Science of the Total Environment 776 (2021) 145913

Contents lists available at ScienceDirect

Science of the Total Environment

journal homepage: www.elsevier.com/locate/scitotenv

Review

Management status of waste lithium-ion batteries in China and a

complete closed-circuit recycling process
Shiqiang Sun, Chenxi Jin, Wenzhi He ⁎, Guangming Li, Haochen Zhu, Juwen Huang
State Key Laboratory of Pollution Control and Resource Reuse, Shanghai, PR China
School of Environmental Science and Engineering, Tongji University, Shanghai, PR China

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• The latest management regulations of

waste LIBs in China are presented.
• The physical recycling methods of waste
LIBs are reviewed emphatically.
• Some management suggestions and a
complete closed-circuit recycling pro-
cess of waste LIBs are put forward.

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

Article history: Lithium-ion batteries (LIBs) were used extensively in people's lives, especially with the vigorous promotion of
Received 3 December 2020 new energy vehicles, which led to the generation of a large number of waste LIBs. In consideration of the enor-
Received in revised form 25 January 2021 mous quantity, environmental risk, and resource properties, many countries have issued a series of laws and reg-
Accepted 12 February 2021
ulations to manage waste LIBs and developed a lot of recycling technologies. As the biggest producer of batteries
Available online 18 February 2021
in the world, China has also taken necessary measures to deal with this situation. This paper presents the latest
Editor: Daniel CW Tsang regulations of waste LIBs in China and reviews the recycling strategies of waste LIBs, especially physical recycling
methods. Based on the analysis of the current management status of waste LIBs in China and the recycling tech-
Keywords: nologies, some management suggestions, and a complete closed-circuit recycling process including cascade uti-
Regulations lization and resource recovery were put forward. A rough economic evaluation of the process was also conducted
Spent LIBs to demonstrate the economic feasibility of the proposed process. The purpose of this paper is to provide some
Recycling technologies valuable references for decision-making bodies in the improvement of waste lithium-ion battery management
Cascade utilization and to provide an environmentally friendly and industrial feasible recycling process for reference.
Physical methods
© 2021 Elsevier B.V. All rights reserved.
Management suggestions

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
2. Management status of waste LIBs in China . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
3. Recycling methods of waste LIBs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4

⁎ Corresponding author at: State Key Laboratory of Pollution Control and Resource Reuse, Shanghai, PR China.
E-mail address: hithwz@163.com (W. He).

https://doi.org/10.1016/j.scitotenv.2021.145913
0048-9697/© 2021 Elsevier B.V. All rights reserved.
S. Sun, C. Jin, W. He et al. Science of the Total Environment 776 (2021) 145913

3.1. Cascade utilization of waste LIBs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4

3.2. Resource recovery of waste LIBs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3.2.1. Physical methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3.2.2. Chemical methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
3.3. Complete closed-circuit recycling process of waste LIBs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
3.4. Economic evaluation. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
4. Conclusions and prospects . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
Declaration of competing interest. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
Acknowledgment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9

1. Introduction
Since they were introduced in the 1990s, lithium-ion batteries (LIBs)
have been used extensively in cell phones, laptops, cameras, and other
electronic devices owing to its high energy density, low self-discharge,
long storage life, and safe handling (Gu et al., 2017; Winslow et al.,
2018). Especially in recent years, as shown in Fig. 1 (NBS, 2020), with
the vigorous promotion and use of new energy vehicles, the growth
rate of LIBs is bound to show an increasing trend year by year (Chitre
et al., 2020; Harper et al., 2019). Generally, the average life-span of
LIBs is 1–3 years, even the life-span of LIBs in new energy vehicles is
only 5–8 years. However, due to the increasing speed of the replace-
ment of electronic products and the people's continuous pursuit of
high-end electronic products, LIBs are often discarded before reaching
their maximum life-span that results in large numbers of waste LIBs
enter the municipal waste stream. The total weight of retired LIBs in
China reached 355,000 tons in 2019 and it will reach about 800,000
tons in 2025 (GGII, 2020).
Since there are many toxic materials including heavy metals and or-
ganic electrolyte that will decompose into harmful gas, such as aldehyde
and ketone. Thus, it will lead to serious risks to the environment and
human health if discarded LIBs are treated improperly (Kang et al.,
2013; Winslow et al., 2018).
Wastage of valuable metal is another important issue of waste LIBs.
Waste LIBs are considered to be the “metal mine” with high grade be-
cause waste LIBs contain many valuable metals such as copper, alumi-
num and cobalt, etc. and it is easier to recycle these metals from waste
LIBs than that from natural ores (Xiao et al., 2020). Meanwhile, recycling
valuable metals from waste LIBs in place of natural ores can release the
heavy burden of industrial raw ore shortage, save water and energy, and
reduce waste generation (Larcher and Tarascon, 2015; Meshram et al.,
2014; Yu et al., 2014). On the whole, recycling of waste LIBs can not
only reduce environmental pollution and achieve sustainable develop-
ment but also bring significant economic benefits.
In consideration of the enormous quantity, environmental risk, and
resource properties that have mentioned above, many countries have
issued a series of laws and regulations to manage waste LIBs and
achieved remarkable results (Choi and Rhee, 2020; Salhofer et al.,
2016; Turner and Nugent, 2016). The most significant legislation is the
Batteries Directive, which was introduced by the European Union in
2006. In the Directive, the collection rates of waste LIBs had to reach
25% in 2012 and 45% in 2016 (Directive, 2006). As an advanced country
in the EU, Germany actively carried out the Directive and established
the Producer Responsibility System for the management of waste LIBs
(Corsini et al., 2017; Welfens et al., 2013). Other member states such
as Denmark, Sweden, and Netherlands are also actively involved in
the management of waste LIBs and have met the recycling targets of
the Directive (Commission, 2014; Zhang et al., 2018b). In the US, there
are no federal regulations for the management of waste LIBs, but some
states including New York, California, and Minnesota have enacted
their stringent regulations in order to reduce the release of toxic metals
from waste LIBs (Kahhat et al., 2008; Silveira and Chang, 2010). As a
country with a very developed electronics industry, Japan has formu-
lated several laws to cope with the generation of large amounts of
WEEE, including the “Law for the Promotion of Efficient Utilization of
Resource” approved in 2001 and the “Law on the Promotion of
Recycling and Reuse of Used Small Electronic Equipment” approved
on 2012 (Ogushi and Kandlikar, 2007; Xu et al., 2016). By the two
laws, government, manufacturers, retailers, consumers, processing en-
terprises, and mobile phone operators all are responsible for the
recycling of waste LIBs (Kiddee et al., 2013; Nnorom and Osibanjo,
2008; Terazono et al., 2015). As the biggest producer of batteries in
the world, China has also taken necessary measures to deal with this sit-
uation (Winslow et al., 2018; Xu et al., 2016; Zhou and Xu, 2012).
At the same time, more and more scientists have made great efforts
to achieve economically and environmentally feasible recycling
methods of waste LIBs. Most of them focused on the recovery of valu-
able metals from cathode materials through hydrometallurgy and pyro-
metallurgy, but pay less attention to economical and environmentally
friendly physical methods that are easy to operate and the recovery of
essential anode materials such as graphite (Brückner et al., 2020;
Pagnanelli et al., 2017; Ruismäki et al., 2020).
This paper presents the latest regulations of waste LIBs in China and
reviews the recycling strategies of waste LIBs, especially physical
recycling methods. Based on the analysis of the current management
situation of waste LIBs in China and the recycling technologies, some
management suggestions, and an environmentally friendly and indus-
trial feasible recycling process of waste LIBs were put forward.
2. Management status of waste LIBs in China
As is known, China is the largest consumer of electronics and pro-
duces the highest number of LIBs when compared to other developed
countries. However, the management of waste LIBs started lately in
China compared with developed countries, resulting in the failure of ef-
fective management of waste LIBs. In the past decade, China had issued
specific and pertinent legislations to direct and normalize the recycling
of waste batteries (Sun et al., 2015; Zhang et al., 2018b). The more im-
portant legislations related to waste batteries in China are summarized
as followed in Table 1. At the initial stage of the development of the elec-
tronics industry, most of the relevant regulations and laws were aimed
at lead-acid batteries. With the development of science and technology,
mobile phones and other mobile devices began to be popularized, and
then the management regulations related to lithium-ion batteries
began to be gradually introduced.
In response to the rapid updating of electronic products and the in-
creasing number of new energy vehicles, regulations on the manage-
ment of waste LIBs are also constantly being updated in China. The
Policy on Pollution Prevention Techniques of Waste Batteries was re-
leased by the Ministry of Ecological and Environment (MEE) on 26
December 2016, which mainly includes the pollution prevention and
control technologies on waste LIBs collection, transportation, storage,
utilization, and disposal. The policy regulated that the pollution preven-
tion and control of waste LIBs should follow the comprehensive preven-
tion principles of closed-loop and green recycling, resource utilization
priority, rational and safe disposal. Also, the use of information technol-
ogy was encouraged to build a whole-process supervision system of
waste batteries (MEE, 2016). On 25 December 2016, the General Office

