Current and Prospective Li-Ion Battery Recycling and Recovery Processes
Current and Prospective Li-Ion Battery Recycling and Recovery Processes
JOSEPH HEELAN 0
ERIC GRATZ 0
ZHANGFENG ZHENG 0
QIANG WANG 0
MENGYUAN CHEN 0
DIRAN APELIAN 0
YAN WANG 0
0 1.-Department of Mechanical Engineering, Center for Resource Recovery and Recycling (CR3), Worcester Polytechnic Institute , 100 Institute Road, Worcester, MA 01609 , USA. 2.-Battery Resourcers LLC , 200 Westboro Road, North Grafton, MA 01536, USA. 3.-
The lithium ion (Li-ion) battery industry has been growing exponentially since its initial inception in the late 20th century. As battery materials evolve, the applications for Li-ion batteries have become even more diverse. To date, the main source of Li-ion battery use varies from consumer portable electronics to electric/hybrid electric vehicles. However, even with the continued rise of Liion battery development and commercialization, the recycling industry is lagging; approximately 95% of Li-ion batteries are landfilled instead of recycled upon reaching end of life. Industrialized recycling processes are limited and only capable of recovering secondary raw materials, not suitable for direct reuse in new batteries. Most technologies are also reliant on high concentrations of cobalt to be profitable, and intense battery sortation is necessary prior to processing. For this reason, it is critical that a new recycling process be commercialized that is capable of recovering more valuable materials at a higher efficiency. A new technology has been developed by the researchers at Worcester Polytechnic Institute which is capable of recovering LiNixMnyCozO2 cathode material from a hydrometallurgical process, making the recycling system as a whole more economically viable. By implementing a flexible recycling system that is closed-loop, recycling of Li-ion batteries will become more prevalent saving millions of pounds of batteries from entering the waste stream each year.
Lithium ion (Li-ion) batteries are a very important
member of the rechargeable battery family, due to
their high discharge voltage, high volumetric and
gravimetric energy density, and long cycle life. A
typical Li-ion battery consists of an intercalated
lithium compound as the cathode and graphite as
the anode. The electrolyte supplies the ionic channel
for lithium ions transferring between the cathode
and anode. Cathode acts as the source of lithium ions
while the anode initially contains no Li-ions.1 In the
history of lithium battery development, the Li-ion
battery was derived from the lithium metal battery.
In 1972, Whittingham at Exxon reported the first
lithium metal battery with TiS2 as the cathode,
lithium metal as the anode, and lithium perchlorate
in dioxolane as the electrolyte, since TiS2 was the
best intercalation compound available at that time.2
However, the progress of this system was hindered
by dendritic growth of lithium during cycling of the
lithium metal. Later on, lithium alloy3 was
considered as a substitute for lithium metal to solve the
dendrite issue. However the volume swing caused
by lithium intercalation/deintercalation led to poor
cyclability. To circumvent the safety issue, the
insertion materials that could accept Li-ions were
simultaneously adopted as the cathode and anode
by Murphy et al.4 and then by Lazzari and Scrosati5
which led to the first Li-ion battery technology at
the end of the 1980s and early 1990s.
In the next stage of Li-ion battery advancement, a
lithium-oxide material was used as the cathode
when it was discovered that oxides permitted
suitable lithium intercalation.6 Later on, a
framework structure (V6O13) proved to be an excellent
electrode material for Li intercalation.7
Goodenough proposed a better solution for
cathode chemistry using the formula LixMO2 (M = Co,
Ni or Mn). This family of cathodes is widely used in
modern Li-ion batteries.8–10 In 1991, the Sony
Corporation commercialized the first Li-ion battery
composed of LiCoO2 as the cathode and carbon as
the anode.11 For safety and capacity reasons, Ni and
other metals, such as Al, Ga, Mg or Ti, were applied
as a cation substitute for Co. For example,
LiNi1 xTix/2Mgx/2O2 was claimed to be safer and
has a specific capacity of 180 mAh g 1 compared to
LiCoO2 which has a specific capacity of
140 mAh g 1.12 In 1996, Goodenough et al.
proposed lithium iron phosphate as a cathode
alternative and Chiang et al. improved the material’s
performance in 2002 by doping the material with
aluminum, niobium and zirconium.13 LiFePO4 has
an olivine (magnesium iron silicate) oxyanion
scaffolded structure, which possesses M-O-X bonds.
