increasing raw material prices and innovations,
One of the major challenges for setting up a performant col- the composition and design of LIBs is constantly changing.
lection infrastructure lies in the heterogeneity of battery types While for many years LiCoO2 (LCO) was the commercially
available on the market. LIBs are used for a wide range of dominant cathode material for LIBs, increasing costs for cobalt,
applications, resulting in a large variety of battery designs that as well as the limited thermal stability and rapid capacity fading
differ with regard to their capacity, shape, size, and chemical of LCO-LIBs, have led to the commercialization of alternative

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cathode materials. The most widely used cathode types today directly in recycling facilities. Since not all recycling facilities
also include LiNi0.8Co0.15Al0.05O2 (NCA), LiNixCoyMnzO2 (NMC), are capable of processing every type of battery, this could result
LiFePO4 (LFP), and Li2Mn2O4 (LMO, Spinel type). Beyond that, in additional transport routes. A possible solution would be the
several other materials, including LiMnO2 (LMO, Layered type), setup of fully integrated recycling plants capable of specifically
LiMnPO4 (LMP) and conversion-type cathodes, such as sulfides, treating various types of cells. Building such plants, however
are under development.[2] New developments are also pro- may require large capital investments and should be difficult to
gressing in the fields of anode materials, electrolytes, and sepa- achieve in a private economy. A third option, the establishment
rators. Although graphite and other carbons are considered the of a decentralized pre-treatment infrastructure, could therefore
state-of-the-art LIB anode materials, alternative LIB anode types be beneficial. Sorting of battery types, as well as other processes
such as silicon and silicon composites, as well as lithium metal such as battery deactivation, removal of casings, and other
anodes, and zero-excess anodes for lithium metal batteries physical separation methods, could already be applied as a pre-
(LMBs) are being researched. At the same time, new electro- treatment, enabling an early separation of material streams,
lyte systems continue to find application. Especially solid-state minimizing transportation costs, and improving the overall
electrolytes, which are usually based on polymers, ceramics, or efficiency of battery recycling.[31,60]
hybrid systems, are attracting more and more attention.[2,67–70] Since the chemical composition of a battery is not visible
The different LIB cell chemistries pose a major challenge to from the outside, appropriate labelling is an important prereq-
current recycling systems. Not all processes are economically uisite for battery sorting. In addition to the essential informa-
viable for the recycling of any battery type. Due to the high tion on the battery type and chemical composition, labels could
investment costs, pyrometallurgical treatment, for example, contain data regarding the manufacturer, the date of manufac-
is primarily suitable for the recycling of batteries with high ture and the use of the battery. This information would enable
cobalt and nickel content, such as LCO, NMC, and NCA bat- effective sorting but could also significantly improve safety
teries. Lithium and aluminum end up in a slag and can only be during the handling of used battery cells.[60]
recovered with considerable additional effort. Hydrometallurgy, In the EU, current legislation mainly aims at providing
on the other hand, also enables the recovery of lithium and is end users with necessary information for the proper handling
applicable for a mixture of different cathode types. However, of battery cells. This includes the symbol shown in Figure 1a,
due to the low intrinsic material value of LFP batteries both which indicates that batteries must be collected separately from
processes fail to recover valuable products from this battery household waste. In addition, the battery capacity and the pres-
type. Another approach, direct recycling, aims at the recovery ence of the heavy metals Hg, Cd, and Pb must be indicated.[76]
of cathode materials with a still usable morphology. Since the In 2020, the European Commission has proposed a new
number of further processing steps for the re-synthesis of directive with more comprehensive battery labelling require-
cathode materials is reduced, this method has a comparatively ments. The proposed legislation requires additional label-
low environmental impact and currently represents the only ling of cells with information about the manufacturer, date
process by which significant value can be generated from used of manufacture, date of market introduction, battery type,
LFP and LMO cathodes. A major disadvantage of direct recy- battery model, chemistry, hazardous substances, carbon foot-
cling is that the process requires single cathode types as input print, recovered materials, and critical raw materials contained.
in order to recover high quality materials.[60,71–74] Through a so-called battery passport, the information should
To overcome the challenge posed by the material mix, an be made available with a QR code printed or engraved on
effective separation of different battery types based on their the housing and an electronic battery information exchange
chemical composition is required.[31,75] The sorting could be system. Independent operators shall also be given access to
implemented through a more differentiated collection of bat- the battery management system of rechargeable industrial bat-
teries by the end-users. However, this would lead to a consid- teries and EV batteries with internal storage with a capacity
erable additional effort for consumers and in order to achieve above 2 kWh, for the purpose of assessing and determining the
high collection rates, more convenient collection schemes state of health and remaining lifetime of batteries in order to
could be advantageous. Another option is to sort batteries enable second-life applications. Parameters for determining the

Figure 1.  Battery labels required by different federal policies in the EU and USA. a) Label indicating separate collection from mixed municipal waste;
required by EU Battery Directive 2006/66/EC. b) Möbius loop indicating recyclability of batteries; required by US Mercury-Containing and Rechargeable
Battery Management Act. c) LIB transport label indicating classification as Class 9 Dangerous Goods; required by US law 49 CFR § 172.447.

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state of health of batteries include: remaining capacity, overall flammable electrolyte components and the decomposition of
capacity fade, remaining power capability and power fade, cathode materials, which can lead to fires, explosions and the
remaining round trip efficiency, actual cooling demand, evo- release of toxic substances.[25,87–91] There have been numerous
lution of self-discharging rates, and Ohmic resistance and/or incidents in the past where LIBs have led to fires at recycling
electrochemical impedance.[44] and waste treatment facilities. In the UK, for example, it is
A comparable regulation was already issued in China in 2018 estimated that approximately 48% of all waste fires occurring
with the Interim Provisions on the Traceability Management of each year are caused by LIBs, costing the UK economy approxi-
Power Battery Recovery and Utilization of New Energy Vehicles. mately 158  million  pounds annually.[92] Unfortunately, official
This policy requires the establishment of a national manage- statistics on LIBs as cause of fires in waste transportation and
ment platform for the traceability of batteries throughout their waste treatment facilities are rare, as they are often included
entire life cycle, including production, sale, use, disposal, and in the category of self-ignition. Still, the fire hazard associated
recycling.[42,53] In the U.S., there is no comprehensive federal with spent LIBs is generally considered to be high.[90,93]
regulation for the labelling of LIBs. Current laws only include As a result, lawmakers have set specific safety requirements
the labelling of Ni–Cd and Pb–acid batteries with a reference to for the transportation and handling of newly produced and
the respective battery type, as well as the requirement for bat- EOL LIBs. Different national and international laws define
tery recycling. Additionally, the batteries must be labelled with restrictions on transport quantities, specifications for safe
the recycling symbol shown in Figure 1b.[47–49] Further labelling packaging and package sizes, labelling requirements, and pre-
requirements for LIBs in the U.S. are in place in the context scriptions for safety tests. One of the most important interna-
of transportation. These regulations are targeted at transporta- tional standards for the transport of LIBs is specified in the UN
tion safety and include, for instance, certificates for safety tests, Manual of Tests and Criteria, Part III, Subsection 38.3. This
packaging guidelines, an additional LIB label (Figure  1c) and provision is applied in most regions of the world, including the
transport volume limitations.[47] EU, US, and China, and requires that battery cells (excluding
As a central part of battery recycling, the development of a small production runs and prototypes) must pass certain safety
suitable collection infrastructure for EOL batteries is essential. tests in order to be transported. The safety tests include alti-
In particular, the better use of currently available resources and tude simulations as well as heat, vibration, shock, external
the expansion of collection capacities for the fast-growing EV short circuit, impact, overcharge and forced discharge tests. In
market are crucial. In addition, the establishment of a suitable the EU, LIB transport by road, rail and sea freight is regulated
pre-treatment system for sorting as well as further pre-treat- by the Agreement concerning the International Carriage of
ment steps, such as cell deactivation and physical separation of Dangerous Goods by Road (ADR), the Regulations concerning
cell components, is promising. Policy plays a particularly impor- the International Carriage of Dangerous Goods by Rail (RDI),
tant role in this regard, as the introduction of standardized bat- and the International Maritime Dangerous Goods Code (IMDG
tery labels, mandatory collection rates for spent batteries and an Code).[94–97] Comparable provisions in the U.S. are provided
EPR could contribute to a more effective battery collection. by Part 49 of the Code of Federal Regulations. In China, there
are few national transportation regulations, but responsible
authorities follow international provisions such as the ADR,
2.3. Transportation and Handling RDI, and IMDG Code.[77]
According to these regulations, LIBs with energies >100 Wh
The high energy density and the presence of toxic and flam- are classified as Class 9 Dangerous Goods. Transport quantities
mable substances lead to significant safety risks when han- for these batteries in road transport are limited to 333  kg per
dling and transporting LIBs. One of the most serious hazards transport unit and strong outer packaging that prevents short
is the thermal runaway, which can be described as a cascade circuits and unintentional activation is required. For smaller
of uncontrolled exothermic reactions that is caused by an ini- batteries with energies ≤100  Wh no transport quantity limits
tial overheating of a battery cell.[77–79] and depends on the age of apply, but similar package requirements must be met, and
the used cells.[80–84] Potential reasons for the initial overheating package sizes may not exceed 30  kg. Further, batteries must
are external heat sources, overcharging or external and internal be labelled adequately and pass the UN safety tests. Defective
short circuits. The risk for internal short circuits of LIBs is batteries must be classified as critical or non-critical. Batteries
increased by lithium metal plating, due to inaccurate battery that are liable to decompose rapidly, react dangerously, produce
assembly, or inappropriate operation, such as overcharging, a flame or a dangerous evolution of heat, or emit toxic, corro-
over discharging or low temperatures and high current densi- sive, or flammable gases or vapors are classified as critical. The
ties during charging. Several strategies, such as the addition transport of critical battery cells must be approved by a com-
of electrolyte additives that support the formation of effective petent authority. For non-critical batteries, as well as batteries
SEIs,[85] or protective coatings with artificial SEIs can reduce the designated for disposal and recycling, there are no restrictions
dendrite formation in state-of-the-art LIBs.[78,86] However, the on transport quantities, but special packaging regulations apply.
problem still remains and represents one of the most important The batteries must be protected against short circuits, dan-
challenges for next-generation anodes, such as lithium metal. gerous heat generation and leakage. This requires, for example,
Short circuits can also occur during handling, due to external individual securing of the battery terminals, inner packaging
mechanical stress or incorrect storage. A single short-circuited to prevent contact between batteries, specially designed battery
cell can thereby cause the initiation of the thermal runaway terminals, use of a suitable cushioning and absorbing material,
of many other cells. The consequences are the combustion of leak proof inner packaging and venting devices.[94–97]