2
S. Sun, C. Jin, W. He et al.
Fig. 1. The yield of lithium-ion batteries in China in the past decade.
of the State Council (GOSC) issued The Implementation Plan of the
Extended Producer Responsibility System, which determined to imple-
ment the extended producer responsibility system for four categories of
products, including electrical appliances and electronics, automobiles,
lead-acid batteries, and packaging materials. The Implementation Plan
also set specific recycling targets to achieve a recovery rate of 40% for
major waste products (including waste LIBs) by 2020 and 50% by
2025. The government and social capital cooperation mode and third-
party services mode were encouraged to attract social capital to partic-
ipate in the recycling of waste LIBs (GOSC, 2016).
Meanwhile, with the rapid development of new energy vehicles, rel-
evant departments of the Chinese government have also issued some
regulations on power lithium-ion battery recycling. In February 2018,
seven ministries and commissions including the Ministry of Industry
and Information Technology (MIIT) jointly formulated The Interim
Measures for The Management of Power Battery Recovery and
Utilization of New Energy Vehicles, stressing that automobile
manufacturers should shoulder the primary responsibility for power
battery recovery and carry out the full life cycle management of power
batteries. Besides, it is encouraged to carry out the reuse of power
batteries in accordance with the principle of cascade utilize firstly and
recycle lately, so as to realize the maximum benefit of comprehensive
Table 1
Legislations related to waste batteries in China.
Laws and regulations
Law of the People's Republic of China on the Prevention and Control of
Solid Waste Pollution
Technical Policy for the Prevention and Control of Hazardous Waste
Pollution
Policy on Pollution Prevention Techniques from Waste Batteries
National Hazardous Waste List
Administrative Measures on the Collection and Using of Waste
Electrical and Electronic Product Treat Fund
Directory of Waste Electrical and Electronic Equipment Treatment
(2014)
Technology Policy for the Recycling of Power Battery (2015 edition)
Policy on Pollution Prevention Techniques of Waste Batteries
The Implementation Plan of the Extended Producer Responsibility
System
The Interim Measures for The Management of Power Battery Recovery
and Utilization of New Energy Vehicles
The Interim Provisions on The Traceability Management of Power
Battery Recovery and Utilization of New Energy Vehicles
The Notice on the Pilot Work of Power Battery Recycling of New
Energy Vehicles
The Law of the People's Republic of China on the Prevention and
Control of Solid Waste Pollution (2020 edition)
The Notice on Matters Related to the Total Ban on Solid Waste Import 2020 The import of solid waste in any way is prohibited
Science of the Total Environment 776 (2021) 145913
utilization of resources (MIIT, 2018a). Subsequently, the Ministry of
Industry and Information Technology issued The Interim Provisions
on The Traceability Management of Power Battery Recovery and
Utilization of New Energy Vehicles in July 2018, which required that
the comprehensive management platform for national monitoring
and power battery recovery and utilization traceability of new energy
vehicles must be established to carry out traceability management for
the whole process of power battery production, sales, use, scrap,
recovery, and utilization. It also stipulated that the battery production
and cascade utilization enterprises should apply for the manufacturer's
code and record the code rules, so as to encode and mark the power
battery or cascade utilization battery products produced by the
enterprise (MIIT, 2018b).
In July 2018, seven ministries and commissions including the Minis-
try of Industry and Information Technology issued The Notice on the
Pilot Work of Power Battery Recycling of New Energy Vehicles, which
confirmed that Beijing, Shanghai, Jiangsu, etc. as pilot regions and
China Iron Tower Co., Ltd. as a pilot enterprise to carry out the pilot
work of power battery recycling (MIIT, 2018c). This marked that
China's power battery recovery has entered the stage of large-scale im-
plementation. In this case, major key cities have supplemented or intro-
duced relevant local regulations according to the development status of
local power batteries to promote the standardization of power battery
recycling. In 2018, Shenzhen took the lead in issuing a plan to establish
a battery regulatory recovery system and proposed to improve the de-
posit mechanism for power battery recovery. In January 2019, it issued
The Financial Support Policy for Promotion and Application of New
Energy Vehicles in Shenzhen in 2018, in which the power battery
recycling subsidy appeared in the local subsidy policy for the first
time, and Shenzhen became the first city in China to set up the power
battery recycling subsidy (Shenzhen, 2019).In addition, 109 related
enterprises in 29 provinces had been included in the waste electrical
and electronic products disposal fund subsidy list by the end of 2018
(MEE, 2019).
According to GGII data, 129,000 tons of waste LIBs were recovered
nationwide in 2019, accounting for 36.3% of the total quantity of retired
lithium-ion batteries. Among them, 33,000 tons of retired power batte-
ries were recovered, accounting for 24.8% of the total quantity of retired
power lithium-ion batteries in the market. Therefore, the recovery of
waste lithium-ion batteries is still lower than expected (GGII, 2020).
Therefore, The Law of the People's Republic of China on The Prevention
Year Major regulations on battery recycling
1995 Waste batteries are dangerous solid wastes and need to be recycled separately
2001 Phase-out batteries containing mercury and cadmium
Battery industries should take responsibility for collecting waste batteries and for proper
2003
labeling
2008 Lead-acid batteries are dangerous solid wastes that need to be collected and treated separately
2012 Manufacturers or importers are responsible for the fund collection
2015 Waste LIBs were officially added to the scope of the Fund
2016 Provisions on the recycling and utilization of waste EV batteries
2016 The pollution prevention and control technologies of waste LIBs
2016 Implement the extended producer responsibility system for batteries
Automobile manufacturers should shoulder the primary responsibility for power battery
2018
recovery
The comprehensive management platform for national monitoring and power battery recovery
2018
and utilization traceability of new energy vehicles must be established
Confirmed some pilot regions and pilot enterprises to carry out the pilot work of power battery
2018
recycling
The establishment of a credit record system for the prevention and control of solid waste
2020
(including waste LIBs) pollution
3
S. Sun, C. Jin, W. He et al.
and Control of Solid Waste Pollution was amended and adopted at the
17th Session of the Standing Committee of the 13th National People's
Congress (NPCSC) on 29 April 2020 and came into force on 1 September
2020. The main added contents of this amendment include the estab-
lishment of a credit record system for the prevention and control of
solid waste (including waste LIBs) pollution and the illegal information
will be included in the national credit information sharing platform and
publicized. It made clear that China will gradually realize zero import of
solid waste. Also, strict legal liability has been laid down for the unau-
thorized dumping, stacking, and discarding of industrial solid waste (in-
cluding waste LIBs) and the provision of continuous penalties on a daily
basis has been added (NPCSC, 2020). In order to implement the revised
contents of the import management of solid waste, the Ministry of
Ecology and Environment and other three departments issued The
Notice on Matters Related to the Total Ban on Solid Waste Import on
25 November 2020 (hereinafter referred to as the Notice), which will
take effect from 1 January 2021. The Notice made it clear that the import
of solid waste in any way is prohibited. And it is forbidden to dump, pile
up, and dispose of solid wastes outside the territory of China (MEE,
2020). The Notice is an important institutional reform aimed at promot-
ing green development, protecting the ecological environment and the
health of the people. It is beneficial to reduce the amount of domestic
solid waste stockpiles (including waste LIBs), standardize the domestic
solid waste recycling market, and bring China's waste recycling industry
into a new direction.
In order to promote the development of the recycling industry of
waste LIBs, in terms of science and technology investment, the key pro-
ject of “solid waste recycling” of the National Key Research and Devel-
opment Plan deployed research and development tasks related to the
cascade utilization and precise dismantling of retired power batteries
in 2018 (MST, 2018), followed by research and development tasks re-
lated to the recovery and utilization technology of retired lithium iron
phosphate batteries and retired ternary lithium batteries in 2019
(MST, 2019).
As can be seen from the above, China has made great efforts and
achieved much progress both in the policy management and science
and technology investment of waste LIBs recovery in recent years. It is
not difficult to foresee that the blue ocean of waste lithium-ion battery
recycling industry is slowly forming, with a very broad prospect in the
future, and China will also become one of the largest markets for
lithium-ion battery recycling.
3. Recycling methods of waste LIBs
As is shown in Fig. 2 (Li et al., 2016b), LIBs are mainly composed of
metallic shells, cathode, anode, organic electrolyte, and separator. The
Fig. 2. The structure of the lithium-ion battery.
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Science of the Total Environment 776 (2021) 145913
cathode is mainly composed of organic binder (polyvinylidene fluoride
(PVDF)), aluminum foil, and cathode materials such as LiCoO2, LiMn2O4,
LiPePO4, etc. while the anode is mainly composed of copper foil, organic
binder, and anode materials (graphite) (Chagnes and Pospiech, 2013).
The electrolyte is mainly composed of some organic solvents and lith-
ium salts such as LiPF6, LiBF4, etc. (Zeng et al., 2014). As a result, the
composition of LIBs is relatively complex and contains valuable metals,
which makes them called a high-grade “metal mine” (He et al., 2020).
According to the application field, LIBs can be divided into power
lithium-ion batteries, consumption lithium-ion batteries, and energy
storage lithium-ion batteries. Generally, power lithium-ion batteries
are considered to have reached their end of life in EVs when the residual
capacity amounted to less than 80% of their original capacity, which can
be used in other devices that require less power (Williams and Lipman,
2010). Therefore, the recycling process of waste LIBs can be divided into
cascade utilization and resource recycling.
3.1. Cascade utilization of waste LIBs
Cascade utilization is mainly aimed at the power lithium-ion batte-
ries with 60–80% residual capacity after the retirement from electric ve-
hicles. After re-testing and analysis, they can be used in other areas
where the operating conditions are relatively simple and the battery
performance requirements are relatively low such as renewable energy
installations in buildings, fast EV charge stations energy storage applica-
tions, portable power generators, E-Bike application, etc. (Casals et al.,
2019; Cusenza et al., 2019; Liu et al., 2020). The cascade utilization of
waste LIBs has a good prospect in both economic and environmental as-
pects. Although it is still in the stage of demonstration application at
present, there have been successful cases in China.
In 2017, BAIC New Energy launched the “Optimus Prime Plan”,
which plans to invest 10 billion yuan to build 3000 optical storage elec-
trical changing stations nationwide by 2022, with a total investment of
500,000 battery changing vehicles and more than 5GWh of cascade uti-
lization of waste LIBs (SOHU, 2018). In January 2018, Chongqing
Changan, BYD, Yinlong New Energy, and other 16 vehicle and battery
companies signed a strategic partnership agreement on the recycling
and utilization of power lithium-ion batteries of new energy vehicles
with China Tower Company, which is a major power battery recycler
in China. In early 2019, WM Motor and Clou Electronics signed a strate-
gic cooperation agreement on power lithium-ion battery recycling and
utilization and agreed to promote the application of echelon battery en-
ergy storage systems nationwide (SMM, 2019).
In general, some enterprises have made some breakthroughs in bat-
tery life evaluation, system integration, and battery monomer repair.
However, there are still some problems such as low efficiency, imma-
ture technologies for evaluation on battery residual life, and consistency
(MIIT, 2019).
3.2. Resource recovery of waste LIBs
Retired batteries that are no longer useful need to be disassembled
and recycled to extract valuable materials to be used as raw materials
for the re-manufacture of lithium-ion batteries. Resource recovery
methods of waste LIBs are mainly divided into physical methods and
chemical methods. A great deal of research on resource recovery of
waste LIBs focused on chemical methods, among which pyrometallurgy
and hydrometallurgy account for 16.79% and 57.25% respectively in all
recovery technologies (Zeng et al., 2014). This paper mainly focuses
on the review of the physical methods on resource recovery of waste
LIBs, and only briefly introduces the chemical methods.
3.2.1. Physical methods
Physical methods are usually used as a pre-treatment process to sep-
arate different components of waste LIBs according to different physical
properties of materials, mainly including mechanical crushing, particle
S. Sun, C. Jin, W. He et al.
size separation, gravity separation, magnetic separation, flotation, and
so on. The advantages of high processing capacity, simple operation,
and low cost make the physical method have a good industrial applica-
tion prospect in waste LIBs recovery (Al-Thyabat et al., 2013).
3.2.1.1. Particle size separation. In mineral processing engineering, parti-
cle size separation refers to the method of mineral separation according
to the content distribution of different mineral components in different
