Perspective

Recycling End-of-Life Electric

Vehicle Lithium-Ion Batteries
Mengyuan Chen,1 Xiaotu Ma,1 Bin Chen,1 Renata Arsenault,2 Peter Karlson,2 Nakia Simon,2
and Yan Wang1,*

Lithium-ion batteries (LIBs) play a significant role in our highly electrified world Context & Scale
and will continue to lead technology innovations. Millions of vehicles are equip- The rapid increase in the use of
ped with or directly powered by LIBs, mitigating environmental pollution and lithium-ion batteries in electric
reducing energy use. This rapidly increasing use of LIBs in vehicles will introduce vehicles will introduce a large
a large quantity of spent LIBs within an 8–10-year span. Proper handling of end- quantity of spent lithium-ion
of-life (EOL) vehicle LIBs is required, and multiple options should be considered. batteries in the near future, and
This paper demonstrates that the necessity for EOL recycling is underpinned by the options to properly handle the
leveraging fluctuating material costs, uneven distribution and production, and spent lithium-ion batteries include
the transport situation. From a life-cycle perspective, remanufacturing and re- remanufacturing, repurposing,
purposing extend the life of LIBs, and industrial demonstrations indicate that and recycling. Remanufacturing
this is feasible. Recycling is the ultimate option for handling EOL LIBs, and and repurposing are extending
recent advancements both in research and industry regarding pyrometallurgi- the life of batteries, and recycling
cal, hydrometallurgical, and direct recycling are summarized. Currently, none closes the loop by returning
of the current battery recycling technologies is ideal, and challenges must be materials back to the value chain.
overcome. This article is anticipated as a starting point for a more sophisticated Pyrometallurgy, hydrometallurgy,
study of recycling, and it suggests potential improvements in the process and direct recycling are the three
through mutual efforts from academia, industry, and governments. recycling processes for spent
lithium-ion batteries. Academic
Scope and Method of This Perspective Paper innovations and industrial
In this paper, the needs and options to address end-of-life (EOL) lithium-ion batte- demonstrations of these three
ries (LIBs) are first discussed. Furthermore, the current status of LIB recycling, recycling processes are constantly
including academic innovations and industrial demonstrations, are systematically re- emerging and attempting to make
viewed, focusing on pyrometallurgical, hydrometallurgical, and direct recycling an impact. However, none of the
methods. The challenges facing current recycling technologies are analyzed, along current recycling technologies is
with potential suggestions or solutions. This study was conducted by establishing perfect, and challenges do exist.
scope and approach, searching related literature and industry demonstrations, By providing insights and
screening for inclusion, and providing insights. In addition, experts and industry rep- suggestions in this perspective
resentatives were interviewed to validate the accuracy of this study. paper, the direction for
improvement of lithium-ion
Needs battery recycling becomes clear.
LIBs currently dominate the market for electric vehicles (EVs), due to their high en- With the mutual efforts from
ergy and power density, and long life-span, combined with sweeping cost reduc- academia, industry, and
tions over the last decade. Millions of electric and hybrid vehicles that are powered governments, recycling will play a
by LIBs have been sold to date, and this number is projected to increase significantly significant role from both ecologic
in the coming years with the continued electrification of the automobile industry. Ac- and economic points of view.
cording to Avicenne Energy,1 LIBs represent the highest growth and the major
portion of industry investments. For example, worldwide, LIB sales have increased
by an average of 16% per year from 1996 to 2016. In 2016, the global LIB market
was over $20 billion at the cell level. By 2025, it is projected to reach $40 billion,
of which more than $15 billion will be from the hybrid and electric vehicle (xEV) mar-
ket. In the United States, there will be 1.4 million EV sales in 2035, as forecast by the

2622 Joule 3, 2622–2646, November 20, 2019 ª 2019 Elsevier Inc.

U.S. Energy Information Administration (EIA). This high demand for LIBs by the EV
market will translate into a large number of spent LIB packs, estimated at 1 million
in 2030 and 1.9 million in 2040. The cumulative EOL LIB packs generated between
2015 and 2040 will be as many as 21 million.2 Although the LIBs in these vehicles
are expected to last at least 8–10 years, EOL options must be considered now to
ensure infrastructure readiness when recycling needs reach greater volumes. In
fact, LIBs recycling is critical for several key reasons: buffering the uncertainties
associated with fluctuating material costs, rebalancing the uneven distribution and
production sourcing of strategic materials, and addressing the transport situation.