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Further transport regulations include the International Civil 2.4. Battery 2030+ Initiative in Europe
Aviation Organization Technical Instructions (ICAO TI) and
the International Air Transport Association Dangerous Goods The Battery 2030+ roadmap suggests research actions to radi-
Regulations (IATA DGR), which specify the international trans- cally transform the way to discover, develop, and design ultra-
port of dangerous goods by air. According to the directives, LIBs high-performance, durable, safe, sustainable, and affordable
can generally be transported by air if the previously mentioned batteries for use in real applications. The purpose is to make a
UN safety tests have been passed and ventilation, short cir- collective European research effort to support the urgent need
cuit protection, reverse current flow prevention and additional to establish European battery cell manufacturing. Addition-
packaging conditions are met. The transport of LIBs intended ally, recyclability is a key cross cutting topic, which is consid-
for disposal and recycling is prohibited, unless approved by ered from the very beginning of the Battery 2030+ research
national authorities. Defective or damaged LIBs may not be program.[100] New battery materials engineered interfaces and
transported by air and standalone LIBs (UN number: UN3480) smart battery cell architectures will be developed bearing in
must have a state of charge (SOC) ≤30% to be transported. mind the manufacturability, scalability, recyclability, and life-
National regulations regarding air transport of LIBs in the EU, cycle environmental footprint of the novel technologies. The
US and China are in accordance with the IATA DGR and the future recycling process, in which materials escape from the
ICAO TI.[94–97] technosphere into the biosphere as non-reusable materials, will
The security risks and the resulting safety regulations be dramatically improved by novel recycling approaches. This
have a significant impact on the costs for transport and han- approach that will lead to a drastic reduction of the propor-
dling of LIBs. Along with the transport distance, the trans- tion of batteries to be treated in classical recycling processes.
port quantities, capacity utilization, and additional safety Challenges to overcome regarding the reconditioning of the
precautions are important cost factors. Taking into account active materials are numerous and require further fundamental
emissions trading and CO2 prices, additional transport studies. As an example, for the cathode material, being the
routes can have a great impact on the future profitability of most expensive battery materials cost factor, new processes
battery production and recycling. Several studies have esti- need to be further developed to restore its original chemical
mated the transportation costs as a percentage of total recy- composition, crystallography, and coatings (Figure 2).
cling costs. In a review of these studies, Slattery et al. found Would the material/components not be suitable to be recon-
an average contribution of 41%. The transport cost estimates ditioned to battery grade because of, for example, structural or
vary significantly from $0.24/kg to $5.51/kg for a standard purity constraints, a fallback alternative in the last stage of the
distance assumption with an average value of $1.54/kg.[98] new process could consist of converting them to precursors and
Reasons for these deviations include regional differences in eventually changing the composition ratios, anticipating future
fuel and labor costs, as well as different calculation methods. chemistry changes and new generation materials as shown in
The high transportation costs directly affect the profitability Figure 3.
of recycling. Especially batteries with low material value (e.g.,
LFP or LMO) could become a financial liability to owners
and recyclers, so that there are fewer incentives for battery 3. State of the Art Recycling Technologies
recycling.
One possible solution to this problem would be the intro- 3.1. Pre-Treatment
duction of an EPR through legislation, including a physical,
as well as financial responsibility. This way, costs for collec- Handling of Li-ion modules consists of two main processes:
tion, transport, recycling, and disposal would be covered by discharging, and dismantling of battery modules, including
battery producers and the profitability of the recycling step disconnecting of major components (cables, battery cells,
would increase. As an additional incentive for end-users to frames, electronics, etc.). After cell removal, those go under the
return batteries to collection points, a deposit system could mechanical processing and separation. Mechanical separation
also be useful. Beyond that, the costs for collection transport techniques separate cell components based on their different
and recycling should generally be reduced. An option to mini- physical properties such as particle size, density, conductivity,
mize transportation costs is the strategic siting of collection magnetic properties, etc.
points and recycling facilities.[98,99] The resulting reduction
of transport distances has an impact on the total transport
costs, but also reduces potential safety risks during transport. 3.1.1. Discharging
Another option is the establishment of a decentralized pre-
treatment system for EOL batteries. This would enable the Batteries are discharged before manual dismantling primarily
sorting, deactivation, dismantling and physical separation of to secure the safety of the personnel and to eliminate the risk of
batteries into different waste streams prior to recycling. After electric shocks. Additionally, sparks might cause the ignition of
pre-treatment, the different materials could be transported to volatile organic compounds during the crushing process[21,101]
centrally located recycling facilities. A major advantage of this and thus cause fires.
type of system is that pre-treated battery components (e.g., Discharging can be performed by different methods. Several
black mass or battery casings) may not be classified as haz- companies use thermal pre-treatment (e.g., Accurec or REDUX
ardous goods, which could significantly reduce transportation in Germany),[96] salt-water based baths (NaCl or Na2SO4),[102–105]
costs and safety risks.[98] or controlled discharging via external circuits. NaCl and

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Figure 2.  Roadmap for the Battery 2030+ initiative.

alternative salts (Na2S and MgSO4) were tested to discharge depending on several factors, but predominantly on the solu-
portable batteries. It was concluded that NaCl provided the best tion resistance—itself depending on the conductivity of the
discharge profile. Also, Na2S was a sufficient discharge media, solution and the distance between the electrodes.[105]
while solutions containing MgSO4 were not capable to fully dis-
charge the batteries.[106]
In some cases, batteries are discharged via cryogenic 3.1.2. Mechanical Pre-Treatment
methods using liquid nitrogen or in vacuum atmospheres. Nev-
ertheless, these methods are connected to higher OPEX and Mechanical pre-treatment is used to disintegrate batteries and
CAPEX.[106,107] separate particular components into several streams. The main
However, salt-water based discharge is still the most pref- scope is to separate metallic particles (casing, copper and alu-
erable method in the industrial environment. It was reported minum foils) and to concentrate the black mass, which is the
that it is a flexible and comparably safe way to stabilize dif- mixture of cathode and anode active materials. Black mass
ferent types of high-energy cells. The rate of discharge varies is the most valuable battery cell component and mechanical

Figure 3.  Battery 2030+: Anticipation of future chemistry changes and new generation materials.

