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Opportunities to Improve Recycling of Automotive Lithium Ion Batteries

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DOI: 10.1016/j.procir.2015.02.039

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Procedia CIRP 29 (2015) 752 – 757

The 22nd CIRP conference on Life Cycle Engineering

Opportunities to Improve Recycling of Automotive Lithium Ion Batteries

Alexandru Sonoca and Jack Jeswieta*, Vi Kie Soob
a
Mechanical Engineering,Queens University, McLaughlin Hall, 130 Stuart Street, Kingston, ON. Canada, K7L 3N6
b
FEIT Australian National University, Australia
* Corresponding author. Tel.: +1- 613-533-2577. E-mail address: jeswiet@me.queensu.ca

Abstract

A high recovery of lithium from recycled lithium ion batteries (LIBs) is essential to ensure the growth and sustainability of the electrical
vehicle market. Without recycling, lithium demand is predicted to outstrip supply in 2023. Current industrial processes are focused on
recovering cobalt and other valuable metals because, given lithium’s current low price, it is economically unfavorable to recover it. As part of
our efforts to create a process where the recovery of lithium is economically viable we have analyzed the current industrial processes. We have
determined that, when applied to recycling automotive LIBs, they are needlessly energy intensive and complicated. In these processes whole
LIBs are incinerated, cryogenically cooled, or shredded under an inert atmosphere in order to make their cells safe to open. Instead of such
extreme measures, LIBs can be disassembled by automated processes, which recovers valuable electronics for reuse, their cells can be
discharged, which recovers residual energy, and then can be opened safely in air.
©
© 2015
2015 The
The Authors.
Authors. Published
Published by
by Elsevier B.V. This is an open access article under the CC BY-NC-ND license
Elsevier B.V.
Peer-review under responsibility of the International Scientific Committee of the Conference “22nd CIRP conference on Life Cycle
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Engineering.
Peer-review under responsibility of the scientific committee of The 22nd CIRP conference on Life Cycle Engineering
Keywords: automotive lithium ion batteries; battery recycling; safe opening of lithium ion batteries

1. Predicted shortage of lithium and shortcomings of
current processes of recycling lithium ion batteries
The world is on track to facing a severe scarcity of lithium
in the early 2020’s. Lithium, in the form of lithium carbonate,
is an essential ingredient in all lithium ion batteries. Lithium
ion batteries (LIBs) are the preferred battery choice for
portable devices, where they are used almost exclusively [1],
and for electric vehicles, whose production the IEA projects to
be 100 million vehicles annually in 2050 [2]. Electrification of
the world’s vehicle fleet along with a concomitant increase of
electricity production from renewable sources is highly
desirable as it is a major way to reduce greenhouse gas
emissions [2]. For the mid and near future (today towards
2030) it is projected that only batteries based on lithium
chemistries will satisfy the requirements of electric vehicles
[2]. Unfortunately, given the projected increase in demand for
lithium from batteries, even the most optimistic supply
scenario will not meet demand in 2023 [3], [4]. The supply
crunch could be averted if LIBs were recycled – 100%
recycling rate with a lithium recovery of 90 % would ensure
an adequate supply for all of the 21st century [5].
Unfortunately, today only 3% of lithium ion batteries are
recycled [3] and lithium recovery is negligible [1].
