Carbon Capture Science & Technology 5 (2022) 100074

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Carbon Capture Science & Technology

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Full Length Article

A perspective of low carbon lithium-ion battery recycling technology

Ye Shui Zhang a,b,∗, Kirstin Schneider c, Hao Qiu c, Hua Lun Zhu a,b,d
a
School of Engineering, University of Aberdeen, Aberdeen, AB24 3UE, UK
b
Department of Chemical Engineering, University College London, Torrington Place, London, WC1E 7JE, UK
c
Institute of Mineral and Waste Processing, Recycling and Circular Economy Systems (IFAD), Clausthal University of Technology, 38678 Clausthal-Zellerfeld, Germany
d
Department of Chemical Engineering, Imperial College London, London, SW7 2AZ, UK

a r t i c l e i n f o a b s t r a c t

Keywords: With the significant rise in the application of lithium-ion batteries (LIBs) in electromobility, the amount of spent
Lithium-ion battery LIBs is also increasing. LIB recycling technologies which conserve sustainable resources and protect the environ-
Recycling ment need to be developed for achieving a circular economy. Recycling of LIBs will reduce the environmental
Low carbon
impact of the batteries by reducing carbon dioxide emissions in terms of saving natural resources to reduce
Pyrometallurgy
raw materials mining. This work reviewed the most advanced and ongoing LIB recycling technologies, and cat-
Mechanical processing
Hydrometallurgy egorized the reviewed technologies according to the components of the LIB cells, including cathodes, anodes,
Carbon emission electrolyte and separators. Most recycling technologies focus on the recovery of valuable metals, particular for
cobalt by hydrometallurgical method from the cathodes. The commercial process based on the combination of
the pyrometallurgical and hydrometallurgical technologies which was commercially developed by Umicore, and
Retriev, is mainly focusing on the developed hydrometallurgical technology for optimizing the recovering effi-
ciency. There is research undergoing to recover graphite from anodes through Fenton oxidation, froth flotation
and thermal treatment with a combination of hydrometallurgical process. As LIB recycling technologies are under
development, there is great potential to reduce emission of carbon dioxide and this should be a focus in research.
There is also a high need to develop a more advanced LIB recycling technology to recover more valuable materials
with reduced carbon emission, therefore to contribute to “Net zero” ambition.

1. Introduction
Lithium-ion batteries (LIBs) are ubiquitous within portable applica-
tions such as mobile phones and laptops, and increasingly used in e-
mobility due to their relatively high energy and power density. The
global LIB market size is expected to reach $87.5 billion by 2027
(GVR, Lithium-ion Battery Market Size 2020). The manufacturing of
these batteries has largely been performed in the same way since their
initial commercialisation by Sony in the 1990s (Kim et al., 2020). The
LIB cell is predominantly composed of different layers that are cathode
layer, anode layer, a separator, and electrolyte enclosed with a cell hous-
ing (Gratz et al., 2014). The cathode material in LIBs is mostly a metal
oxide, such as lithium nickel manganese cobalt oxide (NMC), lithium
iron phosphate (LFP), lithium cobalt oxide (LCO), lithium manganese
oxide (LMO) and many more coated on aluminium (Al) foil as current
collector (CC). The anode is the negative electrode layer with active
material (AM) (typically graphite) on a copper foil. The electrolyte is
usually sandwiched between the negative and positive electrodes, which
plays an important role in transporting the positive lithium ions between
the cathode and anode. Electrolyte is also insulating electronic conduct-
ing to guarantee the operation of batteries. The electrolyte salts used
include lithium hexafluorophosphate (LiPF6 ). LiPF6 is preferably used
lithium salt in most LIBs (Hu and Lu, 2020). The separator is made of
polymers like polypropylene (PP) or polyethylene (PE). The function of
the separator is to avoid short circuits between the electrodes, as well as
facilitating ion transport in the cell (Zeng et al., 2014, Meshram et al.,
2020).
Spent LIBs recycling gained remarkable attention in the past few
years due to the rapid increase in demand for critical metals, the neg-
ative impact on the environment from raw materials mining and in-
correct disposal of spent LIBs. Spent LIBs not only contain significant
quantities of valuable materials but also contain hazardous compounds
(Meshram et al., 2020). Landfilling spent LIBs can contaminate soil
and groundwater due to electrolyte and metals leaching (Mossali et al.,
2020). Furthermore, LIBs release toxic gases (i.e. hydrogen fluoride, HF)
in contact with moisture and can induce fire accidents if not properly
handled (Mossali et al., 2020, Winslow et al., 2018).
Recycling of LIBs will reduce the environmental impact of the batter-
ies by reducing carbon dioxide (CO2 ) emissions in terms of saving nat-
ural resources to reduce raw materials mining. Therefore, it could also

∗
Corresponding author at: Chemical Engineering, University of Aberdeen, Aberdeen AB24 3UE, United Kingdom
E-mail addresses: yeshui.zhang@ucl.ac.uk, yeshui.zhang@abdn.ac.uk (Y.S. Zhang).