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pre-treatment is mostly designed to achieve its maximum those processes.[114,115] Since the remaining carbon from the dif-
recovery and separation. Mechanical processes involve crushing, ferent components would interfere with the lithium recovery,
sieving, magnetic separation, fine crushing, and classification, the removal is mandatory. The used conductive carbon and
which are performed in sequence.[101] Multistage crushing and acetylene black decompose above 600  °C.[116] Also, the binder
sieving result in quite effective separation. Magnetic separation can be removed by applying the respective decomposition tem-
is used to remove pieces of steel casing or joints. Traditional peratures which are typically lower compared to the carbon
mechanical pre-treatment is performed by companies such as species.[117]
Akkuser (Finland), Batrec (Switzerland), or Duesenfeld (Ger- Mostly pyrolysis and incineration steps are applied for the
many). At Akkuser Oy, the batteries are crushed using a two- pre-treatment. While similar processes, they can be distin-
phase crushing process. Disintegrated material is separated guished by the presence or absence of oxygen or air.[118] By
using air separation and magnetic separation. An inert atmos- adding oxygen or air, incineration can be used to remove the
phere is used during the crushing process. At Batrec the bat- binder or carbon species. However, all plastic parts and electro-
teries are also crushed in a controlled atmosphere of CO2 gas. lytes are lost during the process.[38,119] Nevertheless, by choosing
The individual components, such as aluminum and steel casing, an appropriate temperature range, the subsequent recovery of
black mass, nonferrous metals, and plastic are separated in a lithium and other metals can be supported.[114,117,119–122]
multistage separating plant and sold to other producers. Duesen- In comparison, in an oxygen-free environment pyrolysis
feld is a start-up company, which also applies mechanical treat- allows the transformation of the organic compounds into lower
ment of the batteries coupled with electrolyte recovery. The LIBs molecular compounds or their recovery by recondensation.[123]
are discharged, shredded under nitrogen, and the electrolyte is Further literature reports the separation of current collector
evaporated and condensed. The dry materials are then separated foils and active material by pyrolysis.[124–126]
using their physical properties via air separation and sieving.[108]
A flowchart for black mass recovery was proposed by Widi-
jatmoko.[109,110] Cells were shredded and sieving was applied to 3.2. Hydrometallurgy
separate the components into different size fractions. An attri-
tion scrubbing technology was used to liberate fine black mass There are more than fifty companies worldwide, which process
from coarse foils. In the milling step, the 850 µm size fraction spent LIBs. The majority of the companies operate in China and
gives the best composition of the black mass recovery with South Korea, followed by the European Union, Japan, Canada,
minimum presence of copper and aluminum. However, most and the USA. It is predicted that over 700 000 tons of batteries
of the black mass was held together by the PVDF binder.[110] will become obsolete by 2025. The worldwide recycling capacity
Beside the mechanical pre-treatment, mineralogical tech- is estimated to be around 400  000  tons at that time.[127] Recy-
nologies such as flotation have been applied to recover the black cling companies in China have different outcomes and achieve
mass.[111] Flotation is using the difference in hydrophilicity and different grades of final purities, however almost all companies
hydrophobicity of electrode materials and other battery compo- use hydrometallurgical approaches. The main recovery prod-
nents. Yet, there are still challenges in using this technique since ucts are salts such as NiSO4, CoSO4, and Li2CO3 or products in
the efficiency of cathode material recovery is not sufficient. form of mixtures for precursor production based on NMC and
Due to the low evaporation temperature of most electrolyte NCA.[127] In the European Union, the most common recovery
components (below 280°C), their recovery remains a key challenge methods are pyrometallurgy, hydrometallurgy, and combina-
in mechanical pre-treatment. Several approaches have been tested. tions of both. Due to the requirements of the new EU Battery
The most common is the thermal pre-treatment below 300°C to Directive, the high demands on the precursor materials for bat-
evaporate the electrolyte. This method has been applied in the tery production, and the goal of creating a circular economy,
industry, but still results in insufficient electrolyte recovery.[101] hydrometallurgy will be the most preferable process. The main
Some novel methods such as high-voltage treatment or the reason is the ability to recover larger amounts of battery com-
use of supercritical CO2 for more effective separation have been ponents and reach very high purities of metal salts. One of the
reported.[112,113] By using high-voltage treatment 94  % of cathode downsides of hydrometallurgy is the need for mechanical pre-
particles were separated from the Al foil by sieving and 99 % of the treatment consisting of two main processes: disintegration of
particles maintained the chemical structure of original NMC.[112] the batteries and separation of the particular components.
Use of supercritical CO2 lead to the separation of cathode mate- Hydrometallurgical recycling of LIBs is based on the disso-
rial from the current collector when almost 99  wt% of polyvi- lution of metallic components mostly coming from the active
nylidene fluoride (PVDF) dissolved in a supercritical CO2-dime- material (mixture of cathodes and anodes), preferably with
thyl sulfoxide system at 70 °C and 80 bar pressure after 13 min.[113] mineral acids, followed by metal separation by solvent extrac-
Despite promising results more investigation is required before tion, ion exchange, and precipitation. A thermal pre-treatment
the application of these new methods in industrial processing. (pyrolysis or calcination) can be applied as well.[41,28]
Leaching is applied as the first step in the hydrometal-
lurgy process after mechanical or also thermal pre-treatment.
3.1.3. Thermal Pre-Treatment The leaching media are usually mineral acids (H2SO4, HCl,
and HNO3), in some cases also alkali and organic acids.[129,130]
Thermal pre-treatment methods are applied to safely deactivate Studies show that inorganic acids are highly effective for the
the battery with regards to the combustible components of the recovery of metals (>99%) in the leaching procedure when
electrolyte. Discharging of the battery can be achieved during applied under optimal conditions. The most common acid is

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sulfuric acid due to its effectiveness, costs, and compatibility is high, solvent extraction is applied for its recovery instead
with metal separation techniques. Generally, under compa- of precipitation. Lithium is usually recovered via precipitation
rable conditions, leaching efficiencies of Li and Co from LCO with sodium carbonate, carbon dioxide, or via ion exchange.
cathodes are H2SO4 ≈ Cl > HNO3 > H2SO3.[131] In the leaching The first step in leachate processing is the impurity (Fe/
process, graphite stays in a solid residue after filtration. A Cu/Al) removal via pH adjustment and precipitation.[101] How-
significant number of leaching studies have been published ever, these methods are related to a significant loss of valu-
and concluded that the temperature (40–60 °C), solid to liquid able metals (sometimes Co loss can be around 10%). Recently
ratio S/L (1/10–1/20) and the presence of the reduction agent a novel approach via ion exchange has been reported.[150] The
(e.g., H2O2) are the most important factors affecting the com- suggested process produced a >99.6% pure Li/Co/Ni solution
plete recovery of metal ions.[132–134] A different approach has (battery grade) with a Co loss of around 1% only.
been published by,[135] where foils from current collectors were The most common method for Mn/Co/Ni separation is
used as a reduction agent. It was reported that more than 99% solvent extraction.[134,151–153] The acidic extractant di-(2-ethyl-
of Li and Co can be extracted by addition of Al/Cu containing hexyl) phosphoric acid (D2EHPA) is very often applied for
fractions.[135] Iron scrap has also been applied as a reduction Mn recovery.[152,154,155] The extractant concentration reported
agent utilizing the reduction potential of ferrous ions.[23] is usually around 0.4–0.5  m D2EHPA diluted in kerosene.
The use of organic acids such as ascorbic, citric, malic, tar- Operation temperature is very often ambient, and the process
taric, and succinic acid has been reported as well.[136–139] To is performing sufficiently at pH 2.2-5. The contacting time is
eliminate the use of inorganic reductants, organic reduction reported to vary from 5–15 min.[156]
agents were also tested, including ascorbic acid and carbohy- Co and Ni are separated using organophosphorus acids,
drates (e.g., cellulose, etc.).[138] Still H2O2 was the most common chelating oximes, carboxylic acids, and high molecular
reduction agent applied. The organic reagents might represent weight amines (HMWA). The organophosphorus acids (e.g.,
a lower risk for the operations and equipment used. Such rea- Cyanex 272) and chelating oximes are most widely used and com-
gents also decompose under aerobic and anaerobic conditions mercially acceptable.[157] When using acidic extractants cobalt is
with limited gas generation. From the tested acids lactic acid extracted at lower pH before Ni. Co is tetrahedrally coordinated
showed a high recovery of Li (98%), Co (99%), Ni (98%), and in Cyanex 272 as Co(R2H)2 and nickel forms the hydrated octa-
Mn (98%) using 1.5  m lactic acid, S/L of 20  g L−1, 70  °C, and hedral complex Ni(R2H2)2(RH)2. Co is extracted at pH around 5
0.5  vol% H2O2, with very short leaching time of 20  min.[140,141] while Ni is efficiently recovered around pH 6.5.[158,159]
However, very high leaching efficiencies were reported for the After the separation, Co and Ni salts are recovered using con-
majority of tested organic acids when a reduction agent (H2O2) trolled crystallization.[101] Recently a new approach was tested
was applied. using eutectic freeze crystallization to separate and recover
A novel approach is based on applying ultrasound when metal ions after hydrometallurgical treatment of LIBs.[147]
leaching with mineral acids[142] or organic acids.[143] In all cases The eutectic freeze crystallization (EFC) is a method to sepa-
a higher efficiency has been reported. rate aqueous inorganic solutions into ice and solid solutes via
Bioleaching and biotechnologies are using microorganisms freezing at the eutectic point. The advantages of EFC are lower
to recover metals from different resources.[144] The group of energy requirement and the possibility of complete conversion
microorganisms involved in the bioleaching of metals from into water and solidified solutes.[149] It was reported that with
LIBs were usually chemolithotrophic prokaryotes, hetero- suitable control of supersaturation, ice and cobalt and nickel
trophic bacteria, and fungi.[145] Relatively high recoveries of Ni salt crystals can be recovered as separate phases below eutectic
(90%), Mn (92%), Co (82%), and Li (89%) from spent LIBs in temperatures.[148]
72 h with a solid content of 100 g L−1 were achieved using bac- Li is usually the last metal recovered from the stream. The
teria—Acidithiobacillus ferrooxidans.[146] However, despite exten- most common way is the precipitation with sodium carbonate
sive research, biotechnologies are not commonly applied in bat- or sulfate. The concentration of lithium ions in the solution
tery recycling due to comparably slow process kinetics, leading directly affects the recovery efficiency and the purity of the
to long processing times. Some battery components such as compound precipitated. Larger concentrations involve higher
typically used organic solvent based electrolytes and selected, recovery efficiencies with the drawback of a maximum con-
mostly fluorinated binders are also toxic to microorganisms. centration value after which the purity starts to decrease.[160]
Another disadvantage is that at high pulp density, the efficiency According to ref. [161], when the solid Na2CO3 is used directly as
of the process is much lower. Using bioleaching, there is no the precipitant, the lithium recovery rate is higher than using a
potential for changing the metal valence state, which is com- saturated Na2CO3 solution while the purity obtained would not
monly needed for a better cobalt recovery.[145] be affected. The concentration of Na2CO3 or Na3PO4 added in
After the leaching step an effective separation of metal ions the solution is also significant and affects the recovery efficiency,
is necessary. The most common separation methods are sol- and the purity of the compound precipitated. Several tempera-
vent extraction (SX), chemical precipitation, ion exchange (IX), ture values (from 25 to 95  °C) have been studied for the pre-
electrochemical deposition, and more novel eutectic freeze crys- cipitation of lithium carbonate or lithium sulphate and studies
tallization.[147–149] The separation procedure is usually a combi- show that the closer the temperature is to 100  °C, the more
nation of several separation techniques. Precipitation is most effective is the precipitation.[162] Also, the pH of the solution is
common for the removal of the impurities Fe, Al, and Cu. Sol- a determinant factor in the precipitation of lithium carbonate/
vent extraction is usually applied to separate NMC metals such phosphate. When using Na2CO3, optimal pH of operation is
as Mn/Co/Ni. In case that the Cu concentration in the leachate between 10 and 11.5, while for Na3PO4 this range is between 11