particle size fractions after crushing and screening (Chatterjee, 1998).
Particle size separation also plays an important role in the recovery of
waste LIBs, mainly because the active materials of cathode and anode
are black powders, also referred to as the “black mass”, such as LiCoO2
powders and graphite powders (Kim et al., 2004). In particle size sepa-
ration, the most critical process is usually mechanical crushing, which
aims at achieving selective liberation of electrode active materials. The
current collectors such as Cu and Al can also enter this black mass, and
their concentration depends on the conditions under which they are
crushed (Diekmann et al., 2016).
Wang et al. (2016c) studied the particle size separation process of
spent LIBs using a commercial granulator, and the results showed that
the active materials and graphite were mainly concentrated in the ultra-
fine (<0.5 mm) fraction, copper pieces were visibly detected in the mid
(1–6 mm) fraction while casings and plastic separators mainly entered
the coarse (>6 mm) fraction. Widijatmoko et al. (2020) studied the se-
lective liberation of positive electrode active material during milling,
and they found that in the size fraction <850 um, the recovery of
LiCoO2 is 43.7% with a minimum recovery of Al and Cu (8.8% and
10.3%) from the waste LIBs. Zhang et al. studied the influence of dry
and wet crushing methods on the overall crushing of waste LIBs, and
the research results showed that both of them can achieve the selective
crushing of waste LIBs, that is, the electrode materials are mainly con-
centrated in the fine fraction (<0.25 mm), while aluminum, copper,
plastic and other materials mainly entered the coarse fraction
(>0.25 mm). They also found that dry crushing performed significantly
better than wet crushing. Because, in wet crushing, the electrode active
materials passed through the screen with water before it has liberated
from the foil, resulting in a high content of copper and aluminum in
the fine fraction (Zhang et al., 2013).
3.2.1.2. Magnetic separation. In the recovery of waste LIBs, magnetic sep-
aration is mainly used to remove the steel casings such as Fe through
magnetic force after shredding. Therefore, there are few researches on
magnetic separation. Shin et al. (2005) and Yamaji et al. (2011) had
used a magnetic separator to remove pieces of steel casing, and almost
100% of iron pieces were separated from nonmagnetic pieces which
contain cathode active materials. Li et al. (2016a) presented a new envi-
ronmentally friendly process on recycling of waste LIBs that combined
oxygen-free roasting and wet magnetic separation. In this process,
graphite and LiCoO2 reacted under oxygen-free roasting and generated
the residue with a mixture of Co, Li2CO3, and graphite. Then, the residue
was further separated by wet magnetic separation based on the mag-
netic property differences. After wet magnetic separation, the recovery
rate of Co, Li, and graphite is 95.72%, 98.93%, and 91.05%, respectively.
3.2.1.3. Gravity separation. Gravity separation refers to a separation
method according to the sufficient density difference in different com-
ponents of waste LIBs with the same particle size after sieving, which
is mainly used to separate out the low-density parts such as the separa-
tor, plastics, and Al foil (Zhang et al., 2018c). As well, gravity separation
can be used to realize the separation of positive and negative electrode
materials due to the great density difference between them (Zhu et al.,
2017). The gravity separation process can be achieved through shaker
tables, vibrating screens, a fluid of intermediate density, or air separa-
tion (Diekmann et al., 2016).
Bertuol et al. (2015) studied the application of spouted bed elutria-
tion in the recovery of waste LIBs, the results showed that spouted
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Science of the Total Environment 776 (2021) 145913
bed elutriation is a simple and economical way to separate the different
materials of waste LIBs including electrode active materials, polymers,
Cu and Al. Diekmann et al. (2016) applied air-classification to separate
the components with higher densities and light products. 74.3 wt% Al,
13.8 wt% Fe, 5.0 wt% Cu, and 4.0 wt% plastics were recovered into
heavy parts, the current collector foils, separator, and plastic foils got
into light parts. Bi et al. (2019) achieved effective separation of the cop-
per and aluminum fragments without classification of particle sizes by
using pneumatic separation, which led to the mass fraction 97% of the
copper fragments and 96% of aluminum fragments.
In recent years, some scholars have carried out relevant studies on
the gravity separation of positive and negative electrode materials.
Zhu et al. studied the gravity separation of graphite and LiCoO2 using
an enhanced centrifugal separator, and the graphite content reached
to 65% in the low-density parts. The separation results also showed
that the separation efficiency could significantly be influenced by cen-
trifugal force and particle size (Zhu et al., 2017). Zhang et al. studied
the separation of positive and negative electrode materials using Falcon
centrifugal separator, the structure and schematic diagram of Falcon
centrifuge is shown in Fig. 3. Their results showed that after Falcon cen-
trifugal separation, the grade of LiCoO2 is 84.87%, and the recovery of
LiCoO2 is 83.14% (Zhang et al., 2018d).
It is worth noting that although it is theoretically feasible to separate
positive and negative electrode materials by gravity separation, the sep-
aration efficiency gradually decreases with the decrease of particle size
(Zhang et al., 2018d; Zhu et al., 2017). Due to the particle size of the sep-
arated electrode materials is very small, gravity separation cannot
achieve the ideal separation effect.
3.2.1.4. Flotation. Flotation is a mineral processing method that utilizes
the different physical and chemical properties of the mineral surface
to separate different minerals, especially for fine minerals. As shown
in Fig. 4 (Sommerville et al., 2020), by adding the flotation agents, the
hydrophobic mineral particles can be attached to the bubbles and float
to the surface of the pulp to form a mineralized foam layer, while the hy-
drophilic mineral particles still remain in the slurry, so as to achieve the
separation purpose of different minerals (Wang et al., 2017). Therefore,
it is theoretically feasible to realize the separation of positive and nega-
tive electrode materials by flotation technology as a result of their obvi-
ous hydrophilic and hydrophobic differences caused by different lattice
structures (Zhang et al., 2014). However, the electrode particles after
the mechanical crushing are wrapped by organic binder such as PVDF
and residual electrolyte, which greatly reduces the hydrophilic and hy-
drophobic difference between the cathode and anode materials,
resulting in the failure of effective separation of electrode particles in
the flotation process (Kim et al., 2004). Therefore, it is essential to re-
move PVDF and residual electrolyte from the electrode material surface
in order to improve the flotation results. In this regard, several effective
Fig. 3. The structure and schematic diagram of Falcon centrifuge.
S. Sun, C. Jin, W. He et al.
Fig. 4. The schematic of flotation.
methods have been developed, including grinding modification, Fenton
modification, roasting modification, pyrolysis modification and so on.
The separability of electrode materials from waste LIBs was studied
using the flotation technique by Zhan et al. They found that over 90%
of anode materials and only 10–30% of cathode materials were floatable
after rinsing off electrolytes due to the coverage of hydrophobic binders
and carbon additives on surfaces. Subsequently, cathode materials with
a grade of 88.2% and a total recovery of 74.3% were obtained after a finer
grinding, which exposed fresh hydrophilic and hydrophobic surfaces of
the electrode material and improved the flotation result (Zhan et al.,
2018). Yu et al. studied grinding flotation for the separation of LiCoO2
and graphite, their results showed that the concentrate LiCoO2 with a
grade of 97.19% and a recovery rate of 49.32%, the tailings graphite
with a grade of 82.57% and a recovery rate of 73.56% were obtained
with the optimum condition of 5 min grinding (Yu et al., 2018). It can
be seen that grinding flotation could improve the grade of cathode ma-
terials to a certain extent, but the recovery is low. Moreover, it only
destroyed about 25% of the organic binder PVDF, which has a certain in-
fluence on the subsequent metallurgical process (Yu et al., 2020).
He et al. developed a Fenton reagent-assisted flotation process to ef-
fectively recover LiCoO2 and graphite of waste LIBs. They obtained the op-
timal conditions for removing the most of organic binder PVDF, i.e. the
Fe2+/H2O2 ratio is 1:120, and the liquid-solid ratio is 75:1. Their results
showed that under the optimal conditions, the enrichment ratios of Co,
Mn, Cu, and Al were 1.41, 1.27, 1.35, and 1.25, and their recovery rates
were 98.99%, 89.45%, 94.95%, and 87.83% respectively (He et al., 2017).
Obviously, Fenton flotation can be used as an effective method to remove
PVDF from the surface of electrode materials and to recover electrode ma-
terials from waste LIBs. However, Fenton flotation introduced Fe2+ into
the reaction process and covered the surface of electrode materials,
which complicated subsequent metallurgical processes (Yu et al., 2017).
Roasting flotation was developed to remove PVDF and electrolyte
and recover valuable metals and graphite of waste LIBs by Wang et al.
The results showed that after roasting treatment at the temperature of
450 °C for 15 min, most of the organic binder PVDF was removed, and
the enrichment ratios of Co, Mn, Cu, and Al were 1.35, 1.29, 1.25 and
1.19, the recovery rates were 97.66%, 93.66%, 90.14%, and 86.29%, re-
spectively (Wang et al., 2018). Although roasting flotation could
6
Science of the Total Environment 776 (2021) 145913
improve the flotation effect, its use is limited because toxic gases such
as HF are produced during roasting (Zhang et al., 2018a).
Zhang et al. studied the pyrolysis flotation process to remove the or-
ganic binder and residual electrolyte so as to enhance the flotation be-
havior of electrode materials. Their results suggested that at a
pyrolysis temperature of 550 °C, the cathode with a grade of 94.72%
and a recovery of 83.75% was obtained. However, there was some resid-
ual pyrolytic carbon remaining on the surface of electrode materials, so
that wet-ball grinding was used to further improve cathode recovery
from 83.75 to 91.35% (Zhang et al., 2020). After pyrolysis and two-
stage flotation processes, the grade of LiCoO2 increased from 67.25% to
98.00% (Zhang et al., 2019). They also proposed pyrolysis-ultrasonic-
assisted flotation technology to recover graphite and LiCoO2 of waste
LIBs, and they found that ultrasonic cleaning can effectively remove
the pyrolysis products from the surface of the electrode materials and
enhance the flotation effect. With the assist of ultrasonic cleaning, the
grade of LiCoO2 was improved from 67.25% to 93.89%, and the recovery
rate was increased from 74.62% to 96.88% (Zhang et al., 2018a). Com-
pared with Roasting flotation, pyrolysis flotation can not only remove
the organic binder PVDF and effectively recover electrode materials,
but also recover pyrolysis products such as pyrolysis gas and oil for fur-
ther treatment (Zhang et al., 2018a).
3.2.2. Chemical methods
As was mentioned above, there is a great deal of research on re-
source recovery of waste LIBs focused on chemical methods, which
mainly include hydrometallurgy, pyrometallurgy, and mechanochemi-
cal technologies. Metallurgical technology occupies a dominant position
in the field of waste lithium-ion battery treatment, mainly because it
can realize the separation and purification of various metal elements
and facilitate the subsequent recycling of valuable metals.
Hydrometallurgy is to dissolve the pre-treated waste lithium-ion
batteries in acid and alkali solution (Chen et al., 2011; Chen et al.,
2018), and then to extract valuable metals through precipitation (Zhu
et al., 2012), electrochemical deposition (Celante and Freitas, 2009), sol-
vent extraction (Wang et al., 2016a) and other technologies. Common
leaching agents include inorganic acids such as sulfuric acid and hydro-
chloric acid, organic acids such as oxalic acid and citric acid, and alkali
such as ammonium sulfate (Xiao et al., 2020). Some details of the
leaching process of waste LIBs are summarized in Table 2. It is obvious
that hydrometallurgy is a necessary link in the recycling process of
waste LIBs since it can obtain relatively pure metal compounds. How-
ever, the technology is mainly aimed at the recovery of cathode mate-
rials with high economic value in consideration of the cost of leaching
reagents.
Pyrometallurgy is a method of recovering valuable metals from
waste LIBs under high-temperature conditions. Because of its simple op-
eration, it also plays an important role in the recycling process of waste
lithium-ion batteries (Nie et al., 2015). As a pyrometallurgical method,
carbothermal reduction technology has attracted broad attention,
which can convert LiCoO2 into CoO and Li2CO3, and then separate
Li2CO3 from CoO by means of water leaching (Tang et al., 2019; Xiao
et al., 2017). Recently, the mechanochemical method has been widely
used for metal recovery from waste LIBs, which utilizes co-grinding
LiCoO2 with polyvinyl chloride (PVC) or ethylenediaminetetraacetic
acid (EDTA) to convert LiCoO2 into Li and Co chlorides. Then the Co
and Li were further extracted by water leaching (Saeki et al., 2004;
Wang et al., 2016b).
As an alternative to chemical methods, bio-metallurgy has attracted
extensive attention in the field of metal recovery due to its advantages
of low cost and low pollution (Xin et al., 2009). It mainly uses special mi-
crobial bacterial metabolic processes to achieve the selective leaching of
valuable metals. However, its leaching process relies too much on bacte-
rial metabolism, resulting in unstable recovery efficiency of valuable
metals (Niu et al., 2014). Table 3 summarizes the advantages and disad-
vantages of different recycling methods of waste LIBs.
S. Sun, C. Jin, W. He et al. Science of the Total Environment 776 (2021) 145913