https://doi.org/10.1016/j.ccst.2022.100074
Received 31 August 2022; Received in revised form 8 October 2022; Accepted 8 October 2022
2772-6568/© 2022 The Author(s). Published by Elsevier Ltd on behalf of Institution of Chemical Engineers (IChemE). This is an open access article under the CC
BY license (http://creativecommons.org/licenses/by/4.0/)
Y.S. Zhang, K. Schneider, H. Qiu et al.
manage safety issues and eliminate waste production (Bankole et al.,
2013). It has been reported that 13% of LIB cost per kWh could be saved
through metals recycling. However, the global recycling ratio of the LIBs
was less than 3% in 2007 (Georgi-Maschler et al., 2012). It is found that
the recyclability of LIBs is very low and the recycling process is not ef-
ficient enough to recover Li for reuse in batteries (Yanamandra et al.,
2022). In the EU, the Battery Directive (Directive 2006/66/EC) and the
Waste Electrical and Electronic Equipment (WEEE) Directive (Directive
2012/19/EU) are the most up-to-date regulations regarding the collec-
tion and recycling of spent LIBs. In February 2022, the Committee on
the Environment, Public Health, and Food Safety (ENVI) adopted a po-
sition on proposed rules to govern the entire battery product life cycle
from design to end-of-life. Members of the European Parliament (MEPs)
want to strengthen new EU rules for design, production and disposal of
batteries, in terms of stronger sustainability, performance and labelling
requirements, due diligence policy for value chain of battery companies,
and more stringent targets for waste collection, recycling efficiency and
material recovery. MEPs mentioned the new measures for batteries are
crucial for the transition to a circular and climate-neutral economy and
for EU’s competitiveness and strategic autonomy (GVR, Lithium-ion Bat-
tery Market Size 2022). In March 2022, the EU Environment Council
adopted new rules for more sustainable batteries. It has been reported
that a decision from the Environment Council has been made to final-
ize an agreement between the EU member states, the European Par-
liament and the European Commission. Following its entry into force,
the batteries regulation will replace the EU Batteries Directive of 2006
(EU Environment 2022). The EU is currently in the process of updating
its main legal framework on batteries through its proposal for a sweep-
ing Batteries Regulation. The proposed regulation is “cradle-to-grave,”
applying obligations to each stage of a battery’s life cycle to promote a
circular supply chain. As a first-mover, the EU may hope to provide a
blueprint for the regulatory moves by other countries (Nicolas Lockhart
and Perantakou, 2022).
The EU member countries are required to set up collection schemes
to deal with the end-of-life portable batteries. The battery manufacturers
are liable for the costs of collection, treatment, recycling and disposal.
Battery manufacturers or producers and distributors are required to col-
lect the spent batteries without extra cost. The regulations also set the
minimum collection rates should be 45% by 2016. However, the revised
report updated in 2019 by the European Commission stated only 14
member states have reached the target of 45% by 2016. In total, 56.7%
of spent portable batteries are not collected back every year which is
∼35,000 tons end up in municipal waste streams (Neumann et al., 2022).
The most important incentive for LIBs recycling is the economic
value of the metals contained in the cathode active material, represent-
ing most of the total value (up to 90%) (Lain, 2001). Considering the
recycling feasibility and final gain, currently only cobalt (Co), Cu, steel,
nickel (Ni) and Al are recycled. Plastics are incinerated for energy recov-
ery and Li, Co and manganese (Mn) are recovered by a solvent extraction
system, but graphite is rarely considered (Dewulf et al., 2010). Most of
the spent LIBs recycling processes in industry are only targeting on LCO
(the cost is estimated at 8900$ t−1 ) and LiNi1−x−y Mnx Coy O2 chemistries
because of the high Co and Ni content. However, these processes are not
appropriate for the lower-value manganese-rich cathode chemistries and
LiFePO4 which do not contain precious metals (Winslow et al., 2018).
Considering also the predominant trend to reduce the Co content, robust
recycling processes should be developed to recover LIBs with different
cathode chemistries and to balance treatment costs with the final effec-
tive revenue.
This work reviewed the most developed LIB recycling technologies
and categorized the reviewed technologies according to the components
of the LIB cells, including cathodes, anodes, electrolyte and separator.
The materials that can be recovered from each type of the cell compo-
nents are summarized in section 2. The recent development of the re-
cycling technologies is discussed in section 3. The current challenges of
the existing recycling technologies have been discussed in section 4 with
2
Carbon Capture Science & Technology 5 (2022) 100074
a follow-up discussion in section 5 to discuss the future perspectives for
developing a combined LIB recycling technology to recover more valu-
able materials with reduced carbon emissions, therefore contributes to
“Net zero” ambition.
2. Recoverable Materials
2.1. Cathodes
The raw material production for batteries has a huge ramifying ef-
fect. Mostly the raw materials used in LIBs are extracted from their re-
spective ores with mainly focusing on Li, Co, Ni, and Mn as they are
used in the production of cathode materials in the LIBs. Co is mainly
extracted from its ores accompanied by Ni or Cu along with the little
amount of arsenic and silver (Ag). The approximate global reserve of
Co is about 7,100,000 MT in 2020, Co contained in purchased scrap
represented an estimated 29% of Co reported consumption (recycling)
(USGS 2021).
Li is an important metal as it shares the largest market in the pro-
duction of LIBs. Chile, Australia and Brazil are the main producers of
Li while other important producers include Argentina, Portugal, the US,
and China. The estimated reserves for Li are about 21,000,000 MT in
2020 (USGS 2021). One domestic company has recycled Li metal and
LIBs since 1992 at its facility in British Columbia, Canada. In 2015,
the company began to operate the first US recycling facility for Li-ion
vehicle batteries in Lancaster, OH. Seven other companies located in
Canada and the US have begun recycling or intended to begin recycling
Li metal and LIBs to some degree. The estimated global reserve for Mn
is about 1,300,000 MT (USGS 2021). Mn was recycled incidentally as
a constituent of ferrous and nonferrous scrap. However, scrap recovery
specifically for Mn was negligible. Mn is recovered along with iron (Fe)
from steel slag (USGS 2021).
2.2. Anodes
Current research on recycling anode materials from end-of-life
LIBs mainly concentrates on graphite, which is a critical raw ma-
terial defined by the European Commission (Keersemaker, 2020,
Vanderbruggen et al., 2021). Based on Canaccord Genuity projections,
the need for graphite will reach 250,000 t year−1 in 2025. (Spencer and
Hill, 2016, Natarajan and Aravindan, 2020). The market price of
graphite ranges from 8-13 USD kg−1 , (Natarajan and Aravindan, 2020,
Yi et al., 2021). and the price of high-quality flake graphite is annu-
ally increasing by 10-12% (Badawy, 2016, Liu et al., 2021, Yang et al.,
2019). Since the graphite content in LIBs is between 13.2-22 wt.%,
which is about 11 times that of Li, (Yi et al., 2021, Gaines et al., 2018)
recovering graphite is becoming more economically attractive.
Since the purity of graphite mines are various and needs to be treated
with HF or high temperature to remove impurities and get battery-grade
product with purity higher than 99%, (Young, 2019, Sophie, 2020) the
process will significantly increase the environmental burden. Thus, the
mining activities can be reduced by recovering the graphite from end-
of-life batteries, therefore minimizing ecological damage.
Hence, graphite in end-of-life LIBs should be recycled from economic
and ecological perspectives. From a process point of view, the high
graphite content in the pyrometallurgical process leads to increased
CO2 emission and impacts the metal recovery efficiency caused by
the changed CO2 -to-CO ratio, reaction kinetics, and melting properties
(Werner et al., 2020, Vanderbruggen et al., 2022). Therefore, early sep-
aration of graphite is beneficial for the pyrometallurgical process. In
addition, it can improve the hydrometallurgical process efficiency of
recovering valuable metals by early separating graphite due to the min-
imized feed material volume (Vanderbruggen et al., 2022, Yang et al.,
2021, Zhan et al., 2020). Last, the treated recycled graphite exhibits
some new properties for making new LIB cells, such as high power ca-
pacity and fast charging performance. These are due to the enlarged in-
Y.S. Zhang, K. Schneider, H. Qiu et al.
terlayer space or the element doping through the regeneration strategy,
including gas-phase exfoliation and element doping, which also facili-
tates its reuse as an anode AM (Natarajan and Aravindan, 2020, Li et al.,
2019, Xu et al., 2022).
2.3. Electrolyte and separators
The indispensable electrolyte serves as the medium for the transport
of Li-ions between the electrodes. The electrolyte consists of one or more
lithium salts dissolved in two or more solvents and additives (Xu, 2004).
The electrolyte salt most commonly used is LiPF6 which shows high
electrochemical inertness and forms a passivation film on the Al CC of
the cathode. However, LiPF6 is very sensitive to water and HF forms
(Aurbach et al., 2007). The solvent dissolves the electrolyte salt, for
example the organic carbonates are state-of-the-art solvents.
Cyclic ethylene carbonate (EC) forms a solid electrolyte interphase
(SEI) to prevent graphite exfoliation. Due to the high viscosity of EC,
linear carbonates such as dimethyl carbonate (DMC) are added which
comes with the cost of increased flammability (Schmitz et al., 2014). To
decrease flammability, either flame retardants such as organic phospho-
rus compounds, (Haregewoin et al., 2016) co-solvents such as propylene
carbonate (PC), (Schmitz et al., 2014) or fluorinated solvents are added
(Xia et al., 2021). The electrolyte composition differs for high-voltage
and high-capacity electrodes because it is difficult to find electrolytes
stable beyond 4.4 V vs. Li/Li+ (Wang et al., 2014). One possibility is to
use highly salt-concentrated electrolytes (Pei et al., 2017). Even though
the first pilot line for salt-concentrated electrolytes has installed, con-
ventional electrolytes containing LiPF6 , EC, and DMC will dominate in
the medium term.
The main purpose of the separator is to prevent physical contact
between the positive and negative electrodes. Besides, the separator
fulfils further important tasks in terms of Li-ions transport, thermal
safety, and mechanical stability during cell production and use phase
(Zhang, 2007). The separator consists of at least one microporous layer
and is less than 25 μm in thickness (Lagadec et al., 2019). Three types
of separator materials exist, including polymer membranes, non-woven
fabric mats, and inorganic composite membranes. Most commonly, sep-
arators are based on polyolefin membranes including PP, PE, and mul-
tilayers thereof (Lagadec et al., 2019).
3. Methods for recycling process
3.1. Pretreatments
The most common LIB pretreatment processes are mechanical sep-
aration, mechanochemical process, thermal treatment and dissolution.
The most up to date sequence of the pretreatment processes has been
updated by Kim et al. (2021) which is shown in Figure 1, including
discharge, dismantling, comminution, classification, separation, disso-
lution and thermal treatment.
Discharge The discharge step aims to stabilize the spent cells before
any further treatment, therefore to prevent thermal runway and product
loss caused by fires. Other stabilization process have also been investi-
gated, including ionic self-discharge, electrical discharge, thermal treat-
ment, cryogenic treatment and in-process control (Sommerville et al.,
2020). The typical discharging solution for LIB discharging process are
distilled water and sodium chloride (NaCl) (Ojanen et al., 2018).
Dismantling The dismantling step is a manual process to disas-
semble cells. Disassembly of LIB cells should be performed in a chem-
ically inert environment with great caution regardless the state-of-
charge (Waldmann et al., 2016). The dismantling process normally
comes with volatile organic compound (VOC) emissions (dimethyl
carbonate, C3 H6 O3 and tert-amylbenzene, C11 H16 ) (Li et al., 2019).
Li et al. (2016) designed a gas release and absorption system for de-
tecting the VOCs during the LIB cells dismantling process. To collect the
gas released from dismantled LIB cells, a set of gas collecting system
3
Carbon Capture Science & Technology 5 (2022) 100074
devices was designed independently, including inlet flow purification,
and an emission and absorption container.
Comminution Comminution is a mechanical treatment to crush and
grind the electrodes into smaller pieces.
Classification Classification step aims to improve the homogeneity
of the crushed material particles for higher recycling efficiency, partic-
ularly for the pyrolysis (Zhang et al., 2020).
Separation An advanced separation method is required to further
separate the crushed materials. The magnetic separation is very effective
to remove the magnetic components contain Fe. It is also capable to
separate LCO based cathode materials from Al CC (Shin et al., 2005).
The metallic shells of the crushed materials can be separated and the
non-ferrous components can be separated manually (Gratz et al., 2014).
The commercial Recupyl process will require a high induction magnetic
separator due to the large fraction of steel components (Pinegar and
Smith, 2019). A dissolution step is needed to liberate AM from CCs with
a suitable solvent (eg. N-methylpyrrolidone, NMP) (Contestabile et al.,
2001).
Thermal treatment Thermal treatment can also be used to remove
the binder, electrolyte and conductive material. After the pre-treatment
steps, the separated components can be further treated with different
methods, for example the cathode AM can be recovered by pyromet-
allurgical or hydrometallurgical methods as described in section 3.2,
roasting process as described in section 3.3, and liquid or supercriti-
cal carbon dioxide (CO2 ) extraction, low-temperature volatilization, py-
rolysis, roasting, wet comminution, and pyrometallurgy. The separator
can be collected directly by mechanical separation process or can be
removed by the methods introduced in section 3.4.
In general, the pretreatment of the end-of-life LIBs are crucial for
achieving a high recycling efficiency with consideration of low energy
consumption and eliminated safety concerns. The most difficult con-
straint for the current LIB pretreatment routes is the comminution pro-
cess due to the inhomogeneity of the battery components. The separa-
tion of the mixed battery components is mainly a physical process which
also produces cross contamination from various recycling streams. There
is indeed a need to improve the current separation process for develop-
ing an economical LIB recycling method (Sommerville et al., 2020).
3.2. Cathodes
The most common cathode recovering methods are pyrometallur-
gical and hydrometallurgical methods. Pyrometallurgical method for
recovering AM of cathode from spent LIBs is a thermal pretreatment
method which has been developed in both of lab-scale and industry-
scale. The typical AM in LIB cathodes include LCO, LiCoNiO2 and
NMC as summarized in Table 1, Table 2 and Figure 2. The pyromet-
allurgy is requiring elevated temperatures to recover valuable metals
from spent LIBs through physical and chemical transformations to pu-
rify the mixed components. Physical transformation including phase
changes and structural changes of the components happen at tempera-
ture between 200-600°C. (Makuza et al., 2021). Higher temperature up
to 1600°C is required to promote the chemical reaction. There are var-
ious parameters involved in the pyrometallurgical process that would
significantly affect the recovering efficiency, including temperature, re-
tention time, purge gas and flux addition (Makuza et al., 2021). The
pyrometallurgical process is mainly for removing the organic compo-
nents from spent LIBs (Makuza et al., 2021). A summary of cathode AM
recovering from spent LIBs by pyrometallurgical methods are listed in
Table 1 and Figure 2, including reduction roasting, sulfation roasting,
nitration roasting, microwave carbothermic reduction, reduction smelt-
ing and oxygen-free reduction.
A hydrometallurgical recovering method is a prevailing technology
to recover the valuable transition metals from cathodes, including Li,
Co, Mn and Ni (Arshad et al., 2020). The process can be categorized
into 4 sections including leaching, impurity removal, metal (Ni, Co,
Mn) recovery, and Li recovery. Firstly, the spent cathode material is
Y.S. Zhang, K. Schneider, H. Qiu et al. Carbon Capture Science & Technology 5 (2022) 100074