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Table 2.  Examples of hydrometallurgical recovery of valuable metals from LIBs in a form of different products and achieved purities.

Reference Hydrometallurgical procedures Products Reported purity

[164] 1) Precipitation in pH 5.5 Li2CO3 >98%
2) Carbonization CoCO3 36-37 %
[164] 1) Precipitation at pH 5.5 Li2CO3 >98%
2) Solvent extraction CoCO3 47%
3) Carbonization
[165] 1) Precipitation of Ni using (CH3C(NOH)C(NOH)CH3) CoC2O4⋅H2O 98%
2) Solvent extraction of Co and Mn using D2EHPA Li2CO3 99%
3) Co-precipitation (NH4OH) and Li-precipitation (Na2CO3) MnSO4 98%
Ni+
[166] 1) Solvent extraction of Mn using D2EHPA MnO2 >99.5%
2) Scrubbing the impurities (MnSO4)
3) Stripping with acid
4) Oxidative precipitation using KMnO4 and MnO2
[167] 1) Extraction with (I)P204 (II)P507 Co-metallic 99%
2) Electrowinning
[168] Using different lithium solubilities Li2CO3 99.5%
[169] 1) Precipitation of Fe Co3O4 83%
2) Solvent extraction CoC2O4 96%
3) Li precipitation using Na2CO3 NiO 89%
Li2CO3 99%
[170] 1) Reductive hydrogen roasting LiOH⋅H2O 99.9%
2) Water leaching of lithium
3) Crystallization of lithium hydroxide

and 13.[162] The time of agitation usually has a minimum value are several companies that apply a combined approach. Nick-
of 35  min and 60  min is a common standard to get recovery elhütte Aue GmbH (Germany) or Umicore (Belgium) use a
efficiencies over 80%. A novel approach to recover Li before the hydrometallurgical treatment after smelting of the batteries to
extraction of heavy metals was reported by ref. [163] using tribu- recover metals from the alloy (matte). Nickelhütte Aue GmbH
tylphosphate (TBP) and FeCl3 with a reported purity of lithium has a hydrometallurgical plant and produces approximately
of almost 99%. Also, Solvay recently developed a phosphorus- 3900 t of Ni per annum. Matte processing starts with commi-
based extractant with the trade name CYANEX  936P for selec- nution followed by pressure oxidation leaching at 6 to 8  bar.
tive recovery of Li. There are different approaches of hydromet- Afterward, impurities are removed prior to solvent extraction of
allurgical processing listed in the Table 2. Cu, Co, and Ni. Before extraction, Fe is precipitated as goethite
Industrially hydrometallurgy is mostly used in China and (FeOOH) by using H2O2 as an oxidizing agent and basic nickel
South Korea (e.g., Brunp, Soundon New Energy, GEM, Huayou carbonate for pH adjustment. Depending on the process setup,
Cobalt, Ganpower, etc.). Since the majority of batteries are copper sulfate, cobalt sulfate, and nickel sulfate, or nickel car-
produced in these countries, the infrastructure is very well bonate and chloride are produced.[171] In general, the processing
organized to gather sufficient volumes of production scrap and and steps are depicted in Figure 4.
spent batteries. In Europe, hydrometallurgical processes are The main advantage of hydrometallurgy is the possibility
used for instance in Sweden, where the battery producer North- to produce new battery precursors from waste with the suffi-
volt AB integrates a hydrometallurgical recycling process in the cient purity. Despite the large demand for chemical reagents,
production cycle in order to secure the raw material supply and hydrometallurgy allows the re-utilization of many solvents and
to decrease the environmental impact of battery production. by-products for several years, minimizing the overall secondary
Hydrometallurgical processing is also used in companies such waste generation.[4] With future battery legislation and demands
Eramet (France) and Fortum (Finland), etc. At Northvolt, the ini- for higher material recovery rates, hydrometallurgy is one of
tial collection and handling of batteries is followed by the pro- the most promising approaches to meet the requirements but
cessing of batteries to recover aluminum, copper, steel, plastics, also to create a path to circular economy in the battery market.
electronics, and electrolyte. The pilot plant has been running
for a few years and the full-scale recycling plant will process
8500 t of black mass per year. At Fortum, LiBs are first disas- 3.2.1. Deep Eutectic Solvents
sembled and treated during a mechanical process at a plant in
Ikaalinen, Finland. The black mass is collected and then taken Within the realm of hydrometallurgy lies solvometallurgy in
to hydrometallurgical processing at another plant in Harjav- which organic phases are exclusively used.[172] Solvometallurgy
alta, Finland. The recycling process achieves recovery rates of offers a complementary set of tools parallel to hydrometallurgy,
up to 95% and involves a chemical precipitation method. There and aims to reduce the waste and environmental impact of

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Figure 4.  Overview about traditional hydrometallurgical processing.