Fluctuating Material Costs

LIB costs have decreased by a factor of 5 over the past 10 years ($1,000/kWh in
2005 to $200/kWh in 2016).3 This is primarily a result of ever-increasing
manufacturing scale. However, material costs have been fluctuating significantly in
the last few years. For example, the price of lithium increased 3–4 fold ( $5/kg in
2010 to $20/kg in 2017) and dropped back to $10/kg at the end of 2018.4,5 Since
early 2017, the price of cobalt has tripled (from $30/kg to $90/kg in March 2018), and
dropped back to less than $40/kg in early 2019.6

Uneven Distribution and Production

The production of the main materials used in LIBs is dominated by a few countries,
shown in Figure 1.7 More than half of the cobalt used is from the Congo.8 Australia
and Chile control 80% of lithium production, while China controls 70% of
graphite production.

Transport Situation
LIBs are classified as category 9 hazardous materials, due to their unstable thermal
and electrical qualities9 and because of the risk of thermal runaway if improperly
handled during transportation. LIBs must undergo and pass a suite of national
and/or international tests prior to shipment by road, sea, or air. Having local and
mature recycling facilities has many advantages (economic, access to strategic ma-
terials, etc.) over shipping batteries to countries with less stringent regulations that
govern transport and recycling.

Reconciling the projected exponential growth in the demand for EV batteries, the
possibility of fluctuating prices for lithium and cobalt, and unsustainable production
of strategic materials poses a serious supply concern for the EV industry. Therefore,
EOL options for EV LIBs must be addressed with appropriate urgency. For example,
given the high costs of transporting spent LIBs, resulting from their hazardous mate-
rials classification, it would be ideal if LIBs could be recycled or rendered inert locally.

Options for End-of-Life EV Batteries

There are three possible options for EOL EV batteries, depending upon their design,
quality, and state of health (SOH): remanufacturing, repurposing, and recycling. Re-
manufacturing and repurposing extend the usage of LIBs, while recycling closes the
loop. To capture the maximum value of LIBs, the ideal scenario would involve rema-
nufacturing or repurposing first, followed by recycling.10,11 Remanufacturing is the 1Department of Mechanical Engineering,
most desirable EOL scenario in terms of maximizing the value and minimizing life-cy- Worcester Polytechnic Institute, Worcester, MA
01609, USA
cle energy consumption and emissions; however, this option is the most stringent in 2United States Advanced Battery Consortium
terms of battery quality requirements. Going directly from first life use (in-vehicle) to (USABC), 1000 Town Center Drive, Southfield, MI
recycling is less desirable from a life-cycle standpoint, because of insufficient 48075, USA
benefit, uncertainty about performance, and the unavoidable material and energy *Correspondence: yanwang@wpi.edu
losses that occur in the process. However, recycling is beneficial because LIBs https://doi.org/10.1016/j.joule.2019.09.014

Joule 3, 2622–2646, November 20, 2019 2623

Figure 1. Global Production of Main Lithium-Ion Battery Materials
Lithium, graphite, nickel, manganese, and cobalt represent the five key elements of current LIBs.
The global production is unevenly distributed and dominated by a few countries.

become part of the circular economy instead of becoming waste. That said, recycling
returns valuable materials back into the value chain promptly, partially mitigating the
need for extraction of new resources. Repurposing batteries for a non-automotive
(second life) use lies between these two scenarios, in terms of desirability. However,
considering the scalability and ease of processing, recycling is probably the simplest
and certainly the most broadly applicable solution for EOL EV batteries. It should be
noted that, even if batteries are first remanufactured or repurposed, they will ulti-
mately be recycled. The first two options only delay the recycling horizon. In this re-
view paper, recycling is the main focus of analysis.

2624 Joule 3, 2622–2646, November 20, 2019

Remanufacturing
Remanufacturing refers to refurbishing EV batteries and deploying them in their
original (automotive) applications. This requires that the EV batteries have accept-
able SOH and meet all OEM-specified requirements for power, energy, cycle life,
etc. According to the United States Advanced Battery Consortium (USABC), batte-
ries are generally not suitable for EV use when the delivered capacity or power of
a cell, module, or pack is less than 80% of its original rated value.12 Examination
of the entire battery pack could show that only a small percentage of cells failed
to hold the required capacity, and abandoning the entire battery pack represents
an incomplete usage. The idea behind remanufacturing is to replace inferior cells
or modules in the packs and return the remanufactured battery packs for use in EVs.

Industry Demonstrations. The number of EOL vehicle LIBs is likely to reach 50%
of the demand for new vehicle LIBs between the years 2020 and 2033, and according
to the cost-benefit analysis by Foster, remanufacturing spent LIBs saves 40% of the
cost of using new batteries.13 Remanufacturing LIBs involves diagnosis, partial disas-
sembly of battery packs, replacement of damaged cells or modules within the bat-
tery packs, and then reassembly into new battery packs.

