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RECYCLING AND DISPOSAL OF LITHIUM

BATTERIES: AN ECONOMICAL AND
ENVIRONMENTAL APPROACH

ATAUR RAHMAN1*, RAFIA AFROZ2 AND MOHD SAFRIN1

1
Department of Mechanical Engineering, Faculty of Engineering,
2
Department of Economics, Faculty of Economics and Management Sciences,
International Islamic University Malaysia,
Jalan Gombak, 53100 Kuala Lumpur, Malaysia.

*Corresponding author: arat@iium.edu.my

(Received: 28 Nov. 2016; Accepted: 30th Oct. 2017; Published on-line: 1st Dec. 2017)
th

ABSTRACT: The adoption of lithium-ion battery technology for electric vehicles/hybrid

electric vehicles (EV/HEV) has recently received attention worldwide. The price of
cobalt (Co) and lithium (Li) has increased due to the production of EV/HEV. A used
lithium battery is a valuable source of active metals (Co, Li, and Al) and the optimal way
of extracting these metals from this waste is still studied. The focus of this paper is to
recover active metals using the hydrometallurgical method on a laboratory scale with a
48.8 Wh battery to reveal economic and environmental benefits. Calcination of extracted
active metals as pre-thermal treatment has been conducted at 700°C to remove the
organic compounds from the surface of active metals. The experiment has been
conducted and the result shows that the recovery of active metals (cathode) is 41% of the
cell cathode and 8.5% of the cell anode materials, which represent 48.8% and 23.4% of
the cathode and anode cell material price, respectively. By recycling about 47.34% of the
battery active metals, emissions can be reduced by 47.61% for battery metal production
and 60.7% for disposal transportation of the used battery. The total emission can be
reduced by about 52.85% by recycling the active metals in used batteries.
ABSTRAK: Adaptasi teknologi bateri Litium-ion ke dalam kenderaan elektrik/
kenderaan elektrik hibrid (EV/HEV) telah memdapat perhatian seluruh dunia baru-baru
ini. Harga kobalt (Co) dan litium telah bertambah hasil daripada EV/HEV. Perggunaan
bateri litium adalah sumber berharga kepada logam-logam aktif (Co, Li dan Al) dan cara
terbaik untuk mengekstrak logam-logam ini daripada sisa ini masih dipelajari. Fokus
kertas ini adalah untuk mendapatkan logam aktif dengan menggunakan kaedah
hidrometalurgikal dalam skala makmal dengan bateri 48.8 Wh untuk mendedahkan
faedah ekonomi dan alam sekitar. Proses penulenan pada logam aktif yang diekstrak
sebagai rawatan pre-haba telah dijalankan pada suhu 700 oC untuk membuang kompoun
organik daripada permukaan logam aktif. Eksperimen telah dijalankan dan keputusan
menunjukkan logam aktif didapati pada (katod) adalah 41% daripada sel katod dan anod
adalah 8.5% daripada bahan sel anod, di mana 48.8% dan 23.4% daripada sel katod dan
harga bahan sel anod, masing-masing. Dengan kitar semula logam aktif bateri sebanyak
47.43%, pelepasan boleh dikurangkan sebanyak 47.61% bagi penghasilan logam bateri
dan 60.7% bagi pengangkutan pelupusan bateri terpakai. Pelepasan total boleh dikawal
sebanyak 52.85% dengan mengitar semula logam aktif pada pengeluaran bateri.

KEYWORDS: Li-ion battery; electro-chemistry; calcination; recycling;economics and

environmental values

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IIUM Engineering Journal, Vol. 18, No. 2, 2017 Rahman et al.