hydrometallurgy.[172] Currently, the recovery capacities of hydro- voltage (2.7 V), was introduced by Pateli et al.[185] as alternative
metallurgy are able to cover the needs and benchmarks set by using lower temperature and shorter processing times. The
European Policy in terms of metal recovery. Nevertheless, this formation of superoxide that allows for the reaction of oxides
does not address lithium, electrolytes and future water con- into organometallic and chloro complex species is suggested
sumption regulations. The organic phases reduce waste by lim- as the driving force but further studies are required. However,
iting water consumption, performing the leaching and solvent the low proton activity and poor ligand capabilities of ethylene
extraction in a single step, and increasing selectivity. An ideal glycol and urea limits their applicability for direct leaching
organic phase must be efficient, low cost, easily recoverable or when compared to DES with more acidic HBD.[186] Solvometal-
biodegradable.[172] Low transition temperature mixtures (LTTM) lurgical approaches for the leaching of cobalt from LiCoO2 have
can offer all of these properties. LTTM refers to a mixture of been reported using p-toluenesulfonic acid and citric acid as
two or more compounds: one hydrogen bond donor (HBD) and HBDs.[178,184,187] Those studies report higher S/L ratio, shorter
one hydrogen bond acceptor (HBA) that undergoes a second leaching times and lower temperatures than urea, ethylene
phase transition resulting in a glass transition temperature.[173] glycol and glycerole. Recent work on the thermodynamics of
Deep eutectic solvents (DES) refer to a sub-category of LTTM the process have shown that overcoming the lattice energy and
in which there is a significant drop in the melting point and Gibbs energy of the metal oxides is an important factor in con-
which remain liquid at specific molar proportions.[174] There is trolling solubility.[186,188] These findings point to acid-based DES
a broad nomenclature used depending on the composition of as the most promising category for the direct leaching of metals
the solvent.[175] “Hydrophobic DES” is used when both compo- from LIBs in the near future, but the kinetics and solvation
nents are hydrophobic[176], and “Brønsted acid DES” implies mechanisms need to be studied in further detail before scaling.
that the HBA is a Brønsted acid instead of the more commonly LTTMs are the latest entry into the wet (hydro, solvo, iono) met-
used quaternary ammonium salt.[177] These solvents have been allurgy arsenal. They are part of the efforts to lower the entry
recently introduced to the metal and battery recycling flow- barrier of room temperature ionic liquids and their analogues
sheets as successful media for electrochemical recovery,[178,179] into the metallurgy flowsheet. Nevertheless, the fundamental
direct leaching of metals (Li[180], Ni, Co) from LIB cathodes, and knowledge of aqueous solutions cannot be applied to these new
even the dissolution of the polymeric binders in cathodes.[181] solvents and their specific kinetics and speciation remains to
Ethylene glycol,[179] urea[182–184] based DES have the physical be determined. Other challenges like the role and means of pH
properties required to act as leaching agent and electrolyte for variations on the extraction of specific metals, and the effect of
the electrochemical recovery of metals from LIBs. The studies additives and co-solvents are also at early stages of research. As
by Wang[181] and Landa-Castro[182] discuss the role of urea and our understanding of LTTM and DES increases, so will their
ethylene glycol as reducing agents of the leaching reaction. importance for the recycling of LIBs.
This redox process requires high temperatures (above 150  °C) The main advantage of hydrometallurgy is the possibility
and longer leaching times than those using mineral acid to produce new battery precursors from waste with suffi-
leaching. Electrooxidation, a process in which a DES/metal cient purity. Despite the large demand for chemical reagents,
oxide paste coats the anode and the cell is held at constant hydrometallurgy allows the re-utilization of many solvents

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and by-products for several years, minimizing the overall sec- in Li2CO3, MnO, Ni, and Co with high recovery rates.[201]
ondary waste generation.[4] The integration of solvometallurgy Roasting of LCO cathodes was reported under a nitrogen
into critical hydrometallurgical steps, like leaching could boost atmosphere at 1000  °C for 30  min. The resulting residue
the overall efficiency of the approach with citric acid DES being was leached with water and after a wet magnetic separation
able to achieve effective leaching at 55 g L1 S/L versus 25 g L–1 step, the following recovery rates were achieved: Li 98.93%,
of the aqueous solution.[143] Novel organic media use less Co 95.72%, and graphite 91.05%.[190] This approach was fur-
volume and shorter leaching times with higher average loading ther applied for LMO cathodes with the following parameters:
capacities. With future battery legislation and demands for roasting for 45 min at a temperature of 800 °C. Afterward the
higher material recovery rates, hydrometallurgy is one of the residue (Li2CO3 and MnO) was leached with water and was
most promising approaches to meet the requirements but also mechanical separated. 99.13% of the Li was recovered, while
to create a path to circular economy in the battery market. the filter residue was calcined to remove carbon. This resulted
in a 95.11% recovery rate for Mn3O4.[202] In contrast, oxidizing
conditions were used to treat LFP cathodes. Here, an effec-
3.3. Pyrometallurgy tive temperature control is important. At temperatures above
650 °C the oxidizing roasting leads to the release of fluorine-
Pyrometallurgical approaches use a high-temperature fur- containing gas. Furthermore, the recovery of iron is reduced
nace to reduce the component metal oxides from LIBs to due to the formation of Fe2O3.[203] Microwave-assisted carbo-
form an alloy. In general, smelting and roasting/calcination thermic reduction was recently reported as a development for
steps are the main procedures during processing.[189–192] roasting. The reactivity of carbon in a microwave environment
Further classification is possible with regard to the applied results in faster reaction times.[204]
extraction mechanisms and the processing atmosphere. In order to cope with the low solubility of Li2CO3 more
During this process, the organic and volatile parts of the bat- recent advances in pyrometallurgical approaches included the
tery (electrolyte, separator, and binder) are evaporated. While application of salt assisted roasting. Depending on the salt,
high temperatures for metal recovery cause more chemical classification is normally described as chlorination, sulfation,
reactions, low temperatures lead to phase transitions during and nitration roasting. During the roasting, different agents
the process.[193] Therefore, pyrometallurgical techniques are are applied to produce better soluble lithium compounds. For
depending on factors like temperature, processing time, chlorination, agents like NH4Cl were reported.[189] In compar-
types of purge gas, and flux addition.[194] Higher tempera- ison, SO2(g), MgSO4, NH4SO4, NaHSO4·H2O, or Na2SO4 were
tures are used to incinerate the plastics and all remaining applied during sulfation to obtain Li2SO4.[198,205–208] Nitration
organic compounds.[114] roasting aims at the formation of LiNO3.[192]
The process is aided by the metal current collectors and Smelting on the other hand uses temperatures above the
therefore relatively mature compared to other techniques.[72] melting points of the respective battery components. Here, the
In addition, the evaporation and burning of the electrolytes, metals are separated in the liquid phase.[209,210] The advantage
binders and plastics is exothermic, which reduces the energy of this process is its robustness against different cell chemis-
consumption required for the process.[195] The products from tries and that no passivation/deactivation step is needed.[196]
this process are slags, metallic alloys, and gases. The alloys can The electrolyte is evaporated at lower temperature before the
be further refined by hydrometallurgical processes. While the actual smelting. The burning of the remaining organic compo-
lost fraction (electrolyte, salts, plastics, etc.) can significantly nents add additional energy to the process.[36] At higher tem-
reduce the overall recycling efficiency, the process itself con- peratures, alloys, gases, and slags are produced which can be
tains only little risks. However, the production of toxic gases further optimized.[197,211,212]
and the requirement for hydrometallurgical post-processing Nevertheless, pyrometallurgical approaches need a refining
poses an environmental drawback, while the robustness of the step (e.g., hydrometallurgy) after the initial treatment for the
process is well suited for imperfectly sorted feedstock of cells subsequent separation and recovery of the metals.[213] Further-
and no special pre-treatment of cells is necessary.[116,191,194,196,197] more, the lithium recovery must be enhanced.[39,214]
The pyrometallurgical approach is applied in several
industrial processes like the ultra-high-temperature smelting-
technology (UHT) of Umicore, the roasting−smelting process 3.4. Recycling of Specific Components—Short Overview
of Glencore, the high temperature melting recovery (HTMR)
process of Inmetco and the calcination processes of Sony- 3.4.1. Anode (Graphite)
Sumitomo and Accurec.[197,198,199]
Research works mainly focus on the variation of the above- While not established as cathode recycling, anode recycling has
mentioned classification parameters on a laboratory scale. gained more attention in the last years. Anodes can contain
Several methods have been reported for roasting processes natural and artificial graphite, carbonaceous materials or even
involving exothermic processes such as gas-solid reactions silicon. However, graphite is the commercially most applied
at elevated temperatures. Carbothermic reduction roasting material for now.[7,215,216] Several approaches have been reported
uses a reducing agent such as carbon along the cathode in literature, including pre-treatment, pyrolysis, hydrometal-
active material to form alloys.[200] NMC-based cathodes were lurgy, supercritical, and water treatment. The research is still
roasted at a temperature of 650 °C, a roasting time of 30 min, ongoing, with reviews and research papers appearing in a more
and a carbon dosage of 10% of raw material input resulting frequent manner.[216–224]

