Lithium-Ion Battery Recycling – Overview of

Techniques and Trends

Zachary J. Baum,1* Robert E. Bird,1 Xiang Yu,1 and Jia Ma1

1CAS, 2540 Olentangy River Rd, Columbus, OH 43202, USA

*Email: zbaum@cas.org

SUPPORTING INFORMATION

First commercially introduced in 1991, lithium-ion batteries (LIBs) have become an

indispensable part of modern technology, such as vehicles, consumer electronics, power tools,

medical devices, and backup power systems.1-3 LIBs comprise a cathode, an anode, electrolyte, a

separator, and current collectors. Cathode and anode are where reduction and oxidation reaction

take place, respectively. An electrically insulating separator, typically a microporous polymer

membrane, isolates the cathode from the anode to prevent short-circuiting. With this separator in

place, electrolyte is in contact with both electrodes and allows the transfer of lithium ions, but not

1
electrons, between the two electrodes. Current collectors collect electrical current generated at the

electrodes and bridge with external electric circuit. Commonly used materials for LIB components

are summarized in Table S1.

Table S1. Common materials used for each LIB component 4, 5

Lithium metal oxides or phosphates in polyvinylidene

fluoride (PVDF) binder. LiCoO2 (LCO), LiFePO4 (LFP),
Cathode (~7-22 wt%)
LiMn2O4 (LMO), LiNixCoyAlzO2 (NCA), LiNixMnyCozO2
(NCM)

Anode (~15-17 wt %) Graphite or Si/C composite in PVDF binder

Lithium salts in organic carbonate solvents: lithium

hexafluorophosphate (LiPF6), lithium
Electrolyte (~10-15 wt%)
bis(fluorosulfonyl)imide (LiFSI), lithium 4,5-dicyano-2-
trifluoromethyl-imidazolide (LiTDI)

Separator (~4-10 wt%) Polyolefins

Current collectors (~13-

Aluminum, copper
18 wt%)

Casing (~10-26 wt%) Steel or aluminum

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3
BACKGROUND ON AGING

LIB recycling becomes necessary due to aging of the batteries and their components. LIB aging

occurs through undesirable, irreversible physical and chemical changes taking place cumulatively

during battery cycles,6, 7 and while the exact mechanisms are complex and an active research area,

LIB degradation and failure is generally attributed to: (1) chemical degradation, where less

permeable layers of elemental lithium or lithium compounds are deposited at the surfaces of

electrodes due to electrode side reactions, reducing the amount of lithium ions available for charge

transport and restricting electrolyte flow, leading to capacity loss, conductivity reduction and

power fade; (2) physical degradation, where constant volume expansion and shrinkage of

electrodes during charging and discharging, mainly due to lithium ions moving into and out of the

crystal structures, result in stress and crack formation, which not only compromises the mechanical

integrity of batteries but can in turn exacerbate the chemical degradation.8

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Figure S1. Li-ion battery recycling publications by country/region during the years 2010-2021.

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Table S2. Most frequent patent assignees in Li-ion battery recycling during the years 2010-2021.

Number of Patents Assignees Assignee Country

88 Central South University China

69 JX Nippon Mining & Metals Corp. Japan

65 Brunp Recycling Technology Co., Ltd. China
54 Hefei Guoxuan High-Tech Power Energy Co., Ltd. China
51 Institute of Process Engineering, Chinese Academy China
of Sciences
47 Sichuan Normal University China
45 Sumitomo Metal Mining Co., Ltd. Japan
39 Jingmen GEM Co., Ltd. China
37 Tianqi Lithium Corp. China
31 Hunan Keyking Recycling Technology Co., Ltd. China
28 Kunming University of Science and Technology China
22 Anhui Narada Huabo New Material Technology China
Co., Ltd.
21 Lanzhou University of Technology China
20 Dowa Eco-System Co., Ltd. Japan
15 Commissariat a l'Energie Atomique et aux Energies France
Alternatives
15 Guizhou Zoomwe Resource Recycling Industry China
Development Co., Ltd.
15 Jieshou Nandu Huayu Power Co., Ltd. China
15 Jinchuan Group Co., Ltd. China

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Costs and benefits of LIB recycling
There are a variety of reasons why recycling of used lithium-ion batteries (LIB) makes sense.