Table 1
A summary of cathode AM recovering from spent LIBs by pyrometallurgical methods. Adapted with permission from reference (Makuza et al., 2021). Copyright
2021 Elsevier.

Cathode
Pyrometallurgy technique material Additive Condition Recovery efficiency

Reduction roasting with LiNiMnCoO2 C 650°C, 0.5h Li 94%, Ni 93%, Co 98%, Mn 99%.
hydrometallurgical leaching (Liu et al., 2019)
Sulfation roasting with water LiCoO2 SO2 (g) 700°C, 2h Li ∼100%, Co 17%. (Shi et al., 2019)
leaching
Sulfation roasting LiNiMnCoO2 Na2 SO4 750°C, 1.5h Li 85%. (Di et al., 2020)
Nitration roasting LiCoO2 HNO3 250°C, 1h Li 93%. (Peng et al., 2019)
Vacuum pyrolysis LiCoO2 C 600°C Li 93%, Co 99%. (Tang et al., 2019)
Vacuum-gasification- LiNiMnCoO2 Al 1240°C, 2h Co 91%. (Yao et al., 2021)
condensation
Chlorination calcination LiCoO2 NH4 Cl 350°C, 0.3h Li 99%, Co 99%. (Fan et al., 2019)

Microwave carbothermic LiNiMnCoO2 C 900°C, 0.5h Li ∼100%, Ni, Co 98%,

reduction with HCl leaching Mn 97%. (Fu et al., 2020)
Carbothermic reduction smelting LiCoNiO2 Cu slag (slag former) 1450°C, Co 99%, Ni 98%, Cu 94%. (Ren et al.,
0.5h 2017)
Reduction smelting LiNiMnCoO2 Pyrolysis slag 1350°C, Li 80%, Mn 95%. (Ren et al., 2017);Mn
former, SiO2 , CaO; 0.5h 80%, Li 95%. (Guoxing et al., 2016)
MnO-SiO2 -Al2 O3
slag
Oxygen-free roasting LiCoO2 C 1000°C, Co 96%, Li 99%. (Li et al., 2016)
0.5h
(Note: (g) = gas phase)

Table 2
A summary of leaching agents and reducing agents in the reviewed hydrometallurgical process for recycling of cathode AM from LIBs.