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3.4.2. Cathode faster charging capabilities, and longer cycle lifetimes.[2,57] As

the graphite-based lithium-ion technology slowly approaches
Hydro- and pyrometallurgical approaches dominate the recy- its theoretical capacity limits, alternative anode materials are
cling of metals from cathode materials.[96,116,130,150,160,163,170,194] receiving more and more attention. With a more than ten
Bioleaching on the other hand is relatively new in the field times higher theoretical specific capacity compared to graphite
of LIB recycling and seldom reported so far. Some literature (372  mAh g–1 in the unlithiated state), lithium metal anodes
reports the successful application of bacteria to obtain metal (3860 mAh g–1) are one of the most promising options to meet
fractions from spent batteries.[146,225–227] Phytoremediation was these increasing performance requirements. The development
also reported as one way to extract spent cathode material from of safe, high-energy lithium metal batteries (LMBs) is based on
storage and handling sides.[228] several different approaches, including for instance Li−sulfur
batteries (Li−S), Li−oxygen batteries (Li−O2), and Li−intercala-
tion type cathode batteries. The commercialization of LMBs has
3.4.3. Electrolyte so far mainly been hampered by the issue of high surface area
lithium metal deposits (so-called “dendrites”) and the associ-
Similar to the anode, the electrolyte gains more attention in ated safety concerns.[69,86,243,244] However, continuous progress
terms of recycling. While usually evaporated or burnt during in research indicates that LMBs will be one of the dominant
thermal processes, several approaches have been reported to battery technologies among next generation battery systems.
recover at least the lithium from this component.[72,229,230] The Therefore, an early consideration of possible recycling methods
first approach was the recovery of the electrolyte via liquid extrac- for this battery type is important.
tion.[229] Afterward, extraction via sub- and supercritical media In comparison to commercial LIBs, LMBs have significantly
was proposed with relatively good recovery rates,[219,231,232,233–240] higher lithium contents. In view of rising lithium prices and
which was also applied for binder recovery.[113] However, other the lower material value of alternative cathode materials, such
valorisation approaches were reported as well.[241,242] as sulfides, high recycling efficiencies for lithium will be an
important prerequisite for future recycling processes.[245] As
one of the most mature and robust recycling techniques, pyro-
3.5. Differentiation between Academic Approaches and Indus- metallurgy is widely used.[71] However, since non-noble metals
trial Reality such as aluminum and lithium are slagged in this process, fur-
ther refining steps, for example, through hydrometallurgy, are
Despite the recent increase in publications with regard to the required to achieve high recycling efficiencies.[71,72,246] Hydro-
topic of LIB recycling, most of the proposed methods are still metallurgy will therefore play a particularly important role in
based on lab-scale experiments. While under research condi- the recycling of the batteries of the future.
tions, most parameters, chemicals, or processes can be chosen As described in Table 2, there are different approaches for the
freely, but the applicability transfer into larger processes may not hydrometallurgical recovery of lithium from used LIBs. Typically,
be possible or at least rather difficult. Especially in the upscaling these processes consist of the dissolution of metallic compo-
of chemicals, for example, for leaching, cost and safety must be nents followed by various separation processes, such as sieving,
considered. On the other hand, high energy demands, due to solvent extraction, ion exchange, and precipitation.[71,247] In addi-
either high temperatures, long processing times, or high pres- tion, thermal pre-treatment may be applied. For the dissolution
sures can interfere with a successful upscaling of a process. The of metallic lithium, water is a suitable solvent.[248] From aqueous
same is true for high operating costs related to gas consump- solution lithium recovery can eventually be achieved through
tion or special components needed for extraction. Therefore, a precipitation as carbonate, sulphate, phosphate, chloride or
critical view on lab-scale processes and suggested procedures hydroxide.[71,246,248] A well-known method, for instance applied
should always accompany these developments. At the moment, by Retriev Technologies and Recupyl, is based on the precipita-
the main industrial recycling technologies can be divided into tion of Li2CO3 from aqueous solution by adding CO2.[249]
three categories: pyrometallurgy, hydrometallurgy, and a com- A major challenge in the recycling of LMBs results from the
bination of both methods.[40] Therefore, without the research of high reactivity of metallic lithium. This particularly includes
new and out of the box approaches, the recycling of existing and the high energy release (≈32  MJ kg−1 Li) and the formation of
upcoming battery generations will only be developed slowly. hydrogen (≈1.6 L H2 kg−1 Li) during the dissolution in water.[248]
In addition, dendrite formation during aging of LMBs still
increases the risk of short circuits and subsequent thermal run-
4. Recycling of Future Batteries—Current Approaches aways.[69,86,243,244] Special safety precautions must therefore be
taken into account, especially when handling EOL LMBs. Pos-
and Challenges, and Their Critical Assessment
sible approaches to address these issues in the recycling pro-
4.1. Future Generation Battery Chemistries cess include cryogenic treatment with liquid nitrogen prior to
cell crushing, mechanical crushing in an inert atmosphere, or
4.1.1. Li-Metal Systems thermal oxidation of Li prior to dissolution in water.[71,72,247,248]
Beyond that, deactivation of the cells as a pre-treatment could
The emergence of electric vehicles and of new developments be beneficial to reduce potential safety risks. One method
in the field of portable electronics are driving the constantly for the deactivation of battery cells is the discharge through
increasing demand for batteries with higher energy densities, electrical circuits, immersion in salt solutions or placement in

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containers filled with steel chips.[107,250,251] However, since many with the highly reactive Li metal anode, separation and han-
cells are protected against over discharge, they usually retain a dling of the electrodes will complicate future recycling.
residual charge after treatment.[252] Corrosion processes at the
contacts, as well as different cell designs, can also hinder deac-
tivation by discharging. Another deactivation method is based 4.1.3. All Solid State
on the removal of liquid electrolytes by evaporation or extrac-
tion.[232,236,253] Thereby, potentially toxic, and flammable sub- The development of all-solid-state batteries (ASSBs) is driven
stances can be removed from the cells and the hazard potential by several factors, including the need of high-energy batteries,
of thermal runaways can be reduced.[238,254,255] Potential safety improved battery safety and also new applications. Some types
risks associated with the reactivity of lithium metal, however, of solid electrolytes (SE) are now able to achieve ambient-tem-
are not eliminated. Alternative approaches for the deactiva- perature (RT) ionic conductivities in the order of 1  mS cm−1,
tion of LIBs and LMBs are based on the treatment with super- which makes them comparable to conventional liquid electro-
critical CO2. One strategy could be the removal of the metallic lytes.[269,270] Employing solid-state electrolytes also enables the
lithium in the form of CO2-soluble complexes from the battery safe application of Li metal anodes and the operation at high
cells before the actual recycling process. Similar procedures are voltages.[270] Solid electrolytes are generally classified as:[271,272]
known from the extraction of cobalt from LIBs, heavy metals 1) Inorganic/Ceramic:
from soil or radioactive metals from nuclear waste.[256–260] As
complexing agents, organophosphates, β-diketones or crown • Sulfides: for example, Li2S–GeS2–P2S5, Li10GeP2S12, Li6PS5X
ethers could be used. Besides the deactivation, an effective (X = Cl, Br, I), Li7P2.9Mn0.1S10.7I0.3
extraction would enable the early separation of different mate- • Oxides: for example, Li7La3Zr2O12, lithium phosphorus
rial streams and could make subsequent recycling processes oxynitride (LiPON), NaSICON type LiM2(PO4)3 (M = Ti, Ge,
more efficient. In a different approach by Sloop et  al., the Zr, Hf), perovskite-type Li3xLa2/3−xTiO3 (LLTO), etc.
metallic lithium from LIBs is converted to Li2CO3 using super- • Phosphates: for example, LiTi2(PO4)3, LiGe2(PO4)3, y-Li3PO4,
critical CO2.[261] The inert nature of Li2CO3 facilitates the han- LiPON, etc.
dling and transportation of treated cells and can contribute to • Others: for example, LiBH4, LiBH4-LiX (X = Cl, Br, or I),
significant cost savings throughout the recycling process. In LiBH4-LiNH2, Li3AlH6, Li6PS5X (X = Cl, Br, I), etc.
addition, through treatment with supercritical CO2, liquid elec-
trolytes can be partially extracted, increasing the overall recy- 2) Solid polymers:
cling efficiency.[261]
Further challenges for the recycling of LMBs arise from • Polyether based
other cell components, such as the cathode material or the type • Polyester based
of electrolyte. Therefore, in the following, Li–S batteries and all- • Nitrile based
solid-state batteries will be discussed in more detail. • Polysiloxane based
• Polyurethane

4.1.2. Li–S In the future, several aspects of the recycling will be affected
by solid electrolytes in spent batteries. There will be less safety
Using the high theoretical capacity of sulfur (1675  mAh g−1), issues related to the evaporation of the liquid electrolyte and the
lithium sulfur batteries (Li–S) are among the most promising accumulation of harmful fumes. The formation of the corrosive
future batteries. The cell chemistry of Li–S is quite different hydrofluoric acid can also be eliminated. The mechanical pre-
to LIBs. Typically, the Li–S system consists of a lithium metal treatment can be expected to be easier since solid electrolytes
anode and a sulfur/conductive carbon composite cathode with have been reported to be very brittle. For example, sulfide-based
a liquid organic solvent-based electrolyte.[262,263] Since several SE are reported to be elastic and have plastic properties but
disadvantages still hamper a broad practical application of these display low fracture toughness compared to polymer and oxide
batteries, no recycling processes are established so far.[264–266] electrolytes. Also oxide-based SE are in general very hard par-
However, some approaches were reported in the literature.[267] ticles, resulting in brittle layers.[273] The brittle and low-porous
While the challenges with regard to the Li metal are discussed media in ASSBs can be damaged when mechanical force is
in the section above, the separator, binder and electrolyte can applied.[274]
be subject to similar recycling procedures which are used or More challenges can be expected during the mechanical
investigated for LIBs. Nevertheless, it is necessary to carry out separation if very small, brittle particles are formed during the
further studies on the applicability and possible upscaling for crushing processes. Today battery components are more diverse
industrial processes. Regarding the sulfur-containing cathode, and easier to be separated by conventional methods. However,
several points need to be taken into account. During operation if very fine particles are formed the black mass for hydrometal-
(charging and discharging), intermediate Li-polysulfides are lurgical treatment can be more homogeneous.
formed, which makes the recycling process challenging.[268] The most significant effects can be expected for hydromet-
Furthermore, toxic gases like H2S can be formed during opera- allurgical treatment due to the diversification of the chemical
tion, opening and processing of the cells. In best cases, these compositions. Most challenging will be the recycling of the
gases can be converted to elemental sulfur or precipitated as ASSBs using inorganic resp. ceramic electrolytes, which con-
sulfides, for example with copper.[267] However, in combination tain metals that are not present in current cell chemistries.