Spiers New Technologies (SNT), a US-based startup located in Oklahoma, offers 4R

services (repair, remanufacturing, refurbishing, and repurposing) for vehicle original
equipment manufacturers (OEMs), including Nissan and General Motors. Character-
ized and sorted using SNT’s comprehensive diagnostic evaluations, EOL vehicle bat-
tery packs may be remanufactured to their original use (per OEM specifications) or
be repurposed to second-life redeployment in an alternate application. In May
2018, SNT announced its new production center at Ede in the Netherlands and
launched remanufacturing services for the rapidly growing European automotive
and energy markets. Looking ahead, SNT is actively promoting market development
in China, hoping to provide remanufacturing services to the largest xEV market
worldwide.

Global Battery Solutions (formerly Sybesma’s Electronics) has been repairing

electronics since 1958, and recently the company stepped into the field of repair-
ing xEV’s LIBs in western Michigan. Global Battery Solutions offers repair, remanu-
facturing, repurposing, and recycling, depending on the status of the degraded
LIBs. The company states that remanufactured batteries can cut replacement
cost by over 70%, and the BAE Corporation has started to use these remanufac-
tured cells.

Repurposing
Repurposing is another option for EOL batteries, whereby batteries are reconfigured
for ‘‘second life’’ use in less-stressful applications (such as stationary storage), thus
extracting more value by extending their useful lifetime beyond their automotive
‘‘first life’’ usage. In the case where a pack is unable to hold a desired capacity, for
example, 80% remanufacturing seems economically unfavorable, and repurposing
becomes a viable path. Repurposing not only requires replacing damaged cells or
modules but also requires reconfiguring the modules or packs, including establish-
ing a new battery management systems (BMSs), to accommodate a non-vehicle
application. However, repurposing faces numerous challenges, including reliably
grading the EOL packs or modules, dealing with the many different designs and
performance metrics, liability, and the cost of reconfiguration, which must compete
with new, cheaper batteries. For example, the original xEV manufacturer has the
responsibility to offer vehicle-use qualified LIBs. However, the risks and liability of

Joule 3, 2622–2646, November 20, 2019 2625

using batteries in non-original functions are not well defined. If repurposing is to
make a significant impact, liability standards need to be developed.14 Prospects
for battery repurposing require feasible economics and an underlying business
case. Testing, grading, and repackaging are the main cost contributors for repurpos-
ing EOL batteries, and costs could be minimized by exploiting more advanced tech-
nologies. For example, BMSs could be used to transmit SOH information and thus
expedite testing and grading operations. Also, service-based business models
could facilitate increased usage of repurposed batteries by minimizing consumers’
concerns regarding depleted capacity.15 Customers intuitively distrust degraded
batteries, but that uncertainty can be obviated if the manufacturer delivered more
value-added services, such as a warranty, consulting, installation, and maintenance
for repurposed batteries.16

Industry Demonstrations. Repurposed EOL batteries can be employed in various

second-use systems, such as peak shaving, back-up, frequency regulation, renew-
ables integration, and EV charging.17 Differentiated by power and time scale, EOL
batteries are repurposed for optimal alignment with the technical requirements of
second-use applications.14 In one example, Nissan’s repurposed EV LIBs are used
in the xStorage System: xStorage Home is an integrated solar and home energy stor-
age system; xStorage Building is a robust solution to efficiently power businesses
that have high energy-consumption demands.11 As the largest energy storage sys-
tem manufactured by second-life LIBs in Europe (4MW; 4MWh), xStorage Building
uses 280 Nissan LEAF batteries and has been used as back-up power in Amsterdam
ArenA, home to the AFC Ajax football team and a world-famous entertainment
venue.18 In another example, General Motors utilized five repurposed Chevrolet
Volt batteries in tandem with solar arrays and wind turbines, to power GM’s Enter-
prise Data Center in Milford, Michigan.19 Deployment in the charging infrastructure
is another option for repurposed EOL batteries and, to demonstrate this potential
application, Renault EOL EV batteries were installed on highways in Belgium and
Germany in August 2017.19

Recycling
Recycling is the third option, which can and must accommodate battery packs of all
designs and states of health. However, the multiplicity of material chemistries used
in today’s EV LIBs increases recycling complexity, presenting a few technical and
economic hurdles that must be addressed to enable efficient, large-scale automo-
tive battery recycling. First, LIB packs are complex structures, comprised of multiple
modules, in which numerous pouch, prismatic, or cylindrical cells are connected in a
variety of parallel-series configurations (welding, wire bonding, and mechanical
joining are common joining techniques used within LIB cells, modules, and packs).20
The respective architectures of LIB packs, modules, and cells vary significantly from
manufacturer to manufacturer. Within the cells, the chemical composition of active
materials also varies among manufacturers and continues to evolve. Cathode mate-
rials in xEVs can be any one of or a mixture of LiCoO2 (LCO), LiNixMnyCozO2 (NMC,
x + y + z = 1), LiFePO4 (LFP), LiMn2O4 (LMO), and LiNixCoyAlzO2 (NCA, x + y + z = 1),
and manufacturers are moving increasingly toward higher nickel and lower cobalt
chemistries, in response to cost and availability concerns. This leads to a weakening
of existing battery recycling business models, which depend largely on the recovery
of high-value cobalt.21 The cathode material represents the highest value in the LIB,
and, as such, recovering cathode as the final recycling process output is economi-
cally desirable. Of course, recycling more battery materials such as the anode, foils,
and electrolyte further augments recycling process margins, thereby enhancing the
sustainability of the recycling ecosystem.