As already discussed, battery materials are subject to natural limitations in metal extraction that

create vulnerabilities in the long term. While battery compositions have changed over time, earlier

battery designs that are due for recycling were likely to use more cobalt, one of the key battery

materials with supply limitations. Recycling provides domestic security for battery components. It

also limits the ability of suppliers to control the pricing of battery materials; by providing

alternative sources, particularly sources which are unlikely to coordinate their production and

pricing, recycling should insulate battery manufacturers against short-term price variation.

The major benefit of battery recycling is the ability to reduce the cost of LIB and the energy

costs and emissions of LIB manufacture. In order to understand how recycling may be able to

decrease the effects and costs of battery recycling, the materials used in batteries and their costs

should be defined, and the cost of new materials and recycled materials should be compared.

Lithium is widely prevalent, but difficult to refine with brine and spodumite the primary

sources.9 10 Nickel is a more common metal, but its mining also involves significant environmental

costs. Nickel sulfides are the preferred ores for obtaining nickel, but producing nickel from them

generates large amounts of sulfur oxides (of SOx).11 Alternatively, laterite ores can also be

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processed to nickel, with less pollution than sulfide ores, but they are more complicated to process

and require more energy. Cobalt is often found with nickel, and so many of the environmental

costs of nickel also accrue to cobalt as well. In addition, cobalt is often found as arsenide ores,

which must be liberated to form the free metal. The arsenic compounds formed are toxic and

require safe disposal. Finally, much of the cobalt used in batteries is mined in Africa, where child

labor and small mines are used in many cases to obtain the metal; pollution regulations are likely

to be more limited there as well, increasing the costs of cobalt mining.

For example, Sun et al. concluded that recycling of LMO batteries saved energy only when direct

or physical recycling methods were used, while only direct recycling of lithium cobalt oxide (LCO)

batteries reduced energy expenditures.12 Dunn et al. concluded that recycling aluminum could save

33% of the energy costs of battery manufacture, likely because of the electricity used to refine

aluminum.13-15 Similarly, they that recycling the cathode material and current collectors could

reduce energy use by more than 50%. Recycling any of the cathode materials should reduce GHG

emissions, with recycling LCO reducing CO2 emissions by 60-75%. However, Dunn et al. noted

that the technology used for LIB recycling and the fraction of capacity used were significant factors

in determining the energy saving of recycling; battery recycling at lower capacity usage in a

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recycling facility using older technology can use ten times as much energy as a recycling facility

using more recent technology at maximum capacity.

Wu et al.8 noted in their review that the costs of maintaining facilities is significant. While

transportation costs matter, particularly over long distances, Wu et al. determined the recycling

facility operation increased GHG emissions more than longer transport distances.

Pyrometallurgical methods should save 5-56% of the energy costs of battery manufacture and

roughly 23% of the GHG emissions; while hydrometallurgical methods use less energy as well,

making the reagents for recycling requires significant energy. Physical methods require lower

processing temperatures, making them even more likely to save energy. Solvent extraction is likely

better for minimizing the energy and GHG costs of recycling lithium from LIB than carbonation

because it is performed at ambient temperature and uses acid instead of base, but it also requires

the use of reagents (though the extractants may also be recyclable). They concluded that optimal

recycling methods depended on battery type. NCM batteries were better suited to

hydrometallurgical methods because of the need to separate multiple metals, while

pyrometallurgical methods are simpler to recycle LMO and LFP batteries. Finally, Dewulf et al.16

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concluded that recycling of lithium mixed metal oxide batteries was likely to save 40-60% of the

natural resources of manufacturing the batteries from virgin materials.