Table 2
Summary of the leaching process of waste LIBs.

Leaching agent Leaching condition Reduction agent Leaching efficiency Reference

Inorganic Acid Leaching

4 M HCl 60 min + 353 K + 20 g/L N/A 99% Li,99% Co (Wang et al., 2009)
2% vol H3PO4 60 min + 363 K + 8 g/L H2O2 88% Li,99% Co (Pinna et al., 2017)
1 M HNO3 60 min + 353 K + 20 g/L H2O2 ~100% Li, ~100% Co (Li et al., 2011)
4 M H2SO4 120 min + 358 K + 1/10 g/L H2O2 96% Li,95% Co (Chen et al., 2011)
1 M H2SO4 240 min + 368 K + 20 g/L NaHSO3 96.7% Li,91.6% Co,96.4% Ni,87.9% Mn (Meshram et al., 2015)

Organic Acid Leaching

1.5 M malic acid 40 min + 363 K + 20 g/L H2O2 ~100% Li, 90% Co (Li et al., 2013)
1 M oxalic acid 150 min + 368 K + 15 g/L N/A 98% Li, 97% Co (Zeng et al., 2015b)
1.25 M citric acid 30 min + 363 K + 20 g/L H2O2 ~100% Li,>90% Co (Li et al., 2010)
1.5 M succinic acid 40 min + 343 K + 15 g/L H2O2 96% Li,100% Co (Li et al., 2015)
3.0 M trichloroacetic acid 30 min + 337 K + 50 g/L H2O2 99.7% Li,91.8% Co,93.0% Ni,89.8% Mn (Zhang et al., 2015)

Alkali Leaching
4 M NH3 + 1.5 M (NH4)2SO4 300 min + 353 K + 10 g/L Na2SO3 95.3% Li,80.7% Co,89.8% Ni,4.3% Mn (Zheng et al., 2017)
3 M (NH4)2SO4 120 min + 453 K + 83 g/L (NH4)2SO3 98% Li,81% Co,98% Ni,92% Mn, (Chen et al., 2018)

N/A: Not applicable.