2626 Joule 3, 2622–2646, November 20, 2019

Recycling has been successfully implemented for EOL lead-acid and nickel-metal
hydride (NiMH) batteries. For example, the recycling rates of lead-acid batteries
in both the United States and Europe approach 100%. The collection is ensured
via a value-driven model, which does not yet exist for LIB technology. Recycling
rates of small-format LIBs (in the consumer electronics industry) have been re-
ported as low, suffering from low collection rates. As noted, LIB technology faces
more recycling-related challenges than its lead-acid or NiMH predecessors. First,
at least five different cathode chemistries are being widely used in commercial
LIBs, with many EV batteries also using mixed cathodes (a mixture of two or three
cathode materials in a single cell). The vast research efforts presently directed at
cathode materials are certain to produce an even more variable supply chain for
recyclers to process. Because the supply chain for recyclers fluctuates significantly
and includes LIBs with many different cathode (and other) materials, if a recycler
cannot recover pure and consistent material, the recoverable value will be low
and inconsistent. Since cathode materials account for 40% of the material value
in typical LIBs, recycling the cathode materials is especially important for optimal
economics. The three different battery recycling technologies are shown in Fig-
ure 2: (a) pyrometallurgical processes, (b) hydrometallurgical processes, and (c)
direct recycling processes. The first two methods are established and starting to
operate at industrial scales, and the third is presently at the lab and pilot scale.
Novel approaches in all three categories are the subject of extensive development
in industry and academia.

The Pyrometallurgical Process. The pyrometallurgical process is a high-temper-

ature smelting process, which usually involves two steps.22 First, LIBs are
burned in a smelter, where compounds are broken down and organic materials,
such as plastic and the separator, are burned away. Then, new alloys are gener-
ated through carbon reduction.23 In the subsequent steps (often hydrometallur-
gical), metal alloys are further separated to recover pure materials. In this pro-
cess, only expensive metals (cobalt (Co), nickel (Ni), and copper (Cu)) are
recovered with the greatest efficiency. The anode, electrolyte, and plastics
are oxidized and supply energy for the process. Lithium is entrained in the
slag fraction and can be recovered with added processing (which comes with
associated cost and energy), and lithium’s recent increase in value has made
its recovery feasible for some recyclers. Aluminum serves as a reductant in
the furnace and decreases the need for fuel. Pyrometallurgical processes have
generated relatively successful business models to date, due to the high cobalt
content of LIBs that are used in portable electronics. However, as EV batteries
trend toward lower cobalt content, the business models will become less attrac-
tive. The main advantages of pyrometallurgical processes are (1) a simple and
mature process, (2) that sorting and size reduction are not necessary—a mixture
of LIBs and NiMH batteries can be recycled—and (3) that the output consists of
basic, elemental ‘‘building blocks’’ that can be used in synthesizing new cath-
ode materials of many different chemistries. The main disadvantages are (1)
CO2 generation and high energy consumption during the smelting process;
(2) that the alloy requires further processing, which increases the total recycling
cost; (3) that many of the materials in LIBs are not recovered (e.g., plastics,
graphite, and aluminum)—the process recovers Co and Ni from the cathode
materials and Cu from the anode current collector, which only account for
30 wt % in LIBs for electronics—and (4) that the business model may not
work well for EV batteries, due to the low Co concentration. In addition, the
industry is moving toward reduced cobalt or, ultimately, cobalt-free cathode
materials.

Joule 3, 2622–2646, November 20, 2019 2627

Figure 2. Different Recycling Technologies
Currently there are three major LIB-recycling processes including pyrometallurgy,
hydrometallurgy, and direct recycling. Pyrometallurgical process is a high-temperature smelting
process, which usually involves burning and subsequent separation. Hydrometallurgical process is
achieved using aqueous chemistry, via leaching in acids (or bases) and subsequent concentration
and purification. Direct recycling directly harvests and recovers active materials of LIBs, while
retaining their original compound structure. Pyrometallurgy and hydrometallurgy are being
operated at industrial level, and direct recycling is at lab and pilot scale.