Conditions (Temperature,
leaching time, concentration
LIB composition Leaching agent Reducing agent and pulp density) Recovery efficiency

LiCoO2 HCl - 95°C; 3 h; 3 M; 100 g L−1 Li 99 %; Co 100 %. (Zhang et al., 1998)

LiCoO2 HNO3 H2 O2 75°C; 0.5 h; 1 M; 20 g L−1 Li 85 %; Co 85 %. (Lee and Rhee, 2002)
LiCoO2 H2 SO4 - 70°C; 6 h; 3 M; S/L=1:5. Li 80 %; Co 97 %; Cu 98%. (Nan et al., 2005)
LiCoO2 H2 SO4 H2 O2 65°C; 1 h; 6 %; 33 g L−1 Li 90-95 %; Co 70-75 %; Al 60-70 %; Cu ∼90 %. (Dorella and
Mansur, 2007)
LiCoO2 DL malic acid H2 O2 90°C; 0.7 h; 1.5 M; 20 g L−1 ∼ Li 100%; Co 90 %. (Li et al., 2010)
Mixture (LiCoO2 , Citric acid (C6 H8 O7 ) H2 O2 90°C; 1 h; 0.5 M; 20 g L−1 Li, Co, Mn, Ni >95 %. (Li et al., 2018)
LiCo1/3 Ni1/3 Mn1/3 O2 ,
LiMn2 O4 )
LiCoO2 H2 SO4 C6 H12 O6 90°C; 3 h; 2 g/g; 100 g L−1 Li 97 %; Co 98 %. (Granata et al., 2012)
LiCoO2 H2 SO4 Na2 S2 O3 90°C; 3 h; 3 M; L/S=15:1 Li ∼100 %; Co 100 %. (Wang et al., 2012)
LiCoO2 H2 SO4 NaHSO3 95°C; 4 h; 1 M; 20 g L−1 Li 97 %; Co 92 %; Ni 96 %; Mn 88 %. (Meshram et al., 2020)
LiCoO2 Oxalate (H2 C2 O4 ·2H2 O) H2 O2 80°C; 2 h; 1 M; 50 g L−1 Li >98%; Co >98 %. (Sun and Qiu, 2012)
LiCoO2 Citric acid (C6 H8 O7 ) Ascorbic acid 80°C; 6 h; 1 M; 20 g L−1 Li ∼100 %; Co ∼80 %. (Nayaka et al., 2015)
NMC Biodegradable trichloroacetic H2 O2 60°C; 0.5 h; 3 M; 50 g L−1 Li ∼100 %; Co 92%; Ni 93 %; Mn 90 %. (Zhang et al., 2015)
acid
LiCoO2 Citric acid (C6 H8 O7 ) Phytolacca 90°C; 2 h; 1.5 M; 50 g L−1 Li 96 %; Co 83 %. (Chen et al., 2015)
americana
Mixed cathodes Succinic acid (C4 H6 O4 ) H2 O2 70°C; 0.7 h; 1.5 M; 15 g L−1 Li >96 %; Co ∼100 %. (Li et al., 2015)
LiCoO2 Subcritical water+polyvinyl - 350°C; 0.5 h; 3:1; S/L Li ∼98 %; Co >95 %. (Liu and Zhang, 2016)
chloride (PVC) (PVC:LiCoO2 )=16:1
Mixed cathodes Tartaric acid (C4 H6 O6 ) H2 O2 70°C; 0.5h; 2 M; 17 g L−1 Leaching efficiency: Li 99 %; Co, Mn, Ni 99%. (He et al., 2017)
LiCoO2 Maleic acid Ascorbic acid 80°C; 6 h; 1 M; 2 g L−1 Dissolution: Li ∼100 %; Co 97 %. (Nayaka et al., 2016)
LiCoO2 Tartaric acid (C4 H6 O6 ) Ascorbic acid 80°C; 5 h; 0.4 M; 2 g L−1 Li ∼100 %; Co 97 %. (Nayaka et al., 2016)
(chelating
agent)
LiCoO2 Glycine Ascorbic acid 80°C; 6 h; 0.5 M; 2 g L−1 Dissolution: Li ∼100 %; Co >95 %. (Nayaka et al., 2016)
LiNi1/3 Co1/3 Mn1/3 O2 Formic acid H2 O2 60°C; 2 h; 2 M; 50 g L−1 Li ∼100 %; Co, Ni, Mn ∼85 %. (Gao et al., 2017)
LiCoO2 Malic acid Grape seed 80°C; 3 h; 1.5 M; 20 g L−1 Li ∼99 %; Co ∼92 %. (Zhang et al., 2018)
Mixed cathodes - 80°C; 0.2 h; 1:0.5:1 M; 10 g Co ∼100 %. (Ku et al., 2016)
NH3 +(NH4 )2 SO3 +(NH4 )2 CO3 L −1
LiNi1/3 Co1/3 Mn1/3 O2 Acetic acid (CH3 COOH) H2 O2 70°C; 1 h; 1 M; 20 g L−1 Li 98 %; Co, Ni, Mn 98 %. (Li et al., 2018)
LiCoO2 Benzenesulfonic acid H2 O2 90°C; 1.3 h; 0.75 M; 15 g L−1 Li 100 %; Co 97 %. (Fu et al., 2019)
(C6 H5 SO3 H)
LiCoO2 Citrus acid Tea waste 90°C; 2 h; 12 M; 50 g L−1 Dissolution: Li, Ni, Mn ∼100 %; Co ∼90 %. (Chen et al., 2019)
LiNi1/3 Co1/3 Mn1/3 O2 Citrus juice - 90°C; 0.5 h; 50 g L−1 Li ∼100 %; Co 94 %; Mn 99 %; Ni 98 %. (Pant and
Dolker, 2017)
(Note: S/L=solid-to-liquid ratio)