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New elements such as Ge, Ti, Zr, Sn, or rare earths elements As of today, the development of an efficient battery disas-
(REEs) will interfere with the solvent extraction process of cur- sembly on an industrial scale still faces several challenges. On
rent recycling technologies. For example, if the acidic extractant the one hand, the current recycling network is not designed to
D2EPHA is used for Mn recovery, REEs and Zn will interfere process many different material streams, but rather focuses on
with the extraction process.[275] However, some adjustment to treating a wide variety of feedstocks in a single process. This
the recycling processes can be made, and those metals can be is especially true for pyrometallurgical recycling approaches,
recovered prior the extraction of Mn. The REEs, Al, Fe, and Zn which have very low battery pre-treatment requirements but
can be separated from Co and Ni from an HCl leachate at pH 2 offer low recycling efficiencies and material values in com-
using 25% D2EHPA in kerosene.[276] From nitric acid leachates, parison to hydrometallurgy. On the other hand, as the demand
Fe and Zr ions can also be extracted using D2EHPA and then for energy storage continues to grow, more and more players
stripped with oxalic acid.[277] Ti will also react with D2EHPA as it are getting involved in the development, production, mar-
can be extracted from both hydrochloric and sulfuric media.[278] keting and application of batteries, leading to the continuous
As D2EHPA is usually one of the first extractants used, more development of new material concepts and cell designs. This
extraction stages will be required before the extraction of Mn, leads to an increasing inhomogeneity and complexity of the
if current and future batteries are recycled together. Same phe- feedstock for battery recycling, posing significant challenges to
nomena can be expected for Cyanex 272 used for Co extraction. the applied processes.
In case that “new” metal ions are present in the leachate after An important concept to facilitate the development of an
extraction with D2EHPA, they will affect the extraction of Co efficient circular battery economy is called design for recycling.
and Ni. For example Cyanex 272 shows a greater affinity for Ti The concept is based on considering the eventual treatment of
over Fe at very lower solvent concentration.[279] the battery cells during recycling already in the design phase.
Another issue will be the presence of different anions in the The design principles are mainly focused on three levels, pack
system such as Cl–, B–, or F– as they also affect solvent extrac- and module design, cell design, and material design.
tion processes and the formation of organo-complexes.[277] Larger batteries (e.g., EV batteries) typically consist of many
However, this phenomena is not very well documented even individual cells arranged in modules which are then assembled
for current recycling technologies.[131] Major challenges of into a pack. The manual disassembly of such batteries is asso-
future recycling will result from an extremely diverse chemical ciated with high costs, long lead times and significant safety
composition of batteries and low concentrations of valuable ele- risks for workers.[196,285] There are several publications dis-
ments. Today the main motivation to recycle is based on the cussing the automation potential of battery disassembly.[285–288]
high Co/Ni/Li prices and government regulations (especially For instance, Hellmuth et  al. identified a 46-step disassembly
in EU). This should be considered while developing ASSBs for sequence for a 2017 Chevrolet Bolt battery and found that about
real applications and markets. In order to create incentives for one-third of the steps could be automated based on an assess-
recycling, a reasonable range of different metals in SE should ment of the technical feasibility and necessity of automation.
be selected and concentrations of valuable metals should be At present, fully automated disassembly by self-learning robots
sufficiently high to make recycling profitable. remains unrealistic due to the high complexity of some disas-
sembly steps. A more promising approach are hybrid systems
in which human workers perform the disassembly together
4.2. Future Generation Battery Recycling with automated robotic arms (human-robot collaboration).
Regarding battery design, the types of connections between
4.2.1. Design for Recycling the modules and the individual cells are of particular impor-
tance. These include, for example, threaded, screwed, bespoke,
For a sustainable transformation of the energy industry and the or push-fit connections, but also various types of welded
transport sector, it is necessary to enable cost-efficient battery pro- joints.[289] While the mechanical connections are in principle
duction. While production costs are expected to decrease in the easy to detach, the different sizes and shapes of the connec-
medium to long term due to economies of scale, learning curves tions pose a challenge for both human workers and robots.
and technical developments, this should be accompanied by the Standardizing these connections could significantly reduce the
establishment of a circular production chain.[280] In this context, amount of work involved in the disassembly by minimizing the
battery recycling is in constant competition with suppliers of number of tools and steps required. Permanent connections
virgin battery materials, both in terms of prices and material per- based on welds or adhesives, which are often used to assemble
formance.[281,282] Several publications have indicated that better several cells into a module, are much more problematic for dis-
separation of material streams at the beginning of recycling assembly. In order to remove adhesives, organic solvents can
can lead to higher product purity and recycling efficiency, con- be used, which increase costs and pose an additional safety
tributing to a more competitive battery recycling industry.[281–284] risk to human workers.[282,290] Alternatively, adhered cells can
Recently, Thompson et  al. evaluated the recycling costs for ten be detached by heating. However, external heat exposure can
hydrometallurgical recycling processes from the literature and increase the risk of thermal runaways.[291] Flexible cables pose
found that recycling based on shredded starting material offered another problem, especially for robotic disassembly, as they
cost savings of <20% for battery production compared to using can be positioned in unpredictable ways reducing the robots’
virgin materials. In comparison, recycling processes based on freedom of movement and adding complexity. A potential
disassembled batteries as starting material showed cost savings design alternative is a rigid busbar to which individual cells can
of 40–80%, without considering additional disassembly costs.[282] be connected via mechanical connections to form a battery pack

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Figure 5.  Commonly used cell geometries for battery pack construction: a) Pouch cell, b) cylindrical cell, c) prismatic cell. Reproduced according to
the terms of the CC-BY license.[293] Copyright 2020, The Authors, published by MDPI.

in a so-called cell-to-pack design. Such a design reduces the Currently, also high power ultrasonic pulses are being studied
amount of adhesive and cables in the battery pack and simpli- as technology to ease liberation of cathode materials, regardless
fies disassembly into individual cells. A corresponding solution of binder types.[297] The cavitation from the ultrasonic pulses
was presented by the Chinese battery manufacturer BYD with separates the active material from the current collectors in cath-
the so-called “blade battery.” odes. Other methods include thermal processing, high voltage
Disassembly at the cell level is even more challenging since treatment, or mechanical crushing.[111]
manufacturers use different cell geometries, including pris- The issue of active material liberation can also be addressed
matic, cylindrical, and pouch cells (Figure 5). The cell hous- from a material design perspective. The development of new
ings are usually permanently sealed by welding or crimping to binders that can be processed in aqueous solutions or other
reduce the risk of leakage. Built-in designs for an easy opening green solvents like ethanol is of particular interest. Various
of the cells could significantly facilitate the processing. Fea- potential alternatives for PVDF have already been proposed,
tures such as vacuum seals and screw caps could also facilitate for example, polyacrylic acid (PAA), styrene-butadiene rubber
recycling by maximizing the recovery of electrolyte, thereby (SBR), carboxymethylcellulose (CMC), polyethylene (PE) or
improving the recovery of lithium and fluoride compounds.[292] chitosan. While CMC and SBR are already state of the art as
In order to separate electrodes and separator, the jellyrolls of binders for anodes, aqueous processing of cathodes is still
prismatic and cylindrical cells must be unwound. Pouch cells a major constraint due to the high reactivity of commercially
contain stacks of electrodes, which must also be separated. available cathode materials with water. The most promising
Li et  al. reported a disassembly system for pouch cells with results so far have been achieved for LFP cathode materials,
Z-shaped folded electrode-separator compounds consisting of a which have comparatively low sensitivity to water.
vacuum conveyor, multiple pinch grippers, and skimmers.[294]
The system allows automatic separation of anodes, cathodes,
and separators and should also be adaptable for processing 4.2.2. Direct Recycling
prismatic and cylindrical cells. In general, standardization of
cell geometries would contribute to a simplified disassembly. An effective disassembly of batteries also offers opportunities
However, such a severe restriction of design freedom would for the use of new recycling approaches. Especially the concept
significantly limit future innovations in pack and module of direct recycling has received a lot of attention in recent years.
design, including new cooling and battery management The fundamental idea behind direct recycling is to refresh or
systems. reactivate active materials in order to restore the capacity and
Another central challenge for disassembly is the liberation of property losses through cycling, instead of first breaking them
the active materials from the current collectors. A typical binder down into their individual components and then re-synthe-
material for cathodes is polyvinylidene fluoride (PVDF), which sizing them.
has high electrochemical stability and good adhesive proper- By using standardized cell designs and specific battery
ties. However, PVDF only dissolves in very few solvents, one chemistries, the resetting of the lifecycle of batteries becomes
of which is N-methyl-2-pyrrolidone (NMP). The use of NMP a possibility via relithiation and direct recycling. As the bat-
as a solvent to separate the active materials is associated with tery ages, one of the most common indicators of aging is the
high costs and represents a safety risk because it is hazardous, loss of lithium from the layered oxide in the cathodes. After
teratogenic, and irritating.[295] Recently, alternative methods for successful disassembly, the high purity cathode material can
dissolving the PVDF binder, such as supercritical extraction be exposed to high lithium moieties and resintered. A Multi-
with dimethyl sulfoxide (DMSO) as co-solvent[113] or the use tude of approaches have been explored, but the presence of
of green solvents, such as dimethyl isosorbide (DMI)[296] have remained impurities such as different rock salt phases on the
been published. Another chemical method for the liberation material affects its final performance unless a higher tempera-
of the cathode active material is based on the selective etching ture process is used.[298] A thermal reactivation method for
of the aluminum current collector using alkaline solutions.[133] LFP cathodes was presented by Li et  al. who treated the cells