3.3. Complete closed-circuit recycling process of waste LIBs
To sum up, although the physical method is simple to operate, it can-
not obtain pure electrode materials. In contrast, hydrometallurgy can
purify a variety of metal elements, but considering the cost of leaching
reagents, it is not possible to achieve the recovery of the whole compo-
nent of waste LIBs through hydrometallurgy alone. The best solution is
to combine the two methods, just like a mature gold ore dressing pro-
cess (Wang et al., 2011), that is, to make the physical method as the
pre-treatment process for subsequent hydrometallurgy processes. As a
result, a complete recycling flow chart of waste LIBs is put forward,
which is shown in Fig. 5. What needs to be emphasized is that the re-
tired lithium-ion batteries (mainly the power lithium-ion batteries)
should be firstly cascade utilized to make full use of the battery capacity,
then enter the resource recovery stage.
In the resource recovery stage, the waste LIBs should be discharged
first via connection to a resistor (Sonoc et al., 2015) or immersion in a
salt solution (He et al., 2015; Shaw-Stewart et al., 2019) to ensure the
safety of the subsequent recovery process. After shredding of waste
LIBs, the organic membrane and plastics can be separated by air classi-
fication, and then, the metallic shell is recovered by magnetic separa-
tion. The remaining components are pyrolyzed to remove the organic
binder PVDF and recover the electrolyte generated during the pyrolysis
process. Toxic gases generated in the pyrolysis process, such as HF, can
be further treated to reduce the harm to the environment. The process
after pyrolysis is particle size separation, including crushing and screen-
ing. The fraction with particle size greater than 0.2 mm is mainly copper
and aluminum, which can be separated and recovered by pneumatic
separation. While graphite and cathode active materials in the fraction
with particle size less than 0.2 mm can be separated by flotation. The
cathode materials after flotation separation are purified by hydrometal-
lurgy to obtain precious metals such as Co, Li, Ni, Mn, etc. Finally, the
recycled products can be used as raw materials to reproduce new
lithium-ion batteries, thus forming a closed-circuit process.
Since the physical methods and corresponding equipment involved
in this process have very mature applications in the mineral processing
industries such as metal ore and coal mines, especially the sorting pro-
cess of some precious metals such as gold, silver and platinum, which is
a good combination of mineral processing technology and hydrometal-
lurgy technology, the proposed process is industrially feasible. This pro-
cess can be applied to several lithium-ion batteries with graphite as
anode material commonly found in the current market, including ter-
nary lithium batteries, lithium iron phosphate batteries and lithium co-
balt acid batteries, etc., because graphite has natural hydrophobicity.
3.4. Economic evaluation
In this paper, we take the recycling of used LiCoO2 batteries as an ex-
ample and roughly estimate the profit that can be obtained through the
proposed process. The yield of each component of LiCoO2 batteries and
the income that can be obtained from the recycled products are shown
in Table 4.
According to a study by Gasper et al. (2013), the cost of mechanical
separation process consisting of shredding, baking, magnetic separa-
tion, and specific gravity separation was $529 per ton. Considering
inflation and the flotation cost in the proposed process, the cost of

Table 3
Comparison of different recycling methods of waste LIBs.

Recycling methods Advantages Disadvantages

Particle size Positive and negative materials can be separated from other Over-crushed Cu and Al can also enter the ultrafine fraction, so the crushing conditions
separation parts should be well controlled
Magnetic
The steel casings such as Fe can be separated The removed steel casings may contain some active materials
separation
The low-density parts such as the separator and plastics can be
Gravity separation Poor separation of materials with small density differences
separated
Separation of positive and negative materials can be achieved; Only as a pre-treatment method, the obtained active materials need to be further
Flotation
Low cost purified
Great capacity and simple operation;
Low recovery rate; Unable to recycle all metals; High energy consumption and
Pyrometallurgy LIBs of different varieties could be recycled
environmental pollution
together without pre-sorting
Low energy requirement and high purity; High chemical reagents consumption; Complicated processing steps; Need further
Hydrometallurgy
Low pollution; High recovery efficiency wastewater treatment
Bio-metallurgy Low cost and high safety; Environmental friendly Long reaction time and low pulp density; Efficiency instability

7
S. Sun, C. Jin, W. He et al. Science of the Total Environment 776 (2021) 145913

Fig. 5. A complete closed-circuit recycling process of waste LIBs.

mechanical pre-treatment is converted to RMB 6000 yuan/ton. Refer to 4. Conclusions and prospects
the research of Tran et al. (2020), the direct operating costs (chemicals,
labor operation, utilities, energy) to recycle spent alkaline batteries was The extensive application of lithium-ion batteries in people's life led
calculated to be $CAD 726 per ton. Therefore, the cost of chemical puri- to the generation of a large number of waste LIBs. It is crucially impor-
fication of the proposed process is converted to RMB 4000 yuan/ton. In tant to manage and recycle waste LIBs based on their resource attribute
summary, without considering the initial investment and the cost of ac- and environmental harmfulness. In order to manage and recycle waste
quiring waste LiCoO2 batteries, the profit that can be obtained from this LIBs, developed countries have made great efforts and made some
process is about 21,090 yuan/ton, which shows that the process pro- achievements, providing some valuable experiences for other countries.
posed in this paper is economically competitive and feasible. After so many years of continuous development, China has also made
great progress in waste LIB management. However, there are still
some problems in the details of waste lithium-ion battery management,
Table 4 which led to the unsatisfactory recovery effect of waste LIBs. To this end,
The economic evaluation of materials. some management suggestions are put forward:
Component Yield/% (Zeng Price (yuan/ton) Converted pricea Product revenue
et al., 2015a) (TE, 2021) (yuan/ton) (yuan/ton) (1) For waste consumption lithium-ion batteries, the government
b should also improve infrastructure construction, designate col-
Co 12 227500 204,700 24,500
Cu 9 51,500 46,300 4150 lection sites and install convenient collection facilities;
Al 3 12,800 11,500 350 (2) The government should strengthen education on waste lithium-
Fe 18 4100 3700 650 ion battery recycling among citizens, especially school students.
Li 1.5 54,000 48,500 720 The education should focus on the necessity to recycle waste
Graphite 20 4000 3600 720
Total 63.5 – – 31,090
LIBs and how to collect them;
a
(3) Some incentives can be set up to encourage citizens to actively
Converted price: Considering that the purity of the recycled product may not meet
participate in the recycling of waste LIBs, such as the implemen-
international standards, the price of the material is rounded by a coefficient of 0.9.
b
Due to the fluctuation of Co price, the average price of USD 35,000/ton in recent years tation of the points system on waste lithium-ion battery collec-
is taken and all converted into RMB to take the whole number. tion. People can earn points by collecting waste LIBs, and these