4
Y.S. Zhang, K. Schneider, H. Qiu et al.
mixed with weak acid. Acid and reducing agent are then added into the
slurry to leach out Li+ , Ni2+ , Co2+ , Mn2+ , Fe2+ , and Al3+ . Secondly, the
unwanted impurities can be removed through pH adjustment. Thirdly,
metal can be recovered via a chemical precipitation or a solvent extrac-
tion. Lastly, Li can be recovered by chemical precipitation using sodium
carbonate (Na2 CO3 ) or by crystallization by distillation (Jung et al.,
2021). The main step involved in the hydrometallurgical process is
leaching process, the collected cathode AM will be leached with dif-
ferent leaching agents as shown in Table 2 and Figure 2, including hy-
drogen chloride (HCl), nitric acid (HNO3 ), sulfuric acid (H2 SO4 ), malic
acid (C4 H6 O5 ), citric acid (C6 H8 O7 ), oxalate (C2 O4 2− ), biodegradable
trichloroacetic acid (C2 HCl3 O2 ), succinic acid (C4 H6 O4 ), tartaric acid
(C4 H6 O6 ), glycine (C2 H5 NO2 ), formic acid (CH2 O2 ), mixture of NH3 ,
(NH4 )2 SO3 and (NH4 )2 CO3 , acetic acid (CH3 COOH) and benzenesul-
fonic acid (C6 H6 O3 S). Citrus juice has also been investigated as a leach-
ing agent in the cathode AM recovering process (Pant and Dolker, 2017).
The conventional hydrometallurgical process requires the strong inor-
ganic acids as leaching agents to dissolve the metals, which may not
be feasible for large scale applications. The latest investigation on the
recovering of cathode AM in a pilot-scale is using HCl as leaching agent
only (Mossali et al., 2020). The hydrometallurgical process is controlled
by various parameters, including temperature, type of leaching agent
and concentration, reaction time and solid-to-liquid ratio. As summa-
rized in Table 2 and Figure 2, the temperature is in a range between 60-
95°C, the concentration is between 0.4-3 M, the pulp density is between
2-100 g L−1 .The most common used reducing agent is hydrogen perox-
ide (H2 O2 ), other reducing agents are also considered, including glucose
(C6 H12 O6 ), sodium thiosulfate (Na2 S2 O3 ), sodium bisulfite (NaHSO3 ),
ascorbic acid (Vitamin C), Phytolacca Americana, grape seed and tea
waste.
Hydrometallurgical recovering method is highly effective for all
types of battery chemistries recovering. The reported recovery efficiency
with HCl for recycling Co and Mn can reach to ∼99% at 50°C. Two
hours leaching time is required to attain the optimum recovery effi-
ciency (Barik et al., 2017) The process is not requiring high tempera-
ture which eliminated energy consumption. The recovered Li through
hydrometallurgical process is in carbonate form which can be reused as
raw material to manufacture new batch of cathode AM (Mossali et al.,
2020)
3.3. Anodes
The graphite recovery process mainly consists of separating graphite
from CC foils and purification. Graphite particles stick to the CC foils due
to the binder, so breaking the adhesion of graphite particles to the foils
5
Carbon Capture Science & Technology 5 (2022) 100074
Figure 1. The most up to date pre-
treatment sequence for end-of-life LIBs.
Adapted with permission from reference
(Kim et al., 2021). Copyright 2021 Else-
vier.
is the key to separation. It can achieve the separation by using the princi-
ple of similar phase dissolution, where an organic solvent is used to dis-
solve the binder and make the graphite particles peel off from the foils.
A summary of the anode recovering process is illustrated in Figure 3. N-
methyl pyrrolidone (NMP), (Song et al., 2017) DMC, (Zuo et al., 2014)
dimethylformamide (DMF), (Natarajan et al., 2015) dimethylacetamide
(DMAC), (Song et al., 2017, Li et al., 2009, Zhou et al., 2021). Dimethyl
sulfoxide (DMSO) (Zeng and Li, 2014) and ionic liquids (Zeng and
Li, 2014) have been used to dissolve the binder in previous studies.
Also, thermo-treatment (Zhang et al., 2018, Zhang et al., 2019) and me-
chanical processing (Zhang et al., 2018) are often combined to separate
graphite and CC foils as summarized in Figure 3.
As shown in Figure 3, a mixture detaches from the CC foil after the
separation step, which consisting of mainly cathode AM and anode AM,
known as black mass (BM). As a conventional separation technique es-
tablished since the end of the 19th century, froth flotation has been
widely employed for separating and enriching minerals based on their
surface hydrophobic differences (Qiu et al., 2021). In recent years, flota-
tion techniques to separate graphite from the BM in the purification
process have attracted increasing attention because of the significant
surface hydrophobic differences between graphite and cathode AM par-
ticles. Nonetheless, the surface of electrode AM particles is covered with
binder residues, which reduces the wettability difference between an-
ode and cathode particle surfaces, thus reducing the flotation efficiency
(Zhang et al., 2014, Zhang et al., 2014). On the other hand, Qiu et al.
(Qiu et al., 2022) performed a full factorial experimental design and re-
vealed that flotation of untreated BM could not achieve effective separa-
tion and high graphite purity. Also, the styrene butadiene rubber (SBR)
and electrolyte residues such as EC, ethyl methyl carbonate (EMC) and
diethyl carbonate (DEC) were detected (Qiu et al., 2022, Peschel et al.,
2022). An electrochemical method has been extensively applied to ex-
tract and precipitate valuable metals from complicated systems contain-
ing a mixture of special precipitants including OH− , CO3 2− , and C2 O4 2−
anions and metals. For example, Li can be removed by chemical pre-
cipitation using K2 CO3 . (Arshad et al., 2020). Therefore, a suitable pre-
treatment method to remove organic residues must be introduced prior
to flotation. The pretreatment methods are mainly divided into Fenton
oxidation, thermal, and mechanical pretreatment in current studies as
summarized in Figure 3.
Fenton oxidation, which is one of the advanced oxidation techniques,
is a method frequently used for wastewater treatment. It generates hy-
droxyl radicals that have the strong oxidizing ability to degrade or-
ganic compounds into more minor or less harmful compounds by adding
Fe2+ /H2 O2 (Pera-Titus et al., 2004). He et al. (2017) employed the Fen-
ton oxidation for BM pretreatment to remove binder residues followed
Y.S. Zhang, K. Schneider, H. Qiu et al.
Figure 2. A summary of LIB cathode recycling techniques.
by flotation. Besides Fenton oxidation, pyrolysis (oxygen-free) and roast-
ing (oxygen atmosphere) have likewise been used as pretreatment meth-
ods for BM. Although roasting is an excellent approach to remove or-
ganic residues, (Yang et al., 2021, Qiu et al., 2022, Wang et al., 2018)
toxic gases are also generated (Cheng et al., 2022) and graphite loses
some of its mass during roasting (Wang et al., 2018). In contrast, the
pyrolysis method is capable of removing organic residues, recovering
and utilizing pyrolysis products, thus reducing toxic gases (Zhang et al.,
2019, Zhang et al., 2021). However, at high pyrolysis temperatures
or with prolonged duration of the process, pyrolytic carbon is gener-
ated due to the sintering phenomenon, thus affecting flotation efficiency
(Zhang et al., 2019, Zhang et al., 2018). Zhang et al. (Zhang et al., 2021)
pretreated the BM by pyrolysis and removed organic residues from the
particle surface when the pyrolysis temperature reached to 550°C.
Mechanical pretreatment is often used as an adjunct to thermal pre-
treatment to achieve better removal of organic residues. Zhang et al.
(Zhang et al., 2018) reported an ultrasonic treatment method to remove
residual pyrolytic carbon from the BM after pyrolysis. Attrition-assisted
6
Carbon Capture Science & Technology 5 (2022) 100074
flotation was introduced by Vanderbruggen et al. (Vanderbruggen et al.,
2022) to remove organic residues and reduce agglomeration from the
BM after pyrolysis. Liu et al. (Haregewoin et al., 2016) reported a cryo-
genic grinding to remove organic residues from the particle surface. At
present, non-ionic collectors such as kerosene or n-dodecane are used
as flotation chemicals in most of flotation experiments, and concentrate
of the collected graphite after the flotation process has a purity of up
to 80% (Vanderbruggen et al., 2022, Qiu et al., 2022, Yu et al., 2018).
It has been reported that the grade of microcrystalline graphite varies
among 20-40% in graphite content, and its purity fluctuates from 70-
85% carbon after being processed (Jara et al., 2019).
Another common purification method for treating end-of-life LIBs
is hydrometallurgy. Usually, H2 SO4 , HCl, and organic acids are used
as leaching agents with the aim of transferring the metals from the
BM to the solution. After leaching, the purity of graphite can exceed
99% (Gao et al., 2020, Engels et al., 2022). Nevertheless, the recovered
graphite still has impurities that require further purification to be reused
in battery production (Zeng et al., 2014). Ma et al. used 5 M H2 SO4 and
Y.S. Zhang, K. Schneider, H. Qiu et al.
Figure 3. A flow chart of LIB anode recycling techniques.
Table 3
Global warming potential of major methods for recovering graphite.
Recovering techniques
Fenton oxidation assisted flotation (He et al., 2017)
Pyrolysis assisted flotation (Zhang et al., 2019)
Leaching and filteration (Ma et al., 2019)
Curing, leaching and calcination (Gao et al., 2020)
Calcination and leaching (Yang et al., 2019)
Oxygen-free roasting and magnetic separation (Li et al., 2016)
35% H2 O2 to leach the crushed end-of-life LIBs twice at ambient tem-
perature. Most of the metal impurities were transferred into the leaching
solution, and the leached residue was dried and sintered with NaOH at
500°C for 40 min to get graphite products (Ma et al., 2019). Gao et al.
(Gao et al., 2020) attempted to combine the H2 SO4 curing, leaching,
and calcination processes. The impurity containing spent graphite was
first cured with concentrated H2 SO4 to convert the metal oxides into sul-
fates (NiSO4 , CoSO4 , MnSO4 ). Afterward, dilute H2 SO4 was added for
leaching. The leached residue was dried and then calcinated at 1500°C
under Ar atmosphere for 2 hours to remove organic and sulfate residues.
Yang et al. (Yang et al., 2019) pyrolyzed the anode layer at 400°C under
Ar atmosphere and separated graphite from the Cu CC. The residual Cu
foil was then roasted and oxidized at 500°C. Finally, the graphite was
obtained by acid washing with 1 M HCl and 4% H2 O2 .
In addition to the above methods, some other approaches were also
studied. Li et al. reported the recovery of valuable metals and graphite
by anaerobic roasting and magnetic separation. End-of-life LIBs were
crushed and screened, then roasted at 1000°C for 30 min under ni-
trogen (N2 ) atmosphere to reduce LiCoO2 . Finally, graphite was sep-
arated from Co metal by magnetic separation (Li et al., 2016). Yi et
al. reported removing the binder by roasting the anode at 1400°C un-
der N2 atmosphere. The Cu was roasted to spherical particles and then
separated from graphite by ultrasonic vibration and sieving (Yi et al.,
2020). Cao et al. used an electrolytic method to separate Cu foil and
graphite. The purity of graphite can reach to 95% (Cao et al., 2021).
Rey et al. (2021) performed a life-cycle analysis of the above major
methods for recovering graphite and introduced the global warming po-
tential (GWP) for comparison. The authors haven calculated the amount
of CO2 equivalent required per kg of graphite recovered. As shown in
Table 3, pyrolysis assisted flotation, and calcination and leaching recov-
ering techniques have the lowest GWP of 0.53 kg·CO2 equiv.·kggraphite −1
and 1.08 kg·CO2 equiv.·kggraphite −1 , respectively. Fenton-assisted flota-
tion technique comes with the highest CO2 emission which is 48.41
7
Carbon Capture Science & Technology 5 (2022) 100074
GWP / kg·CO2 equiv.·kggraphite −1
48.4 (Rey et al., 2021)
0.53 (Rey et al., 2021)
2.49 (Rey et al., 2021)
2.89 (Rey et al., 2021)
1.08 (Rey et al., 2021)
6.82 (Rey et al., 2021)
kg·CO2 equiv.·kggraphite −1 . It is obvious that the GWP varies consider-
ably for different recovery methods.
3.4. Electrolyte
Several unit operations can recover and/or remove the electrolyte.
Examples are liquid or supercritical CO2 extraction, low-temperature
volatilization, pyrolysis, roasting, wet comminution and pyrometal-
lurgy. These processes can be distinguished between recovery processes
and processes rendering the hazardous substances harmless for down-
stream processing. The separator can be recovered by mechanical sepa-
ration processes, but its recycling is rarely addressed in research. There-
fore, the focus in the following is on electrolyte recycling. The integra-
tion of electrolyte recycling in LIB recycling flowsheets is presented in
Figure 4.
Supercritical CO2 is suitable as an extractant for the electrolyte but
proof-of-principle experiments showed that LiPF6 was only extracted in
traces (Grützke et al., 2014, Liu et al., 2014). Grützke et al. (2015) per-
formed flow-through experiments with liquid and supercritical CO2 . The
authors demonstrated that the addition of co-solvents resulted in im-
proved recovery for all components but most effectively for LiPF6 . The
overall recovery for liquid CO2 extraction with acetonitrile (C2 H3 N)
and PC (C4 H6 O3 ) mixture ration at 3:1 mixture was 89.1 wt.% and
yielded a mixture with almost the original composition. Furthermore,
they showed that extraction is a polarity predominant process. Linear
carbonates such as DMC are better recovered with less polar liquid CO2
and cyclic carbonates such as EC with more polar supercritical CO2 .
The integration of liquid and supercritical CO2 extraction in a re-
cycling process was investigated by Sloop et al. and Rothermel et al.
(Rothermel et al., 2016, Sloop et al., 2020). For a direct recycling pro-
cess, Sloop et al. (Sloop et al., 2020) applied liquid CO2 extraction be-
fore shredding the battery cells. The applied pressure of 62 bar broke
the seal of the cylindrical cells which allows the extractant to pene-
Y.S. Zhang, K. Schneider, H. Qiu et al. Carbon Capture Science & Technology 5 (2022) 100074