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1. INTRODUCTION
Demand for electric vehicles (EVs) is growing around the world fairly rapidly. The
EV/HEV sales share will represent at least 50% of light-duty vehicle sales worldwide by
2050. The aim of EVs/HVs is to contribute greenhouse-gas emission reductions and
deliver substantial benefits in terms of improved oil security, reduced urban area pollution,
and noise. The actual penetration of EVs has been seen as a key factor in material demand
because these vehicles require larger batteries [1].
Lithium-ion batteries play a major role in powering electric vehicles by meeting their
torque and speed demands. However, there is a threat regarding the availability of the
lithium needed for battery production. This threat has shifted focus towards ensuring a
continuous supply of materials needed for the green revolution through reuse and
recycling. The dominant chemistry used in electronics batteries of active metals like Ni,
Co., and Al for LCA battery, Li, Fe and phosphate (P) for LFP and Li, manganese (M) and
sulfate (S) for LMS battery electrochemistry, as shown in Table 1. The battery contains a
weight percentage (wt%) of lithium carbonate that is less expensive compared to cobalt
(Co) or nickel (Ni). The average lithium cost associated with Li-ion battery production is
less than 3% of the production cost while the battery metal production cost is about 200%
higher than the battery metal‟s recycle cost [2]. Intrinsic value for the Li-ion recycling
business currently comes from valuable metals such as Co and Ni that are more highly
priced than Li.
Table 1: Battery materials
System LCA LFP LMS
/Electrodes
Graphite Graphite MS TiO
Cathode LiNi0.8Co0.15Al0.05O2 LiFePO4 LiMn2O4 LiMn2O4
Anode Graphite Graphite Graphite Li4Ti5O12
Note: NCA: nickel, cobalt and aluminum; LFP: lithium iron phosphate;
LMO: lithium manganese oxide; LMS: lithium manganese salt

General Motor‟s claim that “one million tons of lithium is enough to produce 395
million Chevrolet Volts each with the power capacity of 16 kWh and battery
electrochemistry chemistry LiFePO4”, i.e. 158 g of lithium metal required per kWh battery
and hence the lithium needs are in the range of 113-246 g per kWh lithium-ion battery
development. In addition, the theoretical charge density of lithium metal from fundamental
electrochemistry is 3.8 Ah/g, representing 1 g of lithium, could supply 3.8 A of electric
current for 1 hour [3].
Recycled lithium is as much as five times the cost of lithium produced from the least
costly brine-based process [4,5]. However, with the increasing number of EVs entering the
market in the future, and with a significant supply crunch, recycling is expected to be an
important factor for consideration in effective material supply for battery production.
Metal compositions of Li-ion batteries are mainly Al, Cu, Co, Fe, and Li, as shown in
Table 2. The anode typically consists of Cu foil covered by a fine layer of carbon while
the cathode contains Al, Co, and Li metals. It is particularly interesting to focus research
on the recycling of cathodes as the active material. Such components represent 41%, by
weight, of the cell components or 48.8% of the cell price. The price of Al, Cu, Ni, Co and
Li per kilogram are USD1.58, USD5.3, USD10.57, USD27.5 and USD9.5, respectively
[1].

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Research has been reviewed to identify an economical and easy recycling process [6,
7]. Several methods could be preferred to recycle used Li-ion batteries for metal recovery;
hydrometallurgical-based and pyro-metallurgical-based processes are the most
predominant. As the pyro-metallurgical process is expensive and consumes too much
energy, most of the previous literature prefers the hydrometallurgical process for metal
recovery. In this study, the recovery of Al, Co, Fe, and Li metals from the cathode of the
used Li-ion battery is focused using hydrometallurgical processes [8]. The steps are
associated with the hydrometallurgical processes: physical separation of the battery
(dismantling), manual separation of anode and cathode, acid leaching for the cathode, and
crystallization testing for recovery of the Co metal.
The global EV market will represent more than 7% of the light-duty vehicle market
by 2020 and 70% of EVs are powered by Li-ion batteries. The green revolution, through
reuse and recycling of batteries, has become a crucial topic in the automotive industry
ensuring the availability of lithium needed for battery production. Recycling of used
lithium batteries is the primary focuses of this work to extract active valuable metals such
as cobalt (Co) and lithium (Li).

Table 2: Composition of lithium battery [6]

Components Amount (wt%)
Cathode, Anode, and Electrode 40  1.5%
Plastic case 22  1
Steel case 11  1.5
Copper foil 9  0.5
Aluminum foil 6.5  0.5
Electrolyte 5  1.5
Solvent 5.5  1
Electrical board and circuit 1.5 0.5