8
S. Sun, C. Jin, W. He et al.
points can be exchanged for some daily necessities, etc.;
(4) Green material selection and structure design for lithium-ion
battery production should be standardized to solve the problems
of low metal recovery and compatibility of multiple lithium-ion
battery recovery.
Globally, many countries including the United States, UK, Canada,
Belgium, and China have mainly focused on the recovery of waste LIBs
by pyrometallurgy, hydrometallurgy or a combination of both, while ig-
noring the mechanical pre-treatment process of positive and negative
electrode materials (Meshram et al., 2014). Physical methods as pre-
treatment processes are efficient to minimize the energy consumption
for the subsequent chemical processes. Therefore, the future develop-
ment trend of lithium-ion battery recycling process is definitely the
combination of mechanical pre-treatment and chemical purification.
The complete closed-circuit recycling process of waste LIBs proposed
in this paper combines physical methods and chemical methods,
which are very economical, environmentally friendly, and has a good in-
dustrial application prospect. In the future, researchers should pay more
attention to the cascade utilization of retired power lithium-ion batte-
ries owing to its great development potential, especially safety detec-
tion and residual life assessment. At the same time, they should also
focus their efforts on the progressive scaling up of laboratory techniques
for practical application in industry. Finally, they need to continue to re-
search and develop green, efficient, and economical whole-component
recycling technologies for waste LIBs.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgment
The authors disclosed receipt of the following financial support for
the research, authorship, and/or publication of this article: The authors
greatly appreciate the support and funding of Shanghai Institute of
Pollution Control and Ecological Security (HJGFXK-2017-002) and the
support of the State Key Laboratory of Pollution Control and Resource
Reuse (SKL) devices.
References
Al-Thyabat, S., Nakamura, T., Shibata, E., Iizuka, A., 2013. Adaptation of minerals process-
ing operations for lithium-ion (LiBs) and nickel metal hydride (NiMH) batteries
recycling: critical review. Miner. Eng. 45, 4–17.
Bertuol, D.A., Toniasso, C., Jiménez, B.M., Meili, L., Dotto, G.L., Tanabe, E.H., et al., 2015. Ap-
plication of spouted bed elutriation in the recycling of lithium ion batteries. J. Power
Sources 275, 627–632.
Bi, H., Zhu, H., Zu, L., He, S., Gao, Y., Gao, S., 2019. Pneumatic separation and recycling of
anode and cathode materials from spent lithium iron phosphate batteries. Waste
Manag. Res. 37, 374–385.
Brückner, L., Frank, J., Elwert, T., 2020. Industrial recycling of lithium-ion batteries—a crit-
ical review of metallurgical process routes. Metals 10, 1107.
Casals, L.C., Amante Garcia, B., Canal, C., 2019. Second life batteries lifespan: rest of useful
life and environmental analysis. J. Environ. Manag. 232, 354–363.
Celante, V.G., Freitas, M.B.J.G., 2009. Electrodeposition of copper from spent Li-ion batte-
ries by electrochemical quartz crystal microbalance and impedance spectroscopy
techniques. J. Appl. Electrochem. 40, 233–239.
Chagnes, A., Pospiech, B., 2013. A brief review on hydrometallurgical technologies for
recycling spent lithium-ion batteries. J. Chem. Technol. Biotechnol. 88, 1191–1199.
Chatterjee, A., 1998. Role of particle size in mineral processing at Tata Steel. Interational
Journal of Mineral Processing 53, 1–14.
Chen, L., Tang, X., Zhang, Y., Li, L., Zeng, Z., Zhang, Y., 2011. Process for the recovery of co-
balt oxalate from spent lithium-ion batteries. Hydrometallurgy 108, 80–86.
Chen, Y., Liu, N., Hu, F., Ye, L., Xi, Y., Yang, S., 2018. Thermal treatment and ammoniacal
leaching for the recovery of valuable metals from spent lithium-ion batteries.
Waste Manag. 75, 469–476.
Chitre, A., Freake, D., Lander, L., Edge, J., Titirici, M.M., 2020. Towards a more sustainable
lithium-ion battery future: recycling LIBs from electric vehicles. Batteries & Supercaps
3, 1–12.
9
Science of the Total Environment 776 (2021) 145913
Choi, Y., Rhee, S.W., 2020. Current status and perspectives on recycling of end-of-life bat-
tery of electric vehicle in Korea (Republic of). Waste Manag. 106, 261–270.
Commission E. Frequently Asked Questions on Directive 2006/66/EU on Batteries and Ac-
cumulators and Waste Batteries and Accumulators. Available at: <https://ec.europa.
eu/environment/waste/batteries/pdf/faq.pdf> (accessed 8 November 2020). 2014.
Corsini, F., Rizzi, F., Frey, M., 2017. Extended producer responsibility: the impact of orga-
nizational dimensions on WEEE collection from households. Waste Manag. 59,
23–29.
Cusenza, M.A., Guarino, F., Longo, S., Mistretta, M., Cellura, M., 2019. Reuse of electric ve-
hicle batteries in buildings: An integrated load match analysis and life cycle assess-
ment approach. Energy and Buildings 186, 339–354.
Diekmann, J., Hanisch, C., Froböse, L., Schälicke, G., Loellhoeffel, T., Fölster, A.-S., et al.,
2016. Ecological recycling of lithium-ion batteries from electric vehicles with focus
on mechanical processes. J. Electrochem. Soc. 164, A6184–A6191.
Directive, 2006. Directive 2006/66/EC of the European Parliament and of the Council of 6
September 2006 on batteries and accumulators and waste batteries and accumula-
tors and repealing Directive 91/157/EEC. Off. J. Eur. Union 266, 1–14.
Gasper, P., Hines, J., Miralda, J.-P., Bonhomme, R., Schaufeld, J., Apelian, D., et al., 2013. Eco-
nomic feasibility of a mechanical separation process for recycling alkaline batteries.
J. New Mater. Electrochem. Syst. 16, 297–304.
GGII. Analysis on the Market Prospect of Lithium battery recycling in China in 2020. GGII.
Available at: <https://www.gg-lb.com/art-41003-yj.html> (accessed 10 November
2020), 2020.
GOSC. The Implementation Plan of the Extended Producer Responsibility System. The
General Office of the State Council of the People's Republic of China. Available at:
<http://www.gov.cn/zhengce/content/2017-01/03/content_5156043.htm>
(accessed 09 November 2020). 2016.
Gu, F., Guo, J., Yao, X., Summers, P.A., Widijatmoko, S.D., Hall, P., 2017. An investigation of
the current status of recycling spent lithium-ion batteries from consumer electronics
in China. J. Clean. Prod. 161, 765–780.
Harper, G., Sommerville, R., Kendrick, E., Driscoll, L., Slater, P., Stolkin, R., et al., 2019.
Recycling lithium-ion batteries from electric vehicles. Nature 575, 75–86.
He, L.P., Sun, S.Y., Song, X.F., Yu, J.G., 2015. Recovery of cathode materials and Al from
spent lithium-ion batteries by ultrasonic cleaning. Waste Manag. 46, 523–528.
He, Y., Zhang, T., Wang, F., Zhang, G., Zhang, W., Wang, J., 2017. Recovery of LiCoO2 and
graphite from spent lithium-ion batteries by Fenton reagent-assisted flotation.
J. Clean. Prod. 143, 319–325.
He, Y., Yuan, X., Zhang, G., Wang, H., Zhang, T., Xie, W., et al., 2020. A critical review of cur-
rent technologies for the liberation of electrode materials from foils in the recycling
process of spent lithium-ion batteries. Sci. Total Environ. 142382.
Kahhat, R., Kim, J., Xu, M., Allenby, B., Williams, E., Zhang, P., 2008. Exploring e-waste
management systems in the United States. Resour. Conserv. Recycl. 52, 955–964.
Kang, D.H., Chen, M., Ogunseitan, O.A., 2013. Potential environmental and human health
impacts of rechargeable lithium batteries in electronic waste. Environ Sci Technol 47,
5495–5503.
Kiddee, P., Naidu, R., Wong, M.H., 2013. Electronic waste management approaches: an
overview. Waste Manag. 33, 1237–1250.
Kim, Y, Matsuda, M, Shibayama, A, Fujita, T. Recovery of LiCoO2 from wasted lithium ion
batteries by using mineral processing technology. Resources Processing 2004; 51:
3–7.
Larcher, D., Tarascon, J.M., 2015. Towards greener and more sustainable batteries for elec-
trical energy storage. Nat. Chem. 7, 19–29.
Li, L., Ge, J., Wu, F., Chen, R., Chen, S., Wu, B., 2010. Recovery of cobalt and lithium from
spent lithium ion batteries using organic citric acid as leachant. J. Hazard. Mater.
176, 288–293.
Li, L., Chen, R., Sun, F., Wu, F., Liu, J., 2011. Preparation of LiCoO2 films from spent lithium-
ion batteries by a combined recycling process. Hydrometallurgy 108, 220–225.