Figure 4. Schematic overview of LIB recycling processes with a focus on electrolyte recycling. Process steps that incorporate electrolyte recovery and/or removal are
highlighted: A - Mechanical processing including wet comminution, B - Mechanical processing and thermal treatment, C - Thermal pre-treatment methods followed
by mechanical processing, D - Pyrometallurgical processing. Discharge is commonly applied but might be omitted in the case of wet comminution processes. Dashed
lines represent processes at research level. Own illustration based on data from (Zhang et al., 2020, Zhang et al., 2018, Zhang et al., 2019, Georgi-Maschlera et al.,
2012, Tao et al., 2021, Tao et al., 2022, Tao et al., 2022, Diaz et al., 2018, Lombardo et al., 2020, Rothermel et al., 2016, Sloop et al., 2020, Zhong et al., 2019,
Stehmann et al., 2018). (EoF = End-of-life)

trate the cell and dissolve the electrolyte. 50% of the electrolyte was
recovered as a clear solution composed of EMC:EC (3:1) including ap-
proximately 1/3 of conducting salt (Sloop et al., 2020). Rothermel et al.
(Rothermel et al., 2016) investigated the feasibility of graphite recycling
by applying two different CO2 extraction concepts followed by thermal
treatment of graphite at 1,000°C for 5 h in an inert atmosphere. If the
electrolyte is not recovered before thermal treatment, the graphite sur-
face contains decomposition products from the conductive salt, which
affected the electrochemical performance of the recycled graphite. Liq-
uid CO2 extraction with C2 H3 N as co-solvent is considered the best
because the recycled graphite showed the best electrochemical perfor-
mance (Rothermel et al., 2016). The aforementioned studies recovered
the electrolyte but did not use the reclaimed electrolyte to test new cells
with it which has been done by Liu et al. (Liu et al., 2017). Their process
consists of supercritical CO2 extraction and purification by an anion ex-
change resin as well as a molecular sieve. After chemical analysis, the
substances were added accordingly to achieve the original ratio. The
cells with reclaimed electrolyte exhibited high ionic conductivity close
to the commercial electrolyte with the same composition (Liu et al.,
2017).
Wet comminution processes produce a high volume of wastewater
which needs extensive treatment to remove organic solvents and water-
soluble electrolyte components (Werner et al., 2022). If electrolyte re-
covery from the wastewater is possible, further investigation is required
to prove the feasibility and it is not the focus of operating companies.
The separator can be recovered in subsequent mechanical processing.
The advantage of wet comminution is that undischarged traction LIBs
can be processed. Thermal processes are frequently employed in LIB
recycling. Figure 5 illustrates which reactions of the electrolyte’s main
components and separator can be expected to occur with increasing tem-
perature. In the following, thermal processes are presented in the order
of increased process temperature.
Low-temperature volatilization is performed at temperatures be-
tween 50 and 120°C in an inert atmosphere to remove organic solvents
(Zhong et al., 2019, Werner et al., 2022; Zhong et al., 2020). The boil-
ing temperature of solvents can be reduced by 60-80°C if the overall
pressure of the system is lower (Zhong et al., 2019). The condensed or-
ganic solvents are mostly assigned to the low-boiling components, and
only a part of the high-boiling components is recovered (Zhong et al.,
2019, Werner et al., 2022). Solvent recoveries up to 90 % were reported
(Zhong et al., 2019). Besides common electrolyte solvents, Stehmann et
al. (Zhong et al., 2019) detected a small extent decomposition products
such as methanol and ethanol. Therefore, the condensed solvent requires
refining for recycling and the fluorine contained in the gas phase needs