2. MATERIALS AND METHODS

Recycling batteries is beneficial to the environment. It keeps them out of landfill,
where heavy metals may leak into ground when the battery casing corrodes, causing soil
and water pollution. The composition of an Li-ion battery is shown in Table 2.
2.1 Recycling and Disposal
The author [9] has developed a „hydrometallurgy‟ process (Fig. 1) by modifying the
hydrometallurgy process to recover the LiCoO2 battery metals. Mechanical pre-treatment
(Calcination) and physical separation are applied to recover the battery materials such as
plastic, metal casings, Co, Li, Cu, Al, and Fe [7]. In the hydrometallurgical process,
lithium batteries are first dismantled to separate plastic and iron scraps from the active
electrode materials by physical separation using crushing, sieving, and magnetic
separation. The leaching method involves a model to separate the battery electrodes by
dissolving them into an aqueous solution HCl, and H2SO4 with and without H2O2. The
used LiCoO2 battery of 48.8 Wh capacity and 302 g weight has been used in this study to
recover the metals. Mechanical treatment, breaking apart plastic and cells, and some
physical separations have been performed by means of gravity and magnetism. Crushed
plastics from shells can be separated by flotation. Using magnetism the steel parts of the
containers are separated.

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IIUM Engineering Journal, Vol. 18, No. 2, 2017 Rahman et al.

Fig. 1: Lithium battery recycling model (A) metallurgy process, (B) precipation process
by using Na2CO3 solution, (C) solvent extraction process by Cyanex 272 agent, (D)
electrolysis process by using current density 200-250 A/m2, (E) crystalization process.

2.2 Leaching Process

Leaching is a liquid-solid operation. Two phases are intimately in contact; the anode
of the battery is diffused from the electrolyte to the liquid phase, which causes a separation
of the components originally in the solid. The rate of mass transfer of the cathode can be
estimated by,
(1)

where, is the mass rate of cathode materials dissolved into the solution, A is the
surface area of chop particles of cathode in m2, km is the mass transfer coefficient of
cathode into the acid solution in m/s, Scm(s) is the saturation solubility of the battery active
materials (Li, Co, Al) in the aqueous solution (HCl and H2SO4 with and without H2O2) in
kg∙mol/m3, and ca is the concentration of the aqueous soluble compounds of cathode
materials at time t sec in kg∙mol/m3. The rate of accumulation of Li in the solution is equal
to the dissolving beaker:
ca( f ) f t
dca k
ò = m A ò dt
Sli( s) - ca V ti
(2)
ca( i)

If the dissolving time (t) of the cathode material into the solution between time, t= ti to
tf and concentration, ca = ca(i) to ca(f), by integrating Eq. (2), the saturation solubility of Li
can be modelled as,

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IIUM Engineering Journal, Vol. 18, No. 2, 2017 Rahman et al.

km A D t

( )
Scm( s) = ca (f ) - ca( i) + e V (3)

with Dt = ( t f - ti ) . where, Scm(s) is the rate of cathode material accumulation in the

solution kg∙mol/m3.
The 3 M of HCl solution has been prepared by mixing 75 ml of HCl with 300 ml of
distilled water based on reported work [8]. The cathode of the battery was cut into small
pieces of 2g each and put into acid solution and stirred with a magnetic stirrer for 1 hr. The
temperature of the solution was varied to identify the changes in leaching rate. The
leaching test was performed at room temperature of 30 oC and by varying the temperature
in the range of 60 oC - 80 oC with the inorganic acid solutions of HCl and H2SO4 with and
without H2O2. The effect of H2O2 on the percentage of metal obtained from the leaching
process was studied. From observation, the presence of H2O2 as the reducing agent of
H2SO4 makes a „Piranha‟ solution (H2SO5) and separates lithium and Co metal.
2.3 Physical Separation
The composition of the LiCoO2 battery after physical separation is presented in Table
3. The peeled cobalt lithium oxide from aluminum foil is gained by the vacuum pyrolysis
process, which is leached with inorganic acids such hydrochloric acid (HCl), and sulfuric
acid (H2SO4). Hydrochloric acid can leach Co and Li more efficiently and economically.
By adding H2O2 with H2SO4, the Co and Li leaching efficiencies have been increased. The
optimal volume percentage of H2O2 is in the range of 1-10% and can be used in the
leaching process [8, 9]. In this study, 2 vol% of H2O2 with 4 M H2SO4 were used. After
leaching, the leaching solution and insoluble residue were separated by filtration for the
precipitation, solvent extraction, and electrolysis processes to recover Co and
crystallization test to identify the intensity of Cu, Li, CoSO 4 using the established X-ray
diffraction (XRD) method.