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Figure 6.  Proposed framework for the development of future recycling infrastructures.

at temperatures of 600—800 °C with the addition of a reducing To the best of our knowledge, no research has been pub-
gas and Li2CO3 as Li precursor.[299] Similar approaches were lished on the “upcycling” of battery cathodes from high to low
also published elsewhere.[300,301] Another method based on cobalt chemistries. Nevertheless, changes in battery chemistry
hydrothermal relithiation was investigated by Sloop et  al. and such as cobalt-free cells or sodium-based cells are promising
Shi et  al. The cathode materials were treated in LiOH and within the design for recycling approach. The recycling of
Li2SO4 solutions and then thermally annealed.[302,303] Electro- such cells is still a new topic with very limited studies such
chemical methods for relithiation were also investigated.[298] as a recent report of a fully recyclable Na-ion battery using
The methods include, for example, the treatment of LCO in Na3V2(PO4)3 as the cathode material.[306] The cells have an
an aqueous solution with LiOH and KOH with a small cur- innovative design of stacked electrodes that uses Al foil as a
rent of 1  mA cm−2 applied.[250] In a different procedure, short common current collector between anodes and cathodes.
high-voltage pulses were applied at a frequency of 150 Hz.[304] These batteries can be separated with aqueous based solu-
It is essential to remember that the works on direct relithia- tions with NaOH produced as a by-product. Such designs
tion synergize with a disassembly approach and its efficiency are ideal conditions in design for recycling, but the overall
suffers when coupled with the current shredding approach in electrochemical capacity and stability is still missing sig-
commercial recycling. nificant improvements to properly address the needs of the
More recently, there has been an uptick on the production of market. Some of these limitations are being addressed by the
batteries with recycled materials. Ma et  al. have published the design of new sodium battery chemistries that are more envi-
effects of their recycling process on the performance of recy- ronmentally benign from the start such as: new fluorine free
cled batteries.[305] While the details of their leaching process are electrolytes,[307] and biomass based hard carbons[308] among
not public yet, it is important to notice how the recycling pro- other innovations. Nevertheless, the constantly changing bat-
cess affected the final morphology of the cathode material. The tery compositions are a major limitation for direct recycling,
changes in structure are assigned as one of the main drivers on because the reactivation of cathode materials requires a single-
the improved performance of the material. type material input. At the same time, direct recycling can

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www.advancedsciencenews.com www.advenergymat.de

offer advantages especially for the recycling of cathode mate- recycling approaches having lower environmental footprints.
rials with low intrinsic material value, such as LFP or LMO. This transition will be highly dependent on a stabilization of bat-
The prerequisite for a practical application of direct recycling tery chemistries and an increased ability to recover electrolytes.
will therefore be an efficient sorting of battery types based on a
convenient battery labelling.
Acknowledgements
The authors acknowledge BATTERY 2030+ funded by the European
4.2.3. Future Battery Recycling Infrastructure Union’s Horizon 2020 research and innovation programme under Grant
Agreement No. 957213. The authors from Münster would like to thank
As a result of the above discussion of the regulatory framework, the German Federal Ministry of Education and Research for funding the
projects “InnoRec” (03XP0246C) and “Meet-HiEnD III” (03XP0253A). The
available recycling methods, and future developments, we pro-
authors from Uppsala acknowledge the financial support by the Swedish
pose the recycling flowchart shown in Figure 6 as a foundation Energy Agency via project no. P50122-1 and via STandUP for Energy.
for the development of a future recycling infrastructure. Open access funding enabled and organized by Projekt DEAL.
The framework is based on three interconnecting cycles. In
the first cycle, newly produced batteries first go through a use
phase. The resulting end-of-life batteries are sorted and can Conflict of Interest
either be used as a module in second-life applications or are The authors declare no conflict of interest.
broken down to the cell level in the second cycle. The individual
cells are then sorted again and, according to their condition,
can be directly reused or end up in the final recycling cycle. Keywords
Here the cells are first deactivated and disassembled. The cell
all solid state, circular economy, Lithium ion batteries, next generation,
components can then be converted into secondary active mate- recycling
rials through direct recycling or into secondary raw materials
for battery production through classical recycling approaches. Received: September 20, 2021
An important component of the framework is the data col- Revised: November 29, 2021
lection and analysis, which allows the determination of flow Published online: January 10, 2022
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Jonas Neumann studied Chemistry at the University of Hamburg (Germany) and Business
Chemistry at the University of Münster (Germany). After graduating in 2020, he became a Ph.D.
student at the MEET Battery Research Center in Münster (Germany). His research activities focus
on the development of novel battery deactivation and recycling technologies based on super-
critical extraction.

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Martina Petranikova works as an associate professor at Chalmers University of Technology in

Gothenburg in Sweden. Martina’s work deals with thermal and hydrometallurgical processes to
recover valuable metals from primary sources (ores, concentrates) and secondary sources (spent port-
able and car batteries, steel making dust, waste of electric and electronic equipment, etc.). The
research is based on the development of hydrometallurgical or detoxification technologies involving
processes such as: leaching, solvent extraction, ion exchange, etc. Martina’s research is connected to
the recycling and metallurgical industry. She is also a manager for a pilot plant for separation tech-
nologies at Chalmers University of Technology.

Marcel Meeus retired after a professional career at Umicore and he started a private consulting
company SUSTESCO, Sustainable Energy Services Consulting. He is technical advisor to EMIRI,
the European Materials Industrial Research Initiative.

Jorge D. Gamarra is a postdoctoral researcher at Ångström Advanced Battery Centre at Uppsala

University, Sweden, working on direct recycling of batteries. Jorge received his Ph.D. from the
department of materials and chemical engineering at Vrije Universitet Brussel, Belgium and M.Sc.
from.

Reza Younesi is associate professor at Ångström Advanced Battery Centre at Uppsala University,
Sweden, and research leader of a team of Ph.D. students and postdoctoral researchers.
Dr. Younesi worked as a postdoctoral fellow at Technical University of Denmark (DTU) in
2013–2014. Reza received his Ph.D. from the department of Chemistry–Ångström Laboratory at
Uppsala University and M.Sc. from Royal Institute of Technology (KTH), Sweden.

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Martin Winter has been researching in the field of electrochemical energy storage and conversion
for more than 30 years. His focus is on the development of new materials, components, and cell
designs for lithium ion, lithium-metal batteries and alternative battery systems. Martin Winter cur-
rently holds a professorship for “Materials Science, Energy and Electrochemistry” at the Institute
of Physical Chemistry at the University of Münster, Germany. He is founder and scientific director
of MEET Battery Research Center of the University of Münster and of Helmholtz Institute Münster
(HI MS) “Ionics in Energy Storage,” a division of Forschungszentrum Jülich.

Sascha Nowak studied Chemistry at the University of Münster and got his Ph.D. in Analytical
Chemistry. After his doctorate, he joined the working group of Prof. Winter at the MEET Battery
Research Center in 2009 as a postdoctoral researcher where he established the analytical depart-
ment. From 2010–2012, he was the head of the competence areas Analytics and Recycling
and since 2012 he holds a position as scientific staff as the head of the division Analytics and
Environment, which mainly focuses on electrolyte aging, transition metal migration, and surface
investigations, recycling and second life as well as toxicological investigations.

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