There are three industrial recycling processes for LIBs –
the Umicore process, the Sony-Sumitomo process, and the
Toxco process – and one newly commercialized process: the
Recupyl process [6]–[8]. There are also numerous processes
that are in development; an excellent review of them was
written by Zeng et al.[9]. However, the aim of the foregoing
recycling processes, both at the industrial and the lab scales, is
to recover cobalt and nickel as these have the highest value
(see Table 1 for prices of cathode materials); lithium recovery
is not a priority. Recycling processes that have a high recovery
of lithium has been investigated by a few researchers, as the
review by in the review by Chagnes and Pospiech (2013)
shows [10]. The highest lithium recycling efficiency reported
was 74.5% (leaching efficiency of 93.1% multiplied by
precipitation efficiency of 80%) [11]. However, as mentioned
before, typically Li is not a priority. Lithium carbonate is
perceived as cheap and readily available – for example, in a
recycling process developed at the lab scale published in 2014,
virgin lithium carbonate is used as a reagent to recover cobalt,
nickel, and manganese while the lithium present in the used
battery is considered an impurity to be removed [12]. The

2212-8271 © 2015 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Peer-review under responsibility of the scientific committee of The 22nd CIRP conference on Life Cycle Engineering
doi:10.1016/j.procir.2015.02.039
 Alexandru Sonoc et al. / Procedia CIRP 29 (2015) 752 – 757
simple fact is that lithium is still inexpensive to mine and
demand has not reached a point where supply is decreasing,
hence prices remain low.
Focusing only on the recovery of valuable materials while
recycling lithium ion batteries is problematic for two reasons.
First, without lithium there can be no lithium ion batteries.
While it is true that, as high density, easily accessible lithium
deposits become scarce, its value will increase and it will
make sense to improve recovery in the current processes, by
then, the price of lithium ion batteries will have increased.
LIBs already make up a large part of the cost of electric
vehicles, at today’s low lithium carbonate prices; a significant
increase in the price of the batteries will likely stall the
electrification of the world’s vehicle fleet [2]. Second reason:
cell manufacturers are switching to cheaper cathode materials,
such as lithium manganese oxide and lithium iron phosphate
to lower the price of batteries [12]. Without the high value
metals to be sold, processes designed to recover them may not
be adaptable enough to remain profitable if they are modified
to recycle batteries with the new, cheaper, chemistries.
Table 1: LIB cathode compounds and their market values
Compound Value (US$ per kg) Citation
Cobalt 37.00 [13]
LiCO3 6.40 [13]
LiCoO2 18.30 [14]
Li3NiCoMnO6 10.80 [14]
LiMnO2 3.70 [14]
LiFePO4 1.50 [14]
In our research we are developing a recycling processes
specifically for automotive lithium ion batteries, as these are
predicted to constitute the majority of the lithium demand in
the mid and far future [5] and to make up a waste stream of
340,000 tonnes per year by 2040 [15]. The aim of our
research is to develop or modify and existing process such
that lithium recovery is maximized, while energy use and
waste generated has been minimized. We began by examining
the Umicore, Sony-Sumito, Toxco, and Recupyl processes
and have identified that the pre-treatment steps in all of them
Fig. 1: Umicore process for 1 ton of lithium ion and Ni-Mh batteries
753
are needlessly energy intensive or process complicating when
recycling a large stream of automotive batteries. Just
decreasing the energy required for processing would be a
positive step. Pre-treatment is necessary because opening the
batteries “as is” results in an explosive reaction between
lithium ions and air [6], [7]. We present an alternative
pre-treatment – discharging batteries to 0.0V – and through a
safety analysis, which is central to this paper and is not
available for the processes named in the forging processes, it
is shown that it is a safe alternative to current industrial
practices. We also present a feasibility analysis based on
literature data and show that discharging batteries before
opening them is likely industrially feasible. Lastly, we present
preliminary results from LiCoO2 batteries we discharged
showing how much residual energy is left when they are
discharged below 3.0V (their practical lower voltage) to 0.0V.
We begin with a brief overview of the four industrial LIB
recycling processes and identify their lithium recycling
efficiency and energy requirements.
1.1 The Umicore process [14]
The Umicore process is a smelting process for spent
lithium ion and nickel metal hydride batteries (see Fig. 1). An
alloy of valuable materials (Co, Cu, Ni, Fe) is obtained from
the smelter and it is then treated hydrometralugically (acid
leaching followed by chemical precipitation to metal salts) to
give recovered metals. All of the lithium, aluminium and
manganese from the LIBs ends up in the slag and are not
recovered. For 1 ton of batteries 5000 MJ of heat are needed
for the smelter and gas clean-up.