One question about LIB is whether the environmental costs of LIB manufacture, use, and

recycling outweigh the reduction in fossil fuel use they enable. Both Wu et al. and Dunn et al.

noted that the benefits of LIB batteries in plug-in electric vehicles depend on the source of the

electricity used to charge them. When coal-heavy electricity sources are used, the benefits of

electric cars are lower than when electricity generated using renewable sources is used. Wu et al.

summarized that electric vehicles reduced GHG emissions in all cases (though increasing pollution

when coal-generated electricity was used). Dunn et al. concluded that internal combustion engine

(ICE)-driven vehicles use 20-25% more energy and generate 15-50% more GHG emissions than

either plug-in or hybrid electric vehicles. However, battery manufacturing causes electric vehicles

to emit up to 3-fold more sulfur oxides (SOx) than ICE-driven vehicles, a situation that LIB

recycling would be likely to ameliorate.

Methods for recovering valuable materials from spent LIBs

In order to recover materials from lithium-ion batteries (LIB) that are not going to be reused,

they must be subjected to a variety of processes. In most cases, LIB must be pretreated after which

10
they can be subjected to pyrometallurgical methods, hydrometallurgical methods, or a combination

of both. Direct methods (methods in which the cathode material is removed for reuse or

reconditioning) require disassembly of LIB to yield useful battery materials,17 while methods to

renovate used batteries into new ones are also likely to require battery disassembly, since many of

the failure mechanisms for LIB require replacement of battery components and thus battery

disassembly. Reuse of LIB in stationary applications will require battery classification and the

determination of charge state and capacity.

Pretreatment

Pretreatment is the set of processes needed to prepare a LIB for recycling.8 Any of the recycling

methods require the batteries to be classified and prepared so that the materials can be

reconditioned or reused for other purposes. Pretreatment includes three sets of processes –

discharge or inactivation, disassembly, and separation.

LIB have residual stored electrical potential which, if rapidly purged, could cause fires or

explosions. If the potential can be retrieved and stored economically,17 LIB can be electrically

discharged. If not, then the batteries need to be deactivated so the battery materials can be removed.

This is often achieved by immersing LIB in an aqueous salt solution, allowing the charge and heat

11
from discharge to be removed rapidly and preventing combustion of organic byproducts. An inert

atmosphere can be used to prevent combustion as well, and liquid nitrogen is also used both to

inhibit combustion and to cool LIB so that they are less likely to overheat and catch fire. Carbon

dioxide is used in some processes as an unreactive gas for battery inactivation.4 The inactivation

step can be combined with the disassembly step to simplify the recycling process. Next, LIB must

be disassembled to recover the individual components. The simplest method is to shred, crush, or

break apart the batteries into small pieces; performing the shredding under an inert atmosphere

allows the deactivation and disassembly steps to be combined. Shredding, however, does not allow

the current collectors or casing to be separated intact. Alternatively, the batteries can be taken apart

manually; however, manual disassembly exposes the workers to the battery materials and requires

a large amount of labor. Automation could reduce labor costs, but requires better recognition

systems than currently available, a limited variety of input batteries, or a consistent system for

battery labeling and classification. Manually disassembled batteries then require further processes

to obtain battery material; either solvent treatment, calcination, dissolution in aqueous NaOH, or

ultrasonication yield the battery materials. 18 Finally, once the battery materials are removed, they

12
need to be separated. Battery materials can be sorted by size using screens, by density using

solutions or airflows, or using filtration.

Pyrometallurgy

Pyrometallurgy is the use of heating (most often using a furnace) to convert the metal oxides

used in battery materials to either metals or metal compounds.19 In reductive roasting (smelting),

the battery materials (after pretreatment) are heated under vacuum or inert atmosphere to convert

the metal oxides to a mixed metal alloy containing (depending on the battery composition) cobalt,

nickel, copper, and iron and slag containing lithium and aluminum. (LIB may in some cases be

directly submitted to smelting, with the current collectors being used as an added reductant; often,

an external reductant is necessary to reduce the battery materials to their component metals.)