Table 3: Battery (48.8 Wh LiCoO2) materials composition

Components Amount (%)
Cathode, Anode, and Electrode 46.2
Plastic case 18.63
Steel case 10.56
Copper barrel 7.5
Aluminum foil 1.8
Electrical board and circuit 2.75
Others 12.56

2.4 Precipitation
The chemical precipitation method has been conducted for recovering Co and Li. The
precipitation of the leaching processes was collected to recover Li. The ammonium oxalate
[(NH4)2C2O4] 2 M was used with the precipitate for further precipitation of Co. The
precipitation was then collected and treated with Na2CO3 to recover Li and Co. The Li was
recovered about 82% with the Co impurities about 0.90%. The result can be supported by
the findings [10-12]. While the Co was extracted to 84%.
2.5 Solvent Extraction
Solvent extractant Cyanex 272 (a dialkyl phosphine acid extractant) was used to

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Citations (14) References (25)

... They also aspireto contribute to greenhouse gas emission reduction. Because electric vehicles require larger batteries and the actual adoption of EVs
has been viewed as a crucial element in material demand [46] . According to IRNEA (2017), all modern EVs rely on a type of lithium-ion-battery.
High energy density,high specific energy (see figure 7), and long life cycle are all characteristics of lithium-ion batteries. ...
... By 2020, the worldwide EV batteries will account for more than 75 of the market for light-duty vehicles, and 70% OF EVs are powered by Li-ion
batteries. To guarantee the supply of lithium required for battery production, the green revolution has become a major concern in the automobile
industry through the reuse and recycling of batteries [46] . The recycling of some materials doesn't always provide an ecological benefit compared to
the primary manufacturing of these raw materials because of the high process complexity and lengthy process in chains [80]. ...
... Paper ID: 1112722-06 ISSN: 2251-8843 However, given the rising number of EVs expected to hit the market in the future and the service
supply shortage [46] . An affordable and simple recycling procedure has been identified after reviewing the research [90]. ...

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Waleed Ahmed Shaikh · Muhammad Ahmed Kalwar · Asif Nawaz Wassan · Shakil Shaikh

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... Ten articles accounted for EoL transportation in an assessment of the environmental impact of lithium-ion battery reuse (Mathur et al.,
2019;Richa et al., 2017) or recycling (Accardo et al., 2021;Cerdas et al., 2018;Ciez and Whitacre, 2019;Hendrickson et al., 2015; Rahman et al.,
2017; Wang et al., 2020;Wang and Yu, 2021;Xiong et al., 2019a). However, only five discuss or report the results separately. ...
... However, only five discuss or report the results separately. These can be generally categorized as studies that report the relative contribution of EoL
transport as a percentage of overall emissions (Accardo et al., 2021;Ciez & Whitacre, 2019;Xiong et al., 2019;Hendrickson et al., 2015), and studies
that calculate the potential to reduce EoL transportation emissions, either through reuse (Mathur et al., 2019), recycling (Rahman et al., 2017) , or
system optimization (Hendrickson et al., 2015;Wang et al., 2020). ...
... (T.P. Hendrickson et al., 2015) Recycling California Freight trucking contributes 99% of human health damages from particulate matter (PM), 54%
of SO 2 damages, and 62% of total volatile organic compound (VOC) damages. (Rahman et al., 2017) Recycling Global/ Unspecified ...

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... Untuk menjaga produksi baterai lithium berkelanjutan, diperlukan fasilitas pembuangan p-ISSN : 2528-3561 e-ISSN : dan penanganan yang
memadai untuk baterai bekas. Hal ini terkait dengan biaya daur ulang baterai lithium yang sekitar 200% lebih rendah daripada biaya produksi dari
bahan alam [29] . Daur ulang baterai Lithium-ion dilakukan dengan proses hidrometalurgi, setelah elemen dan wadah plastik baterai dipisahkan secara
manual [29]. ...
... Hal ini terkait dengan biaya daur ulang baterai lithium yang sekitar 200% lebih rendah daripada biaya produksi dari bahan alam [29]. Daur ulang
baterai Lithium-ion dilakukan dengan proses hidrometalurgi, setelah elemen dan wadah plastik baterai dipisahkan secara manual [29] . Metode
penghancuran dan pemisahan dengan menggunakan magnet juga digunakan untuk memisahkan logam dari plastik. ...