8
Y.S. Zhang, K. Schneider, H. Qiu et al.
Figure 5. Schematic illustration showing which reactions of the main components of the electrolyte and separator can be expected to occur with increasing process
temperature. Own illustration based on data from (Zhong et al., 2019, Feng et al., 2018, Wang et al., 2006, Campion et al., 2005).
proper treatment (Campion et al., 2005). Since this process is econom-
ically challenging, the condensed solvent is more commonly used as a
substitute fuel, for example in the cement industry. The conducting salt
LiPF6 is unlikely to be recovered because decomposition starts at 60°C
(Campion et al., 2005).
Shredded LIBs or LIB modules or cells can be processed by pyrolysis
which will produce gas, oil and solid fractions. Pyrolysis is typically per-
formed between 250 and 550°C or even higher (Georgi-Maschler et al.,
2012, Zhang et al., 2019, Tao et al., 2021, Tao et al., 2022, Tao et al.,
2022, Diaz et al., 2018, Zhang et al., 2022, Zulkornain et al., 2021). Opti-
mum conditions for temperature, residence time, and gas flow rate vary
according to the battery chemistry (Tao et al., 2021, Tao et al., 2022,
Tao et al., 2022). At 250°C, battery cells can be safely deactivated for
further processing and treatment. The volatile organic electrolyte evap-
orates can be collected in a condenser (Georgi-Maschler et al., 2012).
If the temperature is raised to 450 - 550°C, most of the binder and sep-
arator are degraded into pyrolytic oil and gas. Reducing gases in py-
rolytic gas and graphite can synergistically reduce the cathode powder
to low-valence oxides and convert Li into lithium carbonate (Li2 CO3 )
to facilitate downstream processing (Zhang et al., 2020, Tao et al.,
2021, Tao et al., 2022). According to Georgi-Maschler et al. (Georgi-
Maschler et al., 2012), electrolyte recovery is not feasible since the con-
densate also contains various decomposition products which makes di-
rect reuse impossible. Nevertheless, approximately 80 % of EMC and EC
were recovered at 250°C. The electrolyte salt LiPF6 decomposes at tem-
peratures above 60°C and therefore cannot be recovered by pyrolysis
(Campion et al., 2005).
Incineration of LIB in an oxidative atmosphere at 600°C decomposes
the organics present and releases gas composed of CO2 , CO, and H2 O.
Toxic fluoride-containing compounds are present in both gas and liquid
organic by-product which need proper handling, for example wearing
personal protective equipment (Lombardo et al., 2020). In pyrometal-
lurgy, the electrolyte and the separator are utilized as reductants, and
they mainly report to the gas phase (Cheret and Santén, 2005). The
decomposed electrolyte constituents damage the refractory linen in the
furnace and require extensive gas treatment (Murakami et al., 2020). All
things considered, pyrometallurgy and incineration are robust process-
9
Carbon Capture Science & Technology 5 (2022) 100074
ing routes to remove the electrolyte and the separator. This can have a
positive impact on downstream processing although both components
are not recovered. But the fulfilment of high mass recovery rates might
not be possible as a generic battery system consists of approximately
12 wt.% of electrolyte (Diekmann et al., 2016).
4. Challenges of existing recycling methods
4.1. Cathodes
The life cycle of LIBs defines the complexity in disposition of spent
LIBs. This is due to presence of various interim routes, including reuse
in batteries, use of remanufacturing material in batteries, and regener-
ation of cathode before recycling for use as battery grade material by
stoichiometric additions. A detailed environmental assessment for the
production of LIBs as well as their recycling has been put forth with the
need to pinpoint the precise unit operation that contributes maximum
towards environmental degradation and emission of GHGs. The envi-
ronmental impacts of the production of several different batteries were
studied by McManus (McManus, 2012) who reported that the materi-
als required in LIB production have the most significant contribution to
GHGs and metal depletion.
The energy requirement for the production of these batteries was
reported to be about 90 MJ per kg and 12.5 kg of CO2 equivalent emit-
ted for per kg of LIBs (Ordoñez et al., 2016). Ordoñez et al. (2016) re-
ported that about 1100 t of heavy metals and 200 t of toxic elec-
trolytes were generated from 4000 t of spent LIBs. Apart from this,
there are many occupational hazards during disposal and recycling of
LIBs vis-a-vis components. The major contributors to environmental and
health impact start from its raw material production followed by battery
production, distribution, and transportation requirements, uses, charg-
ing, maintenance, recycling and waste management (Corbus and Ham-
mel, 1995). Recycling efforts are mainly focused on cathode materials
because of their relative mass and presence of critical metals (Kim et al.,
2018, Song et al., 2019). The cradle to grave pathway via all these
stages needs minimization ensuring a shift to adoption of a circular
Y.S. Zhang, K. Schneider, H. Qiu et al.
economy approach to preventing the environment and health effects
(Gaustad, 2018).
4.2. Anodes
In general, the purity of graphite concentrate obtained by flotation is
insufficient to be reused in battery production, and all pretreatment ap-
proaches have different disadvantages. For example, the Fenton oxida-
tion pretreatment introduces Fe-ions into the flotation system, (He et al.,
2017) which is an impurity for the recovered graphite production. The
organic residues and electrolytes on the graphite particle surface can-
not be removed entirely by mechanical pretreatment such as grinding
(Yu et al., 2018, Liu et al., 2020). The roasting method may oxidize the
graphite and leads to the mass loss (Wang et al., 2018). Pyrolysis gen-
erates pyrolytic carbon residues on the graphite surface, (Zhang et al.,
2019, Zhang et al., 2018) which may influence the following flotation
efficiency.
In the case of hydrometallurgical processes, the generated wastewa-
ter and the possible environmental impact need to be considered. On the
other hand, while high purity graphite can be achieved by hydromet-
allurgical methods, it still requires further processing to obtain the
graphite product that can be reused in battery production. Remarkably,
its energy consumption during the graphite regeneration process must
be considered. Also, optimizing its electrochemical properties during
the regeneration process to approach the level as commercial graphite
is another issue that needs to be addressed. Hence, both recovery and
purification methods still have the potential to be optimized. Another
fundamental challenge facing recycling is the renewal of anode materi-
als.
4.3. Electrolyte
Limited research efforts for the recycling of the electrolyte and the
separator exist as lab-scale and commercial activities focus on metal
recovery mainly. The separator and electrolyte are usually consid-
ered unlikely to be reclaimed due to their low economic value and
the environmental benefit of electrolyte recycling is an open question
(Sommerville et al., 2021, Doose et al., 2021). Concerning existing re-
cycling methods, a process step that recovers or removes the electrolyte
is considered mandatory due to the environmental hazard potential of
the electrolyte.
Fluorine-containing compounds pose a risk to the environment
and adversely affect industrial implementation. Chemically aggressive
and toxic fluorinated compounds are present, specifically HF must be
considered in the material selection of equipment, and high safety
requirements for the environment and the employees must be met
(Rothermel et al., 2016, Nowak and Winter, 2017, Brückner et al.,
2020). Furthermore, rare attention is drawn to fluorine and residual
organic solvents as impurities in hydrometallurgical recycling of BM
which can pose a serious problem for leaching, solid-liquid-separation,
and solvent extraction at an industrial scale (Lombardo et al., 2020).
When applying pyrometallurgy, pyrolysis, or incineration techniques
to recycle LIB, neither the electrolyte nor the separator are recov-
ered but efficiently removed. Only CO2 extraction and low-temperature
volatilization can recover up to 90 % of the electrolyte (Stehmann et al.,
2018, Grützke et al., 2015). Liquid and supercritical CO2 extraction are
suitable to recover both the electrolyte salt and the organic solvents, and
supercritical CO2 extraction is an established process in the food and
pharmaceutical industry (Mukhopadhyay, 2000, Gopalan et al., 2003).
Yet, this process needs more research effort toward industrial implemen-
tation in LIB recycling, and economic competitiveness must be achieved.
Low-temperature volatilization of up to 120°C in an inert atmosphere
cannot recycle the electrolyte salt but low-boiling point organic solvents.
If subject to recycling, the recovered electrolyte needs further purifica-
tion. Pilot-scale experiments showed that critical equipment parameters
10
Carbon Capture Science & Technology 5 (2022) 100074
such as fouling and blocking of shovels need to be solved at an indus-
trial plant (Stehmann et al., 2018). Since it is not possible to remove all
the high-boiling electrolyte compounds by low-temperature volatiliza-