1.2 The Sony-Sumitomo process
In the Sony-Sumitomo process LIBs are incinerated at
1000 °C [7]. The organics, lithium, and fluoride in the
batteries are lost as fly ash and are removed from the flue by a
scrubbing system. The metal residue obtained in the furnace is
processed hydrometallurgicaly to recover cobalt [8]. No
lithium is recovered. An estimate of the minimum energy
required to heat 1 ton of automotive li-ion polymer batteries is
992 MJ. The estimate takes 1011.8 J/kg/°C, the heat capacity
of 4Ah electric vehicle batteries given by Pesaran et al. (2001)
[16], and multiplies it by 1 ton of batteries and 980 °C.
754 Alexandru Sonoc et al. / Procedia CIRP 29 (2015) 752 – 757
1.3 The Toxco process [7], [14], [17]
In the Toxco process lithium metal primary batteries and
lithium ion secondary batteries are recycled. Batteries deemed
to be reactive, such a lithium metal batteries and large lithium
ion batteries, are cryogenically cooled with liquid nitrogen to
-196 °C; at this temperature the lithium inside the cells is
unreactive [17]. The batteries are then shredded and immersed
in water. Lithium ion/metal react with the water to produce
lithium hydroxide and hydrogen gas, which is burned above
the solution [8]. See Fig. 2 for an overview of the whole
process. The figure is the most detailed mass flow information
of the process available in the open literature and the only
information which can be used to calculate approximate
lithium yield. The lithium composition for lithium ion
batteries varies between 1.2 and 2 % [18]. If the 907.4 kg of
batteries in Fig. 2 were all lithium ion batteries than the
lithium yield of the Toxco process is between 15 and 26%.
Fig. 2: Toxco process for 907.4 kg of lithium metal and lithium ion batteries [14]
Additionally, per 907.4 kg of automotive li-ion polymer
batteries, the cooling requirement for the process is at least
198 MJ (per ton it is 219 MJ) ( calculated from the heat
capacity of the batteries, 1011.8 J/kg/°C, multiplied by 1000
kg and 211 °C). The shredding power requirement is given in
the figure and is equivalent to 565.2 MJ [14].
1.4 The Recupyl process [7]
In the Recupyl process lithium ion batteries are shredded
by a rotary shearing machine at 11 rpm and then crushed by a
rotor system at 90 rpm. Both steps occur in an air tight
enclosure filled with an inert atmosphere of argon and carbon
dioxide, which prevents a violent lithium reaction. Residual
oxygen content and pressure in the chamber are continuously
monitored and the data is used by a control system to
determine the rate of inert gas injection. The different
fractions obtained after shredding are: a fines fraction rich in
metal oxides and carbon, a magnetic fraction composed of
casings, a dense non-magnetic fraction made of Al and Cu
current collectors, and a low density non-magnetic fraction of
paper and plastic. The fractions are separated, while still
under an inert atmosphere. The fines fraction is added to
water. Lithium in the fines reacts with the water and releases
hydrogen gas. The water is heavily stirred and the fines are
added in a very controlled manner to prevent the
accumulation of hydrogen gas and an explosion. To further
prevent an explosion, the atmosphere above the bath is
maintained oxygen poor. The water becomes rich in lithium
hydroxide and lithium is recovered by adding sodium
carbonate or phosphoric acid. Hydrometallurgical means are
used to recover the rest of the materials. The lithium yield is
unknown.