Alternatively, addition of salts such as aluminum chloride to the battery materials is used for salt

roasting, allowing the metal oxides to be converted to salts such as cobalt(II) chloride.20 The

temperature required depends on the method used and the composition of the recycled batteries;

pyrometallurgical methods require heating at low temperatures (<150°C) to purge battery

electrolyte and binder, with heating at higher temperature needed to consume the battery case and

other organic polymer-containing components. Reductive roasting then requires leaching of the

13
mixed metal alloy to yield the separated metals, while the slag containing the lithium must be

processed if lithium recycling is desired.

Pyrometallurgical methods require simpler pretreatment methods (most often shredding or

crushing) to prepare batteries for recycling and require fewer different methods to recycle LIB of

differing compositions, shapes and sizes. Lithium is recyclable by some pyrometallurgical

methods, but the methods are most effective for particularly valuable metals such as cobalt.

Pyrometallurgical methods are likely (but not certain) to require lower amounts of reagents than

hydrometallurgical methods. However, pyrometallurgy also has significant drawbacks. It requires

larger investments in facilities than hydrometallurgy or direct recycling. Although the organic

components of batteries provide some of the fuel for heating, pyrometallurgy requires far higher

temperatures (and thus energy consumption) than other battery recycling methods. Salt roasting

requires reagents to yield the metal salt products; reductive roasting requires hydrometallurgical

methods to separate the metals from the alloy and reductants to generate the metal alloy. If battery

materials are desired, both pyrometallurgical methods require further reactions to yield cathode

materials. The slag must also be processed to yield lithium;21 many of the components of LIB

14
cannot be recovered at all using pyrometallurgy. Burning the organic components of LIB requires

pollution mitigation measures.

Hydrometallurgy

Hydrometallurgical methods use solutions (primarily aqueous solutions) to extract (leach) and

separate metals from battery (cathode) materials. The pretreated battery materials (with aluminum

and copper removed earlier) are most often extracted with acidic aqueous solutions. The most

common combination of inorganic leaching reagents used is sulfuric acid and hydrogen peroxide

(with hydrogen peroxide acting as a reductant), while hydrochloric and nitric acid are also

commonly used. Organic acids can be used, with ciric and oxalic acids being most often used.

While organic acids require more energy from reagent use and manufacture, cost more, and

generate more carbon dioxide than inorganic reagents, they are more renewable than inorganic

reagents and so are likely to be preferred.12 Alternatively, base solutions of ammonia with either

ammonium sulfate or ammonium carbonate can be used for extraction. Once the metals have been

extracted into solution, they need to be selectively removed from solution; metal salts are either

precipitated selectively using pH variation or extracted using organic solvents containing

extractants such as dialkyl phosphates or phosphinates.

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 Hydrometallurgy provides metals in forms that can easily be manipulated or used in producing

new LIB, and more of the materials from batteries can be easily recovered by hydrometallurgy

than by pyrometallurgy. The lower temperatures required for hydrometallurgy reduce its energy

intensity. Hydrometallurgical facilities also require less capital than pyrometallurgical ones.

However, hydrometallurgy requires large amounts of water (and, when solvent extraction is used

to separate the metal compounds, organic solvents). The wastewater treatment requirements

(including neutralization) for hydrometallurgy are significant. The pretreatment methods needed

for hydrometallurgical methods are more labor-intensive than for pyrometallurgical methods.

Finally, the methods for metal separation need to be selective to avoid cross-contamination of

battery materials. Bioleaching (metal extraction using bacteria or other organisms) has been

studied,22-25 while it is likely to require less water, reagents, and energy than other

hydrometallurgical methods, it also requires more time to extract metals, thus requiring larger

facilities for equal metal output.

Direct recycling

Direct recycling is the removal of cathode material for reuse or reconditioning.17 To directly

recycle LIB, batteries must be disassembled to obtain the separated components. The cathode

16
material must then be delaminated from the current collector. The lithium content in the cathode

material must then be replenished; lithium often remains trapped in the battery anode and is lost

from the cathode and electrolyte6 and cannot be released, requiring the addition of new lithium to

the cathode material. This also requires methods for determining the composition of the battery

material. The cathode material may then need calcination to restore the appropriate crystal

structure and morphology for use in batteries.