Recent Progress: Pyrometallurgical processes prevail widely in industry because of

their simplicity and high productivity; some of the technical advancements are
shown in Table 1. In general, slag systems can be designed to optimize recovery ef-
ficiencies of metals in LIBs during the smelting reduction processes. CaO-SiO2-
Al2O3 and FeO-SiO2-Al2O3 were primarily employed as slag systems in pyrometal-
lurgical processes, whereas the recovery of manganese and lithium was low.22
Lately, Ren et al. adopted a novel slag system (MnO-SiO2-Al2O3) and preferentially
recovered manganese and lithium. Co-Ni-Cu-Fe alloy and lithium-containing man-
ganese-rich slag were produced, and with the further leaching of the manganese-
rich slag, the recovery rates of Mn and Li reached 79.86% and 94.85%.24 Lithium

2628 Joule 3, 2622–2646, November 20, 2019

Table 1. Technical Advancements in Pyrometallurgical Recycling Processes in Recent Literature
Pyrometallurgical Process Product and Efficiency Significance
Slag system: MnO-SiO2- Co-Ni-Cu-Fe alloy and Preferential recovery of Mn
Al2O3; Smelting condition: lithium-containing Mn-rich and Li based on the novel
1,475 C, 30 min slag; Recovery efficiencies of slag system24
Co, Ni, and Cu: 99.79%,
99.30%, and 99.30%;
Leaching efficiencies of Mn
and Li: 79.86% and 94.85%
Simulated slag: SiO2-CaO- LiCl; Recovery efficiencies Innovative method to
Al2O3-Li2O; Chlorination of Li from slag: 97.45% recycle lithium from slag
roasting condition: 1,000 C, pyrometallurgically25
90 min
Oxygen-free roasting: Co, Li2CO3, C; Recovery In-situ recycling of cobalt,
1,000 C, 30 min; Wet efficiencies of Co, Li, and Li2CO3, and graphite in
magnetic separation graphite: 95.72%, 98.93%, LCO/C battery system26
and 91.05%
973 K, 30 min; Vacuum Li2CO3; Recovery efficiency In-situ recycling of Li2CO3
condition (<1 kPa) and purity of Li: 81.90% from spent LCO/LMO/
and 99.7% NMC27
Oxygen-free roasting: Li2CO3 and Mn3O4; In-situ recycling of Li2CO3
1,073 K, 45 min Recovery efficiency of Li: and Mn3O4 in LMO/C
91.30%; Purity of Mn: battery system28
95.11%
Reduction roasting: 650 C, Li2CO3, NiSO4, CoSO4, and A simple and efficient
3 h, 19.9% carbon dosage; MnSO4; Water leaching reduction-roasting process
Carbonated water Leaching efficiency of Li: 84.7%; Acid to recover a NMC/C
and acid leaching leaching efficiency of Ni, Mn, battery system29
and Co: >99%

exists in slag as compound and is hard to be recycled by pyrometallurgy, due to its

high melting and boiling point. Recently, Dang et al. proposed to recover lithium
from slag by evaporation during chlorination roasting, and they found the best chlo-
rine donor, donor dosage, roasting temperature, and time by experimenting on the
simulated slag, resulting in a lithium recovery efficiency of 97.45%.25

In-situ reduction roasting attracts significant research interest and is being studied
in the laboratory. The ‘‘in situ’’ means that no other additives are needed in this
process, and spent batteries can be directly transformed into useful goods via pyrol-
ysis.26–28 Spent battery systems whose cathode is LiCoO2 and LiMn2O4 have been
tested through in-situ recovery.26,28 In the process of oxygen-free roasting, mixed
electrode materials were transformed to Li2CO3, metal and metal oxide without
any additives.26,28 Lithium is released from the oxygen framework within the elec-
trode crystal structure and converted to Li2CO3. Afterwards, Mao and Xiao provided
a theoretical analysis of in-situ recovery and developed a collapsing model, in which
graphite, having a stronger affinity to oxygen than lithium and cobalt, causes the
collapse of oxygen octahedrons and the transformation of Li to Li2CO3.27,30 They
found that burning graphite promoted the pyrolysis of lithium cobalt oxide, due
to the coupling reaction between them. Consequently, the decomposition temper-
ature of lithium cobalt oxide decreased from 1,436 to 1,173 K. The coupling reaction
and collapsing model explained the underlying principles of in-situ recovery, guid-
ing related development efforts in academia and industry.30

Industry Demonstrations: In industry Umicore utilizes the pyrometallurgical process

to recycle LIBs. With the use of an ultra-high temperature (UHT) method, Umicore
can handle 7,000 metric tons per year, and dangerous pretreatment can be elimi-
nated. The UHT process generates a high-value alloy (Co, Ni, and Cu) and slag for