2. Pretreatment alternative: Discharge batteries to 0.0V
then open and shred in air and immerse in leaching
solution
Amongst processes being developed we found a far
simpler pre-treatment procedure [19]. Ra and Han (2006)
report safely opening batteries by: removing packing, circuit
protection modules, temperature safety vents, and all other
materials surrounding individual cells. Individual cells were
then immersed in brine, left to discharge completely, and
opened in air in a ventilated space. Cathode and anode
materials were separated manually and were immersed in
leaching solution. No reactions of any kind were reported.
 Alexandru Sonoc et al. / Procedia CIRP 29 (2015) 752 – 757
Similarly, Krüger et al. (2014) started with individual cells,
discharged them to 0.0V with a resistor, opened them in air,
and immersed them in leaching solution. No adverse effects
were reported either [20].
We were intrigued: if completely discharging cells renders
then safe to open in air and process in water, then soaking in
brine or connecting to a resistor – both simple and low energy
processes – obviate the need for incineration, cooling with
liquid nitrogen, or shredding in airtight enclosures under an
inert atmosphere. Hundreds of MJ of energy would be saved
for every ton of batteries. The Recupyl process would be far
simpler and complex monitoring and heavy stirring would be
unnecessary. The Umicore process would have the
opportunity to be far less energy intensive since it could be
modified to shred batteries, isolate the fines fraction rich in
metal oxides and carbon (like in the Recupyl process) and
smelt only that fraction. Additionally, not only could the
pre-treatment step not be a large energy drain in any recycling
process but it could be a source of energy for the process:
discharging batteries liberates energy. What is missing from
the literature is a safety analysis of the hazards of opening
lithium and how discharging them mitigates them. Such an
analysis is necessary in order to determine if it is safe to open
batteries this way not only for one cell at a time in the lab but
for numerous cells at once in industry. We have performed
such an analysis and present it in this manuscript.
2.1 Hazards of opening a lithium ion cell and their mitigation
The main safety hazard of lithium opening a lithium ion
battery in air is the exothermic reaction of lithium ions or
lithium metal (if present) with oxygen. Opening in water
results in an exothermic reaction and the generation of
hydrogen gas, which is explosive.
Lithium ion pouch cells consist of anode, cathode,
separator, electrolyte, and polymer pouch. The anode is
graphite mixed with polyvinylidene fluoride binder deposited
on a copper foil. The cathode is lithium metal oxide (e.g.
LiCoO2, LiMnO2, LiNiO2, Li3NiMnCoO6, LiFePO4) mixed
with graphite and polyvinylidene fluoride binder deposited on
an aluminium foil. The electrolyte consists of a mixture of
non-aqueous solvents and lithium salts as well as additives to
slow down secondary reactions. When charging, lithium
de-intercalates from the metal oxide and intercalates in the
graphite, where it is thermodynamically unstable. When
discharging the process is reversed and lithium ions are
intercalated back into the lithium metal oxide. [21]
The main source of lithium ions in a cell are the free
lithium ions that cycle back and forth between the cathode
and anode as the cell is charged and discharged. By
completely discharging a cell to 0.0 V these free ions are
immobilized in the cathode, where they form a
thermodynamically stable lithium metal oxide which does not
react violently with water or air [21].
Other sources of lithium ions are the electrolyte salt
(typically LiPF6 [21]) and the solid electrolyte (SEI) interface
layer. This layer is formed on the anode during regular
operation and as it grows the cell loses capacity; when enough
capacity has been lost the cell is discarded. Lithium ions are
present in the SEI as lithium carbonate, lithium fluoride, or
lithium organic polymers [22], [23]; as such they are either
not reactive (in the case of carbonates or fluorides) or are
likely less reactive than free ions (in the case of the organic
755
polymers). Additionally, lithium ions in the electrolyte and
SEI are present in far smaller amounts than free lithium ions
[21]. These other sources of lithium ions have not been found
to be a safety concern when discharged lithium ion batteries
have been opened [12], [19], [24].