This structure attracted significant interest, since
the transition-metal redox potentials can be altered
by the presence of X.14
The anode material has also evolved over time.
Research efforts have been focused on materials
with higher capacity and slightly more positive
intercalation voltages compared to Li+/Li. Li3
xCoxN has a stable and reversible capacity of
600 mAh g 1.15 In 1997, Idota et al. commercialized
a new Li-ion technology by using an amorphous tin
composite oxide as the anode.16 In the Sn-Fe-C
system,17 intermetallic alloys, such as Cu6Sn5, InSb
and Cu2Sb, revealed an appealing low voltage and
reversible reactivity.18 The Li-ion storage
mechanism of MO (M = Co, Ni, Fe, Cu or Mn) was
reinvestigated by Poizot et al.19 Due to its high
capacity, Si is a promising anode material, which
has drawn wide attention from both industry and
Since the inception of the commercial Li-ion
batteries in 1991, the market size has increased
exponentially, especially in portable consumer
electronics. In 2014, there were over 1500 million cell
phones in use powered by Li-ion batteries, up from
less than 300 million in 2000.23 The current overall
Li-ion battery market has reached over US$20
In addition, Li-ion batteries have since 2010
been gradually used in larger size systems such as
hybrid and electric vehicles due to higher power
and energy density.24–26 With 2.72 million HEVs/
PHEVs/EVs being sold in 2015, the current Li-ion
batteries market in the automotive industry has
reached over $5 billion.23 Because of the global
growth of Li-ion batteries used in the automotive
industry over the last 5 years, it is estimated that
the global market for electric vehicles will reach
$25 billion by 2025.27
MATERIALS USED IN LI-ION BATTERIES
Li-ion batteries are mainly composed of four parts:
cathode, anode, electrolyte, and separator.
Electrodes consist of particulate active material, carbon
conductive additive, polymeric binder, and current
collector. Carbon conductive additives are necessary
to provide sufficient electron transport to the site of
lithium intercalation in electrode.28 When the mass
fraction of the additives (such as carbon spheres,
carbon black, carbon fibers, and carbon tubes) is
sufficiently high and exceeds the percolation
threshold,29 there is enough carbon to form a connected,
percolating network throughout the electrode.
Polyvinylidene difluoride (PVDF) is widely used as
the binder,30 but environmentally friendly binders
such as carboxymethyl cellulose (CMC) or styrene
butadiene rubber (SBR) are gradually replacing
PVDF.31,32 Aluminum, abundantly available and a
light metal, is used as the current collector for the
cathode because it forms a passivation layer to inhibit
oxidative corrosion. However, it alloys with lithium
at low potentials, excluding its use as an anode
current collector, for which copper is used instead.
Extensive investigation on Li-ion batteries has
revealed a range of possible active materials. There
are different mechanisms behind lithium uptake and
release. These mechanisms include: (
into a crystalline host (such as in lithium cobalt oxide,
) electroplating (lithium metal), (
) alloying with
metals (such as with silicon33), (
reaction,34 and (
) other types of insertion such as in
amorphous carbon. Among them, several have been
already commercialized or are under development.
Graphite is extensively used as the anode
material.35 Graphite exhibits a low interaction potential,
and has a high specific capacity. Lithium titanate
(Li4Ti5O12, LTO) has a relatively low energy
density, but works in electrochemical windows in which
the organic electrolyte is perfectly stable, resulting
in no formation of SEI and no irreversible charge
losses during lithium intercalation, which leads to
long cycle life.36
Lithium cobalt oxide (LCO) was used in the first
successfully commercialized Li-ion batteries. To
reduce the cost of LCO, the cobalt is often replaced
by ternary transition metals changing the
composition to LiNixCoyMnzO2 with x, y and z close to 0.33.37
These layered nickel-manganese-cobalt (NMC)
oxides have a slightly lower energy density but
superior power density and cycle life compared to LCO.38
The properties of NMC can be fine-tuned by
changing the composition. Lithium iron phosphate
(LiFePO4, LFP) suggested by Padhi and
Goodenough, and lithium manganese oxide (LiMn2O4,
LMO) suggested by Thackeray and Goodenough
derive from inexpensive raw materials which render
LFP and LMO batteries attractive for electric
vehicles.10,14 LFP and LMO have relatively low
energy densities. Recently, lithium nickel cobalt
aluminum oxide (NCA) was developed for electrical
vehicles because of its high energy density and long
cycle life.39 Selecting anode and cathode materials
depends on which desired properties are more
needed for the specific application. Certain
electrochemical properties include energy density, power
density, cycle life, safety and cost.