Joule 3, 2622–2646, November 20, 2019 2629

construction additives. Further separation or purification steps involve hydrometal-
lurgical techniques (leaching, solvent extraction, and precipitation) to produce new
cathode materials, such as LCO and NMC. Previously, the lithium reportedly
existed in the slag, which is used largely for construction,22,31,32 but recently, Umi-
core has demonstrated that, with further processing, the slag from LIBs can be inte-
grated into standard Li-recovery flowsheets, through cooperation with external
partners.33

Accurec utilizes vacuum thermal recycling (VTR) to treat LIBs, although VTR was
originally developed for precious metal recovery. The combined pyrometallurgical
and hydrometallurgical process (EcoBatRec) was finalized in 2016. Spent LIBs are
firstly treated mechanically (disassembly) to remove electronic fractions and plastic
covers, and then VTR (distillation and pyrolysis) is performed to extract the
electrolyte condensate. After crushing, classification, and sorting, Al, Cu, and steel
are recovered by sieving, magnetic separation, and air separation, while the
electrode materials are agglomerated to pellets with binder and converted into a
Co-based alloy by smelting.21,22,31,34–36 Lithium-containing slag (also produced in
this process) can be leached out by acid and converted to lithium carbonate or
chloride.31

Sony and Sumitomo in Japan recycle spent LIBs using a combined pyrometallurgical
and hydrometallurgical processes. At the Sony plant, during a calcination at
1,000 C, plastics and electrolyte are burned off, leaving metallic parts and active
materials. Fe, Cu, and Al can be separated magnetically, while active materials are
sent to Sumitomo for further hydrometallurgical recycling, where cobalt is recovered
as cobalt oxide. The recovered cobalt oxide has high purity and can be used for the
fabrication of new cathode materials.31,34,35,37 Recently, Sumitomo announced its
first practical method to recover copper by pyrometallurgy and nickel by hydromet-
allurgy.38,39 With the utilization of this processing flow, more value is extracted from
spent LIBs, and the depletion of resources is further addressed.

The pyrometallurgical processes of Inmetco and Glencore (formerly Xstrata Nickel)

were not originally designed for LIBs, and consequently some of the materials,
including lithium, are not recovered. Inmetco utilizes a direct-reduced iron
process to treat LIB waste, and the recovered Co, Ni, and Fe are used for the produc-
tion of an iron-based alloy.22,31,37,40 Glencore processes batteries as secondary
feedstock in the extractive routes of Co, Ni, and Cu. With an added
hydrometallurgical process, valued metals such as nickel, cobalt, and copper are
recovered.21,22,31,35,37,41

The Hydrometallurgical Process. In this process, material recovery is achieved us-

ing aqueous chemistry, via leaching in acids (or bases) and subsequent concentra-
tion and purification. For LIBs, ions in solution are separated with various technolo-
gies (ion exchange, solvent extraction, chemical precipitation, electrolysis, etc.) and
precipitated as different compounds.42 The main advantages of the hydrometallur-
gical process are (1) that high purity materials can be generated, (2) that most LIB
constituents can be recovered, (3) low temperature operation, and (4) lower CO2
emissions as compared with the pyrometallurgical process.43 The main disadvan-
tages of the hydrometallurgical processes include: (1) a need for sorting, which re-
quires increased storage space and adds to process cost and complexity; (2) the
challenge of separating some elements (Co, Ni, Mn, Fe, Cu, and Al) in the solution,
due to their similar properties, which can lead to higher costs; and (3) the expense of
waste water treatment and associated costs.

2630 Joule 3, 2622–2646, November 20, 2019

Recent Progress: Some technical hydrometallurgical improvements regarding
leaching, solvent extraction, chemical precipitation, and sol-gel, reported in recent
literatures, are listed in Table 2.

Leaching: Leaching dissolves the metals present in EOL LIBs, and the subsequent
leachate undergoes further treatment to separate metal ions and produce final
products.

Alkali Leaching: Alkali leaching has attracted attention due to its selective leaching
and the resulting potential to avoid costly separation or purification steps. An
ammonia-based system is used because it can form stable ammonia complexes
with metals, such as Ni, Co, and Cu. Zheng and Chen utilized ammonia and/or
ammonium sulfate as a leaching solution and sulphites as the reducing agent. The
overall leaching efficiencies of Ni, Co, and Li were high in both studies and are
summarized in Table 2; Mn showed different leaching behavior.44,45 Chen found
that the leaching efficiency of Mn was largely dependent on the concentration of
(NH4)2SO3, with an optimal concentration of 0.75M.45

Acid Leaching: Acid leaching remains prevalent because of its high recovery
efficiency. With the use of acid in leaching, strong inorganic leaching may cause sec-
ondary pollution (excess acid solution and hazardous gas emission), while organic
leaching offers similar leaching efficiency with biodegradable properties. Acid
leaching agents include HCl, H2SO4, and HNO3, and organic leaching agents consist
of citric acid, ascorbic acid, oxalic acid, and formic acid.