tion, pyrolysis of the BM may be desirable before hydrometallurgical
processing to avoid the problems stated above.
4.4. Industry scale
Recovering of valuable materials from spent LIBs has been commer-
cialised since the early 2000s. As discussed in the previous sections, the
most common recycling processes are pyrometallurgical and hydromet-
allurgical methods with a sequence of pretreatment. The industry-scale
process for recovering valuable materials from spent LIBs is either using
one method or a combined methods to optimize the recovery efficiency
(Zhang et al., 2018). The pyrometallurgical recovering process was com-
mercially developed by Umicore, and the hydrometallurgical recovering
process was developed by Retriev. Umicore developed a combined and
closed loop pyro/hydrometallurgical technology to recover LIBs with
ultra-high temperature. The developed process is integrated a safe treat-
ment without additional pretreatment, and the technology is capable for
all types of battery chemistries. Although the processing volume of Umi-
core can reach to 7000 tons per year, the waste emission was eliminated
by a gas cleaning system. A follow up hydrometallurgical process is in-
troduced to recover Cu, Ni, and Co. The hydrometallurgical process is
similar as the process described in section 3.1, including H2 SO4 leach-
ing, solvent extraction and precipitation (Zhang et al., 2018). Retriev
Technologies has also developed the recovering process which is able to
monitor different types of battery chemistry for an optimized recover-
ing process with eliminated toxic emissions. The company implemented
the most advanced processing technology and equipment which were
certified by the US Environmental Protection Agency (EPA) for battery
recovering (Zhang et al., 2018).
5. Perspectives for recycling lithium-ion batteries on reduction of
carbon emission
5.1. Cathodes
With the rise in the application of LIBs in electronics, the number of
spent LIBs also increases. This demands a recycling process to conserve
the sustainable resource and protect the environment. The reviewed lit-
erature related to recycling of spent LIBs highlights that mechanical
treatment, pyrometallurgy and hydrometallurgy are the major routes
for recycling of the spent LIBs. Hydrometallurgy dominates compared
to other recycling technique as it is an exploitable technology for the
extraction of precious metals from waste LIBs. The necessity for be-
nign recycling methods is stressed upon to alleviate the need for high
temperature and oxidative acid leaching conditions. The various green
lixiviants (organic acids) attempted to extract metals from spent LIBs
have been discussed, efficiencies as well as the various factors (selectiv-
ity, cost, etc.) that govern the use of organic acids in battery recycling.
Organic acids (effective and green leaching agents) have been demon-
strated to play a vital role in the extraction of Li, Ni, Co, and Mn from
spent LIBs. Though they are weaker than inorganic ones, still organic
acids have been examined to a greater extent for leaching of spent LIBs,
thus helping to avoid oxidizing agents, lowering complexity of manag-
ing the pregnant liquor, and thus diminishing the energy loss. The GHG
emissions to extract 90% Co using a process with organic acids stands to
be close to 500 g CO2 −1 eq per kg of Co, as compared to 4000 g CO2 −1 eq
per kg of Co by using an inorganic acid leaching process (Meshram et al.,
2020). Efforts need to be put into developing a low carbon recycling
process to recover LIBs, and therefore to create a win-win scenario of
economic and environmental benefits. A reductive thermal treatment at
a low temperature (<1000°C) under the protection of inert atmospheres
would facilitate subsequent metal extraction by hydrometallurgical pro-
cess. Various green lixiviants can be investigated to extract metals from
Y.S. Zhang, K. Schneider, H. Qiu et al.
spent LIBs. A possible research direction is targeting a substantive reduc-
tion of GHG emissions from a more developed technique comparing to
the current LIB recycling process to ensure economic and environmental
benefits.
5.2. Anodes
It is necessary to compare and combine different graphite recovery
technologies in order to integrate the treatment process. By further refin-
ing the life cycle analysis of each recovery route, the combined process
with the lowest GWP can be selected. For example, the separation of
graphite from CC foils and pretreatment prior to flotation can be com-
bined to optimize the process. In addition, the process parameters of
the individual processes still need to be further optimized, either by in-
troducing new and environmentally friendly chemicals or by increasing
the efficiency to reduce the GWP of the whole process. As the silicon
content in the anode increases, or as the anode material changes from
graphite to a non-carbon anode, it poses a significant challenge to the
existing recycling processes for recovering anode materials.
5.3. Electrolyte and separator
LIB recycling does not imply a reduction of carbon emissions itself
and is a complex process (Cerdas et al., 2018). However, recycling gen-
erates net positive impacts when the environmental effects caused by re-
cycling are lower than the avoided impacts from virgin material produc-
tion and non-material-recovery activities such as landfilling altogether
(Geyer et al., 2016). In life cycle assessment, the impact category of
global warming potential can assess the potential of carbon emission
reduction. Mohr et al. (Peters et al., 2020) calculated the cell-chemistry-
specific environmental benefits of three LIB recycling processes: py-
rometallurgical recycling, current hydrometallurgical recycling, and ad-
vanced hydrometallurgical recycling. The advanced hydrometallurgical
recycling route contained a low-temperature volatilization process and
therefore was the only one able to recover the electrolyte. The additional
recovery of electrolyte contributed to lower net impacts of the advanced
hydrometallurgical process despite the highest process inputs. Yet, the
cell chemistry, recycled material quality, and process recovery rate af-
fect the carbon emission reduction potential (Peters et al., 2020). To de-
velop economic and environmentally sound LIB recycling processes, an
integrated approach is needed to optimize economic and technical per-
formance and to reduce environmental impacts. Despite the expected
shift towards solid-state batteries, polyolefin separators in combination
with liquid electrolytes will most probably dominate the market in the
medium term.
6. Conclusion
This work covered the most developed LIB recycling technologies,
and grouped the reviewed recycling technologies into three sections,
including cathodes, anodes, electrolyte and separator. Mostly the valu-
able metals can be recovered from spent LIB cathodes are Li, Co, Ni, and
Mn as they are used in the production of cathode materials in the LIBs.
Graphite is the only component which can be recovered through a ther-
mal treatment process, hydrometallurgical process, Fenton oxidation,
forth flotation and further purification. Electrolyte can be recovered by
vacuum-thermal treatment and liquid or supercritical CO2 extraction,
but it has very rarely been recovered in industrial scale due to the high
cost of the recovering process. Therefore, most commercial LIB recycling
processes only remove the electrolyte along with the binder. The sepa-
rator is also not recovered in commercial LIB recycling process which
can be mechanically separated. The most common cathode recovering
methods are a combination of pyrometallurgical and hydrometallurgi-
cal methods, which have been developed in lab-scale and industry-scale.
There is predominant trend to substitute Co to lower production costs
for manufacturing LIB cathodes, therefore the recycling processes should
11
Carbon Capture Science & Technology 5 (2022) 100074
be developed to recover the whole cells regardless of their specific com-
positions. The developed process should also balance treatment costs
with the final effective revenue and reduce the carbon emission to help
all stakeholders to achieve the ‘net zero’ target. An emerging need is
required to develop a more compatible route to recover the most of
valuable materials with the consideration of reduced carbon emission
for tackling the environmental issues from spent LIBs.
7. Author Contributions
Conceptualization, Y.S.Z.; methodology, Y.S.Z., K.S., H.Q. and
H.L.Z.; software, Y.S.Z., K.S., H.Q. and H.L.Z.; validation, Y.S.Z., K.S.,
H.Q. and H.L.Z.; investigation, Y.S.Z., K.S., H.Q. and H.L.Z.; writing-
original draft preparation, Y.S.Z. (Abstract, Introduction, Cathode, Con-
clusion and finalising the draft), K.S. (Electrolyte and separator), H.Q.
(Anode) and H.L.Z. (Others and proof-reading); visualization, Y.S.Z.
(Table1 & 2, Figure 2, and Graphical Abstract), K.S. (Figure 4 & 5), H.Q.
(Table 3, Figure 3) and H.L.Z. (Figure. 1); funding acquisition, Y.S.Z.; All
authors have read and agreed to the published version of the manuscript.
Acknowledgement
The authors are grateful for financial supports provided by Royal
Society of Chemistry Mobility Grant (M19-2899), and Nanyang Junhao
Chemical Co. Ltd. P. R. China. Special thanks to Miss Ruike Zhang for
the graphical design.
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