Damaged cells can have significant deposits of lithium
metal on the anode [22], which if exposed to air or water
would be very reactive. However, the presence of such
deposits would increase the internal resistance [22] and be
measurable as an large drop in cell voltage [25]. Damaged
cells cannot be safely opened and therefore should be
recycled, if at all, by processes which include an incineration/
immersion in liquid nitrogen/ or opening under an inert
atmosphere step.
The second safety hazard comes from vapours and gases
emitted by the electrolyte when exposed to air. The electrolyte
comprises 12 to 14% of the mass of a pouch cell used in
automobile batteries [26] and soaks the cell’s porous contents.
The electrolyte is composed of a lithium salt dissolved in an
organic solvent. The salt, typically LiPF6, usually makes up
10% by weight of the electrolyte. The organic solvent is
typically a mixture of ethylene carbonate and propylene
carbonate. LiPF6 hydrolyses in the presence of water via the
following reaction [3]
LiPF6 + H2O ė LiF + POF3 + 2HF
Hydrogen fluoride is a well know toxic gas. Ethylene
carbonate is flammable, a skin irritant, but classified as
non-hazardous in case of inhalation. Propylene carbonate is
flammable and an irritant of skin, eyes, and lungs. Batteries
even fully discharged must be opened in a well ventilated area
free from sparks such that the flammability and toxicity
hazards posed by the electrolyte are mitigated.
A third safety hazard is the discharging process itself. If
the batteries are discharged in brine their initial voltage will
be above the electrolysis voltage of water and hydrogen and
oxygen gases will be produced. These gases must be
ventilated to avoid an explosion. If the batteries are
discharged by a resistor the current must be kept low enough
so that the batteries do not over-heat. As long as cells are kept
below 90 °C, the onset temperature of runaway thermal
reactions [29], it is safe to discharge them.
LIBs are not usually operated at voltages as low as 0.0V.
They have a lower practical voltage, 3.0V for LiCoO2
batteries, and a circuit protection module is used to prevent
the battery from discharging below it [21]. We looked in the
literature for studies where batteries were discharged below
the lower practical voltage to see if there were any safety
hazards associated with discharging to 0.0V. The literature
reports that LiCoO2, LiMnO2, LiNiO2, LiCo1/3Mn1/3Ni1/3O2, or
LiFePO4 batteries suffer decreased cell performance due to
irreversible crystal changes at the cathode if they are
discharged to 0.0V [27], [28]. However, these crystal changes
do not pose any inherent safety risk [27], [28] and, since the
cells are to be recycled, a decrease in performance is
irrelevant.
To test whether discharging to 0.0V is indeed sufficient to
open batteries in air LiCoO2 pouch cells were opened. They
had a nominal capacity of 3.0 Ah, nominal voltage 3.7 V,
energy density of 195 Wh/kg, and a weight of 57 g. Cells that
were discharged to 0.5V produced small red flames and
fumes, showing a potential safety problem. Cells that were
discharged to 0.0 V produced neither flames nor fumes nor
756 Alexandru Sonoc et al. / Procedia CIRP 29 (2015) 752 – 757
did they show any evidence of reaction at all (no temperature
change or discoloration of materials was observed).
2.1 Energy obtained from discharging batteries
As part of the safety experiments, measurements were
made of the voltage of the discharging LiCoO2 batteries,
continuously, while discharging them with a 4.50 Ω
resistance. The voltage was measured every ten seconds and
the energy expended by the battery in a time interval was
calculated with the formula:
ܸଶ
‫ܧ‬ൌ ο‫ݐ‬
ܴ for practical usage due to aging; they are still safe to discharge
The cumulative energy expended by the batteries as they
discharged between 3.0 and 0.0 V was 0.96 ± 0.02 % of their
nominal capacity. For 1 ton of batteries with energy density of
195 Wh/kg this residual energy represents 7 MJ.
If the cells used come discharged to 3.0V to a recycling
plant, 7 MJ is the all that can be extracted from them. If on the
other hand the batteries come charged, say to 80% of their
nominal capacity 1 , then another 562 MJ of energy can be
extracted from 1 ton of 195 Wh/kg LIBs.