Barik and He obtained a leaching efficiency of over 99% by utilizing dense HCl and
H2SO4-H2O2 systems, respectively, when dissolving Co, Mn, and Li. Manganese was
further separated by adding sodium hypochlorite in Barik’s work.46,47 Instead of
using excess acid, Li et al. recovered LiFePO4 in a low-concentration leaching
solution of sulfuric acid and hydrogen peroxide. After operating at 60 C for 2 h,
96.85% Li, 0.027% Fe, and 1.95% P were recovered in the leachate. Subsequently,
95.56% Li was recycled as Li3PO4 with the addition of Na3PO4, and the leaching
residue was recovered as FePO4, through burning off the carbon slag.48 The
reduced usage of inorganic acid in the process leads to a simultaneous decrease
in the amount of secondary waste and overall cost.

Organic acid leaching can reach efficiencies similar to inorganic acid leaching, in
milder environments. Gao et al. introduced formic acid into their closed-loop recy-
cling process to selectively leach lithium ions into solution while precipitating other
metals out for precursor production.49 In this process, Li2CO3 was obtained with
a purity of 99.9%, after removing metal residues.49 Zhang et al. developed an inno-
vative method to recycle NMC by oxalic acid leaching. Lithium was dissolved in the
solution, whereas Ni, Mn, and Co were precipitated as oxalate. Unlike LCO systems,
where the metal oxide can be fully leached out,50,65 the layered NMC structure
still exists after 2 h of leaching with oxalic acid. This occurs because reacted NMC
oxalate precipitate covers the surface of NMC and hinders a continuous reaction,
and the degree of leaching can be controlled by changing the leaching time. Subse-
quent calcination with Li2CO3 transformed oxalate precipitates into regenerated
NMC, which showed excellent electrochemical performance. At 0.2 C, the initial
specific discharge capacity was 168 mAh/g and was better than that in reported
recycled materials (155 mAh/g).61,66,67 The specific capacity was 153.7 mAh/g after
150 cycles, demonstrating a capacity retention of 91.5%. The promising behavior is