The numbers of publications concerning direct recycling of the five common LIB cathode

materials are shown in Figure S2. Publications discussing direct recycling of LCO batteries make

up the largest fraction of direct recycling publications, followed closely by publications discussing

LFP batteries. While the former is consistent with LCO being the most expensive cathode material,

the high publication volume for LFP direct recycling may be a result of (1) the very low price of

iron, making metallurgical recovery of LFP less economically viable than direct recycling;28 (2)

the strong prevalence of LFP cathodes in electric vehicles, especially in China; and/or (3) LFP’s

fixed stoichiometry as opposed to those of NCA and NCM, ensuring universal applicability of

directly recycled materials in new batteries employing LFP cathodes.

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Figure S2. Prevalence of cathode materials recovered directly in Li-ion battery recycling literature.

The publication trends in different recycling methods can be seen in Figure S3, which shows the

annual numbers of publications involving hydrometallurgy, pyrometallurgy, and direct recycling,

respectively, over the past decade. Consistent with the observation from Figure 1, publications

involving all three methods increased overall and have grown significantly in the past few years.

Hydrometallurgy shows very similar trends to pyrometallurgy in the earlier years, but has

outgrown the latter considerably after 2015, which is not surprising considering hydrometallurgy

18
being favored in new developments due to lower facility costs. Direct recycling, despite its

limitations discussed above and slow initial growth, has also grown substantially in most recent

years.

Figure S3. Publication volume for each respective recycling method during the years 2010-2021.

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Methods
Search strategy
To identify journal articles and patents studying LIB recycling published between 2010 and

2021, the CAS Content Collection was first searched using CAS STN® using the following

Boolean query terms:

LITHIUM AND BATTER? AND (RECYCLE OR RECYCLING) OR (LITHIUM AND

BATTER? AND (RECYCLE OR RECYCLING))/CLM AND 2010-2021/PY

NOT BIOMASS NOT COAL NOT WASTE HEAT NOT LI-CO2 NOT A REVIEW NOT

REVIEW/DT

where “?” indicates 0 or more additional characters in a word, “/CLM” includes results from

patent claims, “PY” indicates publication year, “DT” indicates document type, and open-ended

search terms (without “/FIELD”) match based on title, abstract, and expert-curated keywords and

concepts. The fields “NOT BIOMASS”, etc. were introduced to exclude publications studying

production of battery materials from recycled materials, rather than recycling of battery materials.

This search yielded 4,886 document hits, which were then reviewed to identify false positives and

remove the small number of publications that were neither journal articles not patents. This left

3,596 journal articles or patents on LIB recycling. Categorization of these documents into

20
recycling methodologies was based on method-specific language in titles and abstracts, method-

specific expert-curated concepts, and the combination of expert-curated substances with indicators

of their roles in each respective document. For more information on document searching using

STN and STNext®, please see the User Guides on the CAS website.29

Limitations of publication-based assessment

The conclusions that can be made from our analysis of published documents on lithium-ion

battery recycling have some limitations. First, many of the documents discussing LIB recycling

are Chinese patents, requiring translation which may be inconsistent. Document analysis requires

knowledge of both the substances and the text (particularly the abstract and title), and differences

in translation may yield different search results. Second, some LIB recycling methods may be

protected using trade secrets which are unpublished and hence are not covered by our analysis.

Third, our analysis is limited by the nature of battery recycling processes and their correlation to

the substances prepared. Many pyrometallurgical methods require hydrometallurgical methods to

separate and process the metal components, while others may be refined using multiple methods.

While the substances purified in documents can be identified unambiguously, they may be

discussed in documents where multiple methods are used; thus, the correlation between the

21
methods noted in documents and the methods by which the key substances are purified may not

be strong. Finally, while patents may claim a variety of methods for purifying battery components,

a limited number of the methods may be applied to specific components in the examples; thus, the

linkage between battery components and methods claimed in patents may be weaker than desired.

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