Li, L., Dunn, J.B., Zhang, X.X., Gaines, L., Chen, R.J., Wu, F., et al., 2013. Recovery of metals
from spent lithium-ion batteries with organic acids as leaching reagents and environ-
mental assessment. J. Power Sources 233, 180–189.
Li, L., Qu, W., Zhang, X., Lu, J., Chen, R., Wu, F., et al., 2015. Succinic acid-based leaching sys-
tem: a sustainable process for recovery of valuable metals from spent Li-ion batteries.
J. Power Sources 282, 544–551.
Li, J., Wang, G., Xu, Z., 2016a. Environmentally-friendly oxygen-free roasting/wet mag-
netic separation technology for in situ recycling cobalt, lithium carbonate and graph-
ite from spent LiCoO2/graphite lithium batteries. J. Hazard. Mater. 302, 97–104.
Li, J., Wang, G., Xu, Z., 2016b. Generation and detection of metal ions and volatile organic
compounds (VOCs) emissions from the pretreatment processes for recycling spent
lithium-ion batteries. Waste Manag. 52, 221–227.
Liu, Z., Liu, X., Hao, H., Zhao, F., Amer, A.A., Babiker, H., 2020. Research on the critical issues
for power battery reusing of new energy vehicles in China. Energies 13, 1932.
MEE. The Policy on Pollution Prevention Techniques of Waste Batteries (2016). The Min-
istry of Ecological and Environment of the People's Republic of China. Available at:
<http://www.mee.gov.cn/gkml/hbb/bgg/201612/t20161228_378325.htm>
(accessed 09 November 2020). 2016.
MEE. Annual Report on The Prevention and Control of Environmental Pollution by Solid
Waste in Major Cities of China in 2019. The Ministry of Ecological and Environment
of the People's Republic of China. Available at: <http://www.mee.gov.cn/ywgz/
gtfwyhxpgl/gtfw/201912/P020191231360445518365.pdf> (accessed 10 November
2020). 2019.
MEE. The Notice on Matters Related to the Total Ban on Solid Waste Import. the Ministry
of Ecology and Environment and other four departments.Available at: <http://www.
mee.gov.cn/xxgk2018/xxgk/xxgk01/202011/t20201125_809835.html> (accessed 30
November 2020), 2020.
S. Sun, C. Jin, W. He et al.
Meshram, P., Pandey, B.D., Mankhand, T.R., 2014. Extraction of lithium from primary and
secondary sources by pre-treatment, leaching and separation: a comprehensive re-
view. Hydrometallurgy 150, 192–208.
Meshram, P., Pandey, B.D., Mankhand, T.R., 2015. Hydrometallurgical processing of spent
lithium ion batteries (LIBs) in the presence of a reducing agent with emphasis on ki-
netics of leaching. Chem. Eng. J. 281, 418–427.
MIIT. The Interim Measures for The Management of Power Battery Recovery and Utiliza-
tion of New Energy Vehicles. seven ministries and commissions including the Minis-
try of Industry and Information Technology. Available at: <http://www.gov.cn/
xinwen/2018-02/26/content_5268875.htm> (accessed 09 November 2020). 2018a.
MIIT. The Interim Provisions on The Traceability Management of Power Battery Recovery
and Utilization of New Energy Vehicles. The Ministry of Industry and Information
Technology of the People's Republic of China. Available at: <https://www.miit.gov.
cn/zwgk/zcjd/art/2020/art_6abdf0902cc244ad9b4c04820129dfca.html> (accessed
09 November 2020). 2018b.
MIIT. The Notice on the Pilot Work of Power Battery Recycling of New Energy Vehicles.
seven ministries and commissions including the Ministry of Industry and Information
Technology. Available at: <http://www.gov.cn/xinwen/2018-07/26/content_
5309433.htm> (accessed 10 November 2020). 2018c.
MIIT. Research Report on Power Battery Recovery and Utilization of New Energy Vehicles
(Brief Introduction).The Ministry of Industry and Information Technology of the
People's Republic of China. Available at: <https://www.miit.gov.cn/n1146285/
n1146352/n3054355/n3057542/n3057545/c6651773/part/6651783.pdf> (accessed
30 November 2020), 2019.
MST. Project Application Guidelines of the Key Project of "Solid Waste Recycling" for 2018
Annual. Ministry of Science and Technology. Available at: <https://service.most.gov.
cn/u/cms/static/201809/14135408zpor.pdf> (accessed 1 December 2020). 2018.
MST. Project Application Guidelines of the Key Project of "Solid Waste Recycling" for 2019
Annual. Ministry of Science and Technology. Available at: <https://service.most.gov.
cn/u/cms/static/201907/231658111801.pdf> (accessed 1 December 2020), 2019.
NBS. National data. National Bureau of Statistics. Available at: <https://data.stats.gov.cn/
easyquery.htm?cn=A01&zb=A02092D&sj=202012> (accessed 20 January 2021).
2020.
Nie, H., Xu, L., Song, D., Song, J., Shi, X., Wang, X., et al., 2015. LiCoO2: recycling from spent
batteries and regeneration with solid state synthesis. Green Chem. 17, 1276–1280.
Niu, Z., Zou, Y., Xin, B., Chen, S., Liu, C., Li, Y., 2014. Process controls for improving
bioleaching performance of both Li and Co from spent lithium ion batteries at high
pulp density and its thermodynamics and kinetics exploration. Chemosphere 109,
92–98.
Nnorom, I.C., Osibanjo, O., 2008. Overview of electronic waste (e-waste) management
practices and legislations, and their poor applications in the developing countries.
Resour. Conserv. Recycl. 52, 843–858.
NPCSC. The Law of the People's Republic of China on The Prevention and Control of Solid
Waste Pollution. Standing Committee of the National People's Congress. Available at:
<http://www.gov.cn/xinwen/2020-04/30/content_5507561.htm> (accessed 10 No-
vember 2020). 2020.
Ogushi, Y., Kandlikar, M., 2007. Assessing extended producer responsibility laws in JAPAN.
Environmental Science & Technology 3, 4502–4508.
Pagnanelli, F., Moscardini, E., Altimari, P., Abo Atia, T., Toro, L., 2017. Leaching of electrodic
powders from lithium ion batteries: optimization of operating conditions and effect
of physical pretreatment for waste fraction retrieval. Waste Manag. 60, 706–715.
Pinna, E.G., Ruiz, M.C., Ojeda, M.W., Rodriguez, M.H., 2017. Cathodes of spent Li-ion batte-
ries: dissolution with phosphoric acid and recovery of lithium and cobalt from leach
liquors. Hydrometallurgy 167, 66–71.
Ruismäki, R., Rinne, T., Dańczak, A., Taskinen, P., Serna-Guerrero, R., Jokilaakso, A., 2020.
Integrating flotation and pyrometallurgy for recovering graphite and valuable metals
from battery scrap. Metals 10, 680.
Saeki, S., Lee, J., Zhang, Q., Saito, F., 2004. Co-grinding LiCoO2 with PVC and water leaching
of metal chlorides formed in ground product. Int. J. Miner. Process. 74, S373–S378.
Salhofer, S., Steuer, B., Ramusch, R., Beigl, P., 2016. WEEE management in Europe and
China - a comparison. Waste Manag. 57, 27–35.
Shaw-Stewart, J., Alvarez-Reguera, A., Greszta, A., Marco, J., Masood, M., Sommerville, R.,
et al., 2019. Aqueous solution discharge of cylindrical lithium-ion cells. Sustain.
Mater. Technol. 22, e00110.
Shenzhen. The Financial Support Policy for Promotion and Application of New Energy Ve-
hicles in Shenzhen in 2018. Shenzhen Municipal People's Government. Available at:
<http://www.sz.gov.cn/zfgb/2019/gb1087/content/mpost_4998331.html>
(accessed 10 November 2020). 2019.
Shin, S.M., Kim, N.H., Sohn, J.S., Yang, D.H., Kim, Y.H., 2005. Development of a metal recov-
ery process from Li-ion battery wastes. Hydrometallurgy 79, 172–181.
Silveira, G.T., Chang, S.Y., 2010. Cell phone recycling experiences in the United States and
potential recycling options in Brazil. Waste Manag. 30, 2278–2291.
SMM. Recycling policy and market analysis of waste lithium-ion power batteries. SMM
News. Available at: <https://news.smm.cn/news/100901750> (accessed 11 Novem-
ber 2020), 2019.
SOHU. "Cascade utilization" of power lithium-ion batteries has become a hot spot. Sohu
News. Available at: <https://www.sohu.com/a/234408085_470482> (accessed 11
November 2020), 2018.
Sommerville, R., Shaw-Stewart, J., Goodship, V., Rowson, N., Kendrick, E., 2020. A review
of physical processes used in the safe recycling of lithium ion batteries. Sustain.
Mater. Technol. 25, e00197.
Sonoc, A., Jeswiet, J., Soo, V.K., 2015. Opportunities to improve recycling of automotive
lithium ion batteries. Procedia CIRP 29, 752–757.
Sun, M., Yang, X., Huisingh, D., Wang, R., Wang, Y., 2015. Consumer behavior and perspec-
tives concerning spent household battery collection and recycling in China: a case
study. J. Clean. Prod. 107, 775–785.
10
Science of the Total Environment 776 (2021) 145913
Tang, Y., Xie, H., Zhang, B., Chen, X., Zhao, Z., Qu, J., et al., 2019. Recovery and regeneration