2.3 Feasibility of disassembling automotive batteries
The present manuscript has so far shown that discharging
cells to 0.0V is sufficient to opening them safely. It has also
shown that useful amounts of energy can be extracted from
the discharging batteries; this energy could be used to power
parts of the recycling process, such as heating the leaching
vessel. Cells are assembled into batteries; in order for them to
be discharged to 0.0V they must first be extracted from the
batteries whole. Literature on the dismantling of automobile
batteries to their constituent cells is reviewed below and the
argument is made that such dismantling is feasible in an
industrial setting.
Automotive batteries have three scales of organization:
cell, module, and pack [30]. Cells are the smallest component.
They can be cylindrical, prismatic or pouch. The exterior shell
of the former two is made of steel. The shell of pouch cells is
made of a polymer. Since they are light weight, pouch cells
are the preferred cell type for automobiles. In an automobile,
the cells are of the same chemistry and the same size. They
are also numerous: an electric car with 30kWh total electrical
capacity [2] would have 2140 cells if these were 4 Ah cells at
a discharge voltage of 3.5 V [16].
Cells are joined together, mechanically or by welding, in
series and parallel arrangements with heat sinks placed in
between them to make a module. The module is then fitted
with safety electronics (the aforementioned protection circuit
module), which prevent over-charge or over-discharge of the
cells, as well as a compression band and protective casing.
Modules are then connected to each other and control
electronics to make a battery pack. [30]
Herrmann et al. (2012) present a mixed manual and
automated process for disassembling batteries to individual
cells [25]. Batteries are first discharged to their cut-off low
voltage. They are then manually disassembled to the modules.
Control electronics are removed and can be reused. Modules
are automatically extracted from the battery pack and are
1
Rechargeable batteries are considered to have failed when they can only be
charged to 80% of their nominal capacity.
manually dismantled to expose cells. The cells are then
automatically removed from the modules. The authors write
that depending on the battery design it is possible to automate
the entire sequence.
The authors [25] designed an automated cell removal
system and fitted it with a voltmeter. The voltmeter is used to
determine the internal resistance of the cells and the state of
the cell is inferred from the internal resistance. Any cell that
has been damaged, such as by suffering an internal short, is
deemed unsafe to discharge and is discarded. Most cells to be
recycled are not damaged, but rather have a capacity too low
[22], [23].
Gaines (2014) [14] points out that the infrastructure for
collecting automotive batteries is already in place. 98% of
lead acid batteries are currently collected. Dealers are required
to collect them when new batteries are bought and are paid to
return them to manufacturers for recycling. The same
infrastructure could easily be used for lithium ion batteries.
Given the existing collection infrastructure and the high
likelihood manufacturers would standardize their battery
packs, it is probable that, when there will be a large number of
electric vehicles on the road, recycling facilities would have
sufficient battery packs of a similar enough design to recycle
to justify an investment in automated disassembly.
Disassembly of automotive LIBs in an industrial setting is
therefore likely feasible.
3. Conclusions
We have shown that current industrial processes of
recycling lithium ion batteries do not recover an adequate
amount of lithium to meet forecast demand from automotive
lithium ion battery manufacturers. We have also shown that,
when applied to automotive battery recycling, the current
recycling processes are needlessly energy intensive,
complicated, and wasteful in their pre-treatment steps. Instead
of incinerating, cryogenically cooling, or shredding under an
inert atmosphere, automotive batteries can be disassembled to
recover valuable electronic components and their cells can be
safely discharged to recover residual energy and to render
them safe to shred and treat by regular hydrometallurgical and
pyrometallurgical means. The adoption of these processes in
industry will lead to automotive LIB recycling processes
where it is economical to recover lithium as well.
4. Acknowledgements
The authors acknowledge the support of NSERC for this
work.
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