The electrolyte has a significant impact on battery
performance. The rate capability, cycle life,
coulombic efficiency, operation temperature range and
safety of Li-ion batteries are mostly determined by
the electrolyte composition. The two main
components of liquid electrolytes are salt and solvent.
Although a few salts such as LiPF6, LiClO4, LiAsF6
and LiBF4 have been explored for batteries, LiPF6 is
used for commercial systems due to its non-toxicity
and thermal stability.40 The solvent is composed of
mixtures of alkyl carbonates, such as ethylene
carbonate (EC), propylene carbonate (PC),41
dimethyl carbonate (DMC) and diethyl carbonate
(DEC).42,43 In addition, electrolyte additives, such
as vinylidene carbonate (VC),44 are added to
improve the cycle life and safety of Li-ion batteries.
The separator is a critical component in Li-ion
batteries, serving two purposes: (
) to prevent
physical contact of the electrodes and to avoid
internal short circuiting; and (
) to provide an ionic
conduction path for the liquid electrolyte. Porous
polyolefin membranes as separators have been most
widely used in Li-ion batteries with liquid
electrolyte because of their comprehensive advantages
of performance, safety and cost.45,46 The polyolefin
includes polyethylene (PE),47 polypropylene (PP)48
and their blends such as PE–PP49 and high density
polyethylene (HDPE)-ultrahigh molecular
polyethylene (UHMWPE).50 Recently, a ceramic separator
for better mechanical and thermal stability has
been developed and commercialized.51
NEED FOR RECOVERY AND RECYCLING
Though Li-ion battery recycling rates trail many
other common materials and goods, the irony is that
lead acid batteries have almost a 99% recycling
rate.52 There are several reasons for the latter, and
most importantly there exist government
regulations requiring recycling of lead acid batteries
because lead is toxic. Additionally, lead acid
batteries have only one chemistry factor making them
simple and economically effective to recycle.
Moreover, there is a successful business model for the
recycling of lead acid batteries. Collection centers
and recovery technologies are in place. One of the
key lessons is that solutions for sustainability need
to have sustainable business models.
Unfortunately, there is limited economical upside
to recycle Li-ion batteries in today’s commercialized
technologies. This is due to the fact that current
industrial recycling processes depend on recovering
cobalt and nickel metals or their alloys. Although
there are a variety of cathode chemistries and
sortation based on chemistry which is challenging
and difficult, the incoming recycling stream is often
diluted with other metals. Only California,
Minnesota and New York have regulations requiring
Liion batteries to be recycled,53 but enforcement of
these laws is not strict and rarely enforced. As early
as 2006, it was shown that significant Li-ion battery
stockpiles had begun building up in developed
countries.54 Unfortunately, there are no up-to-date
numbers for the recycling rate in North America,
while in Europe, before regulation was imposed, the
recycling rate was only 9%.55
An estimation of the total amount of Li-ion
batteries recycled in North America can be made
by tracking the number and recycling rate of
ewaste devices, specifically those devices that use
Liion batteries. When an e-waste device is recycled, it
is often recycled with the battery and the battery is
sent to a separate recycler for recycling. This
number serves as an estimate and will not include
every Li-ion battery recycled in North America.