of LiCoO2-based spent lithium-ion batteries by a carbothermic reduction vacuum py-
rolysis approach: controlling the recovery of CoO or Co. Waste Manag. 97, 140–148.
TE. TRADING ECONOMICS.Available at: <https://tradingeconomics.com/commodity/co-
balt> (accessed 23 January 2021), 2021.
Terazono, A., Oguchi, M., Iino, S., Mogi, S., 2015. Battery collection in municipal waste
management in Japan: challenges for hazardous substance control and safety.
Waste Manag. 39, 246–257.
Tran, L.-H., Tanong, K., Jabir, A.D., Mercier, G., Blais, J.-F., 2020. Hydrometallurgical process
and economic evaluation for recovery of zinc and manganese from spent alkaline bat-
teries. Metals 10, 1175.
Turner, J.M., Nugent, L.M., 2016. Charging up battery recycling policies: extended pro-
ducer responsibility for single-use batteries in the European Union, Canada, and the
United States. J. Ind. Ecol. 20, 1148–1158.
Wang, R.-C., Lin, Y.-C., Wu, S.-H., 2009. A novel recovery process of metal values from the
cathode active materials of the lithium-ion secondary batteries. Hydrometallurgy 99,
194–201.
Wang, L., Li, S., Zhou, C., 2011. Experimental research on the cyanidation of gold ore con-
taining high content of arsenic in Qianxinan. Precious Metals 32, 41–46.
Wang, F., Sun, R., Xu, J., Chen, Z., Kang, M., 2016a. Recovery of cobalt from spent lithium
ion batteries using sulphuric acid leaching followed by solid–liquid separation and
solvent extraction. RSC Adv. 6, 85303–85311.
Wang, M.M., Zhang, C.C., Zhang, F.S., 2016b. An environmental benign process for cobalt
and lithium recovery from spent lithium-ion batteries by mechanochemical ap-
proach. Waste Manag. 51, 239–244.
Wang, X., Gaustad, G., Babbitt, C.W., 2016c. Targeting high value metals in lithium-ion
battery recycling via shredding and size-based separation. Waste Manag. 51,
204–213.
Wang, W., Zhao, Y., Liu, H., Song, S., 2017. Fabrication and mechanism of cement-based
waterproof material using silicate tailings from reverse flotation. Powder Technol.
315, 422–429.
Wang, F., Zhang, T., He, Y., Zhao, Y., Wang, S., Zhang, G., et al., 2018. Recovery of valuable
materials from spent lithium-ion batteries by mechanical separation and thermal
treatment. J. Clean. Prod. 185, 646–652.
Welfens, M., Nordmann, J., Seibt, A., Schmitt, M., 2013. Acceptance of mobile phone return
programmes for increased resource efficiency by young people—experiences from a
German research project. Resources 2, 385–405.
Widijatmoko, S.D., Gu, F., Wang, Z., Hall, P., 2020. Selective liberation in dry milled spent
lithium-ion batteries. Sustain. Mater. Technol. 23, e00134.
Williams, B.D., Lipman, T.E., 2010. Strategy for overcoming cost hurdles of plug-in–hybrid
battery in California. Transportation Research Record: Journal of the Transportation
Research Board 2191, 59–66.
Winslow, K.M., Laux, S.J., Townsend, T.G., 2018. A review on the growing concern and po-
tential management strategies of waste lithium-ion batteries. Resour. Conserv.
Recycl. 129, 263–277.
Xiao, J., Li, J., Xu, Z., 2017. Novel approach for in situ recovery of lithium carbonate from
spent Lithium ion batteries using vacuum metallurgy. Environmental Science & Tech-
nology 51, 11960–11966.
Xiao, J., Li, J., Xu, Z., 2020. Challenges to future development of spent lithium ion batteries
recovery from environmental and technological perspectives. Environ Sci Technol 54,
9–25.
Xin, B., Zhang, D., Zhang, X., Xia, Y., Wu, F., Chen, S., et al., 2009. Bioleaching mechanism of
Co and Li from spent lithium-ion battery by the mixed culture of acidophilic sulfur-
oxidizing and iron-oxidizing bacteria. Bioresour. Technol. 100, 6163–6169.
Xu, C., Zhang, W., He, W., Li, G., Huang, J., 2016. The situation of waste mobile phone man-
agement in developed countries and development status in China. Waste Manag. 58,
341–347.
Yamaji, Y, Dodbiba, G, Matsuo, S, Okaya, K, Shibayama, A, Fujita, T. A novel flow sheet for
processing of used lithium-ion batteries for recycling. Resources Processing 2011; 58:
9–13.
Yu, L., He, W., Li, G., Huang, J., Zhu, H., 2014. The development of WEEE management and
effects of the fund policy for subsidizing WEEE treating in China. Waste Manag. 34,
1705–1714.
Yu, J., He, Y., Li, H., Xie, W., Zhang, T., 2017. Effect of the secondary product of semi-solid
phase Fenton on the flotability of electrode material from spent lithium-ion battery.
Powder Technol. 315, 139–146.
Yu, J., He, Y., Ge, Z., Li, H., Xie, W., Wang, S., 2018. A promising physical method for recov-
ery of LiCoO 2 and graphite from spent lithium-ion batteries: grinding flotation. Sep.
Purif. Technol. 190, 45–52.
Yu, J., He, Y., Qu, L., Yang, J., Xie, W., Zhu, X., 2020. Exploring the critical role of grinding
modification on the flotation recovery of electrode materials from spent lithium ion
batteries. J. Clean. Prod. 274, 123066.
Zeng, X., Li, J., Singh, N., 2014. Recycling of spent lithium-ion battery: a critical review. Crit.
Rev. Environ. Sci. Technol. 44, 1129–1165.
Zeng, X., Li, J., Liu, L., 2015a. Solving spent lithium-ion battery problems in China: oppor-
tunities and challenges. Renew. Sust. Energ. Rev. 52, 1759–1767.
Zeng, X., Li, J., Shen, B., 2015b. Novel approach to recover cobalt and lithium from spent
lithium-ion battery using oxalic acid. J. Hazard. Mater. 295, 112–118.
Zhan, R., Oldenburg, Z., Pan, L., 2018. Recovery of active cathode materials from lithium-
ion batteries using froth flotation. Sustain. Mater. Technol. 17, e00062.
Zhang, T., He, Y., Ge, L., Fu, R., Zhang, X., Huang, Y., 2013. Characteristics of wet and dry
crushing methods in the recycling process of spent lithium-ion batteries. J. Power
Sources 240, 766–771.
Zhang, T., He, Y., Wang, F., Li, H., Duan, C., Wu, C., 2014. Surface analysis of cobalt-enriched
crushed products of spent lithium-ion batteries by X-ray photoelectron spectroscopy.
Sep. Purif. Technol. 138, 21–27.
S. Sun, C. Jin, W. He et al.
Zhang, X., Cao, H., Xie, Y., Ning, P., An, H., You, H., et al., 2015. A closed-loop process
for recycling LiNi1/3Co1/3Mn1/3O2 from the cathode scraps of lithium-ion
batteries: process optimization and kinetics analysis. Sep. Purif. Technol. 150,
186–195.
Zhang, G., He, Y., Feng, Y., Wang, H., Zhu, X., 2018a. Pyrolysis-ultrasonic-assisted flotation
technology for recovering graphite and LiCoO2 from spent lithium-ion batteries. ACS
Sustain. Chem. Eng. 6, 10896–10904.
Zhang, W., Xu, C., He, W., Li, G., Huang, J., 2018b. A review on management of spent lith-
ium ion batteries and strategy for resource recycling of all components from them.
Waste Manag. Res. 36, 99–112.
Zhang, X., Li, L., Fan, E., Xue, Q., Bian, Y., Wu, F., et al., 2018c. Toward sustainable and
systematic recycling of spent rechargeable batteries. Chem. Soc. Rev. 47,
7239–7302.
Zhang, Y., He, Y., Zhang, T., Zhu, X., Feng, Y., Zhang, G., et al., 2018d. Application of Falcon
centrifuge in the recycling of electrode materials from spent lithium ion batteries.
J. Clean. Prod. 202, 736–747.
Zhang, G., He, Y., Wang, H., Feng, Y., Xie, W., Zhu, X., 2019. Application of mechanical
crushing combined with pyrolysis-enhanced flotation technology to recover
11
Science of the Total Environment 776 (2021) 145913
graphite and LiCoO2 from spent lithium-ion batteries. J. Clean. Prod. 231,
1418–1427.
Zhang, G., He, Y., Wang, H., Feng, Y., Xie, W., Zhu, X., 2020. Removal of organics by
pyrolysis for enhancing liberation and flotation behavior of electrode mate-
rials derived from spent lithium-ion batteries. ACS Sustain. Chem. Eng. 8,
2205–2214.
Zheng, X., Gao, W., Zhang, X., He, M., Lin, X., Cao, H., et al., 2017. Spent lithium-ion battery
recycling - reductive ammonia leaching of metals from cathode scrap by sodium
sulphite. Waste Manag. 60, 680–688.
Zhou, L., Xu, Z., 2012. Response to waste electrical and electronic equipments in China:
legislation, recycling system, and advanced integrated process. Environ Sci Technol
46, 4713–4724.
Zhu S-g, He W-z, Li G-m, Zhou X, Zhang X-j, Huang J-w. Recovery of Co and Li from spent
lithium-ion batteries by combination method of acid leaching and chemical precipi-
tation. Trans. Nonferrous Metals Soc. China 2012; 22: 2274–2281.
Zhu, X., Tao, Y., He, Y., Zhang, Y., Sun, Q., 2017. Pre-concentration of graphite and LiCoO2
in spent lithium-ion batteries using enhanced gravity concentrator. Physicochemical
Problems of Mineral Processing 54, 293–299.