Table I shows that a minimum estimate for the
amount of Li-ion batteries recycled in North
America is 5569 tons with the majority of the battery
mass coming from laptops. The estimated volume
matches up well with the masses of Li-ion batteries
recycled by current commercial operations (see next
section). However, assuming North American
market share of 31% and an average Li-ion battery gets
US$300/kWh then the actually recycling rate is only
3%,23 which means that the Li-ion battery recycling
industry is dominated by laptop batteries. The
reason for this is that the laptop batteries are the
heaviest and have the highest recycling rate. Cell
phones, on the other hand, are the most used but
are recycled less frequently and therefore have a
lower mass. As a result of the low recycling rate, the
majority of Li-ion batteries are landfilled. With the
wide adoption of hybrid and pure electric vehicles,
this situation will become even worse. This creates
environmental concerns. For example, when left
unattended, Li-ion batteries in landfills may catch
fire or, if the electrolyte is exposed to water,
hydrogen fluoride formation can occur.60
Additionally, lithium may enter the ground water.61 All of
these are non-options for a sustainable future.
CURRENT INDUSTRIAL RECYCLING
Li-ion batteries are being recycled commercially
to extract valuable raw materials and to safely
dispose of a hazardous waste. Several companies
have developed predominately in North America
and Europe to handle the flux of end-of-life batteries
entering the waste stream every year (Table II).
The majority of Li-ion batteries come from
consumer electronics and electric/hybrid electric
vehicles. The two major mechanisms for Li-ion battery
recycling are pyrometallurgical and
hydrometallurgical processes. Pyrometallurgical treatment uses
high temperature smelting procedures to recover
cobalt and nickel as alloys. Hydrometallurgical
techniques use chemical leaching to facilitate
RECOVERY OF LI-ION BATTERIES
Li-ion batteries have seen increasing interest in
their recovery for second life applications. This is
particularly true for Li-ion batteries used in hybrid
electric vehicle/electric vehicle (HEV/EV)
applications where the battery is considered no longer
suitable for the vehicle when it reaches 80% of its
original capacity. These second-life batteries are
seeing much interest in being used as grid-level
storage devices.65,66 Additionally, there is interest
in using Li-ion batteries in EVs for vehicle to grid
(V2G) integration. In V2G integration, the EV
communicates with the grid (i.e., smart grid)
whether the battery will charge or discharge based
on the grid’s power demands and the price of
energy. Both scenarios of grid-level adaption of EV
batteries will have the most benefit in their ability
to help the grid meet high power pulses or load
fluctuations. These deviations from base-level grid
demands are estimated to cost the US between 5%
and 10% of its total electrical demand.65 Although
not currently mainstream, second-life use for EV/
HEV Li-ion batteries is a likely outcome for many
batteries. Since most EV/HEV batteries have not
reached their end of life, the percentage of batteries
that will be suitable for second-life applications is
unknown. Navigant predicts the second-life battery
vehicle market to grow from $16 million in 2014 to
$3 billion by 2035.67 While second life is a promising
scenario for end-of-life batteries, ultimately these
batteries will also have to be recycled.
LI-ION BATTERY RECYCLING IN OUR
Although different Li-ion battery recycling
processes have been commercialized, most of the
processes cannot handle mixed cathode chemistry or
only low valle materials are recycled. A new Li-ion
battery recycling process invented by Wang et al.68
at Worcester Polytechnic Institute (WPI) to recycle
Li-ion batteries regardless the battery size, shape or
cathode chemistry directly synthesizes new cathode
materials. This process is being commercialized by
Battery Resources, LLC (BR). BR uses a mixed
physical and hydrometallurgical process to directly
synthesis new active LiNixMnyCozO2 (x + y + z = 1)
cathode materials. Additionally, steel, copper,
aluminum, graphite and plastics are also recovered.
The synthesis of new active cathode materials as
well as the overall recycling process has been
published previously.68–70 The major advantages of
the BR recycling process are that it can handle any
Li-ion battery regardless of size, shape or cathode
chemistry, and recovers active cathode material
which accounts for over 70% of the battery value.68
Thus, the process has significant economic
advantages over traditional recycling processes, where
only the metal value is recovered.
By combining both physical and
hydrometallurgical processes, BR is able to recover all of the elements
of the Li-ion battery with the exception of the
electrolyte and solvent (lithium from LiPF6 is
recovered in the lithium recovery step).68 The only
material lost in the recycling process occurs due to
impurity removal; additionally, at the end of the
process, there is wastewater from the
hydrometallurgical process that must be disposed of. In total,
over 70% of the battery weight accounting for
inefficiencies can be recovered. Additionally, because
there are no pyrometallurgical steps, there are no
direct carbon emissions from the recycling process.
One major advantage of the BR process is the
ability to handle any type of Li-ion battery. While
the first Li-ion batteries used only LiCoO2, in the
current market, the cathode material used in Li-ion
batteries is changing every year. In 2008, over 60%
of Li-ion batteries used LiCoO2 cathode materials;
however, by 2012, that number has dropped to only
37.2% (Table III). That value is also expected to
drop to 25% by 2020.23 The decrease in Co is also
evident in the recycling stream. The composition of
the incoming recycling stream is expected to trail
the current market composition by 3–4 years due to
the lifetime of the batteries. The amount of Co, Ni,
and Mn present in Li-ion batteries collected from
the WPI recycling bins show that, in 2012, Co made
up over 90% of the transition metals present, and by
2014 that number had decreased to less than 60%
The performance of the recovered LiNi1/3Mn1/
3Co1/3O2 from recycled batteries has been tested at
both WPI and Argonne National Laboratory. The
material characterization and electrochemical
performance shows that the recovered material is very
similar to the commercial material. The cathode
materials where spherical and 10 lm in diameter,
with a capacity greater than 150 mA g 1 as tested
at both WPI and Argonne.72 As previously reported,
1 ton of spent Li-ion batteries has the potential to
generate over $6000 in revenue when the active
cathode material, steel, copper, and aluminum are
FUTURE PROSPECTS AND IMPLICATIONS
Today, millions of pounds of Li-ion batteries are
landfilled instead of recycled each year, depleting
natural resources like cobalt, nickel, and lithium.
Large-scale recycling directly equates to a more
sustainable, cyclic society, one that recovers
materials instead of disposing of them. Li-ion battery
recycling has not become more prevalent for three
) Current commercialized technologies are
limited and do not draw a large enough profit margin
to substantiate growth. For the most part, the
products of recycling processes are less valuable than
the batteries being processed and not all valuable
components of the battery are being recovered. The
business model for current recycling technologies is
not robust; (
) The cathode chemistries of Li-ion
batteries are constantly evolving, making it difficult
for recycling companies to adapt. And (
end-of-life Li-ion batteries are characterized as
hazardous, in many countries government mandates do
not exist that would force recycling.
To cope with the increasing number of Li-ion
batteries being used in various technologies,73 a
recovery process must be implemented at an
industrial scale that is economically viable now and in the
future. One solution is to develop a recycling system
that is completely closed-looped. The cathode
material is significantly more valuable than all other
components that make up a Li-ion battery. An ideal
technology could process any type of Li-ion battery
and recover the cathode instead of secondary raw
materials that require further processing to make
new active materials.
It is the responsibility of engineering leaders to
manufacture products that can be recovered at the
end of life and reused. How components are
assembled and how they can be disassembled and
recovered ought to be considered at the initial stages of
design. At present, we are addressing recovery and
recycling as an afterthought. The closed-loop
mindset and manufacturing for disassembly should be
considerations from day one. Today, we are using
most of the Periodic Table to manufacture the
components that our society consumes. These
elements are not renewable resources, and the
materials community has a responsibility to ensure that
we recover and reuse them at their end of life.
A more robust recycling system would provide the
outlet necessary to handle the flux of spent Li-ion
batteries facilitated by the rapid growth of the
electric and hybrid-electric vehicle market. With the
projected growth of future Li-ion battery use
increasing exponentially, it is critical that the
recycling market also react congruently. Although
different Li-ion battery recycling processes are
being commercialized in Europe and America, these
technologies cannot adapt to the changes of cathode
materials in Li-ion batteries and/or produce
highvalle materials. The recycling technology developed
at WPI and BR offers a closed-loop Li-ion battery
recycling process with the ability to recycle Li-ion
batteries of any size, shape and chemistry.
This work has been financially supported by the
National Science Foundation (NSF) under Grants
1230675, 1343439, 1464535 and 1549531, and WPI’s
Center for Resource Recovery and Recycling (CR3
an NSF I/UCRC).
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