Joule 3, 2622–2646, November 20, 2019 2631

Table 2. Technical Advancements in Hydrometallurgical Recycling Processes in Recent Literature
Hydrometallurgical Experiment Condition and Efficiency Significance
Process
Leaching Alkali leaching: NH3-(NH4)2SO4-Na2SO3; Leaching efficiencies Strong selective leaching, in which metal separation (Mn from
of Ni, Co, Mn, and Li: 94.8%, 88.4%, 6.34%, and 96.7% others) is achieved44
Alkali leaching: (NH4)2SO4-(NH4)2SO3; Leaching efficiencies of High leaching efficiencies of metals; adjustable leaching
Ni, Co, Mn, and Li: 98%, 81%, 92%, and 98% behavior of Mn45
Inorganic acid leaching: HCl; Leaching efficiencies of Co, Mn, A successful transition demonstration from lab to pilot scale46
and Li in lab scale: 98%, 99%, and 99.2%; Leaching efficiencies
of Co and Mn in pilot scale: 95% and 90%
Inorganic acid leaching: H2SO4-H2O2; Leaching efficiencies of Reveals that leaching mechanism of having surface chemical
Ni, Co, Mn, and Li: 99.7% reaction as a limiting step47
Inorganic acid leaching: H2SO4-H2O2; Leaching efficiencies of Reduced usage of acid leads to a highly selective leaching and
Li, Fe, and P: 96.85%, 0.027%, and 1.95% effective metal separation48
Organic acid leaching: formic acid-H2O2; Leaching efficiency Selective leaching of Li and separation of metals (Li versus
of Li: 99.93% transition metals)49
Organic acid leaching: oxalic acid; Leaching efficiency of A simple leaching and filtering process to separate and
Li: 98% recover Li and Co from with high efficiency50
Organic acid leaching: oxalic acid; Leaching efficiency of Partial leaching introduces voids of cathode particles and
Li: 81% helps the electrochemical performance of the resynthesized
cathode51
Bioleaching: Aspergillus niger; Leaching efficiencies of Cu, Li, Enhanced and optimized recycling process with the utilization
Mn, Al, Co, and Ni: 100%, 100%, 77%, 75%, 64%, and 54% of Aspergillus niger52
Bioleaching: Aspergillus niger; Leaching efficiencies of Cu, Li, Citric acid is more effective in leaching behavior, when
Mn, Al, Co, and Ni: 100%, 95%, 70%, 65%, 45%, and 38% compared with other organic acid53
Solvent Extraction Extractants: D2EHPA and PC-88A; Purity of cobalt oxalate: Cobalt of high purity is recycled54
99.5%
Extractants: Cyanex 272 with TOA as phase modifier; Purity of Battery-grade materials with high purity requirements are
Li raffinate, organic Co solution and aqueous NiSO4 solution: recovered55
99.9%, 99.6%, and 99.7%
Extractants: D2EHPA and Cyanex 272; Purity of cobalt Spent battery powder is gained from pilot-scale pretreatment;
carbonate: 95% feasibility of this process in industry is proven by the
complexity of the treated sample56
Chemical Precipitants: oxalic acid and H3PO4; Recovery efficiencies of An optimized recycling process that can efficiently recover Co
Precipitation Co and Li: 99% and 88% and Li57
Precipitants: Na2CO3 and Na3PO4; Recovery efficiencies of Li The removal of Na impurity in Li2CO3 can be avoided when
as Li2CO3 and Li3PO4: 74.72% and 92.21% fabricating LIS58
Precipitants: H3PO4; Recovery efficiencies of Fe and Li: 93.05% No secondary waste; a closed-loop recycling process59
and 82.55%
Precipitants: NaClO; Recovery efficiencies of Mn: 97.7% Selective separation of Mn from Co46
Precipitants: Na3PO4; Recovery efficiencies of Li: 95.56% The effective metal separation leads to an easy precipitation48
Co-precipitation Leaching agent: H2SO4-H2O2; Reagent for the co-extraction of Transition metals are co-extracted and co-precipitated;
Ni, Mn and Co: D2EHPA in kerosene; Discharge capacity of electrochemical performance of recycled cathode is
NMC 111 at 0.5C (2.7–4.3V): 150 mAh/g comparable to a pristine cathode60
Leaching agent: H2SO4-H2O2; Extractant for impurities: Low secondary waste and closed-loop recycling process; a
copper extractant and phosphate ester; Discharge capacity of mixture of spent cathode materials are treated61
NMC 111 at 0.1C (2.7–4.3V): 150.6 mAh/g
Sol-Gel Leaching and chelating agent: citric acid; Leaching efficiency Better electrochemical performance than pristine material,
of Li, Ni, Co, and Mn: 99.1%, 98.7%, 99.8%, and 95.2%; due to the stabilization of Al impurity62
Discharge capacity of NMC 111 at 0.2C (2.8–4.3V): 152.8
mAh/g
Leaching and chelating agent: lactic acid; Leaching efficiency Better rate and cycle performance than freshly synthesized
of Li, Ni, Co, and Mn: 97.7%, 98.2%, 98.9%, and 98.4%; 96% cathode; lactic acid is proven to be an effective chelating
capacity retention after 100 cycles at 0.5C agent for sol-gel method63
Leaching and chelating agent: malic acid; Discharge capacity Significant enhancement compared with spent material;
of NMC 111 at 0.2C (2.75–4.25V): 147.2 mAh/g; 95.06% satisfactory electrochemical performance64
capacity retention after 100 cycles at 0.5C

2632 Joule 3, 2622–2646, November 20, 2019

attributed to the creation of submicron-sized particles as well as voids formed
during the regeneration.51

Bioleaching: Bioleaching is another environmental-friendly method, and it utilizes

the acid produced during metabolization of the microorganism to leach spent bat-
teries. Generally, bacteria form inorganic acid, while fungi form organic acid.
However, bioleaching has the drawback of a long culturing time and the susceptibil-
ity to contamination. Bahaloo-Horeh et al. utilized a bio-hydrometallurgical route to
leach spent LIBs, in which Aspergillus niger was cultured. With a pulp density of 2%
(w/v), 100% Cu and Li, 77% Mn, and 75% Al were recovered, while 64% Co and 54%
Ni could be recycled at another experiment setting, with 1% (w/v) pulp density.52
This team also stated that citric acid played a more significant role in bioleaching
than other organic acid produced by Aspergillus niger.53

The efficiency of the leaching process is enhanced by reducing agents since lower
valence metals dissolve more readily. The reducing agents include inorganic and
organic species and metallic current collectors (Cu, Al); the most commonly used
one is hydrogen peroxide. Following leaching, treatment options to separate metals
or remove impurities include solvent extraction, chemical precipitation, electrolysis,
and ion exchange.

Solvent Extraction: The driving mechanism of solvent extraction is the different

solubilities of various metal ions in an organic solvent versus an aqueous liquid.
This approach has the advantage of short reaction time (around 30 min) and high
purity yield of products, but its application is limited by the high cost of solvents
and process complexity. To recover the cobalt from spent batteries, Wang et al.
used D2EHPA (di-(2-ethylhexyl) phosphoric acid) and PC-88A (2-ethylhexylphos-
phonic acid mono-2-ethylhexyl ester) to perform the extraction. First, D2EHPA
was employed to remove Cu and Mn, then cobalt and nickel were separated by
PC-88A. Finally, cobalt was recycled as cobalt oxalate, with a purity of 99.5%.54
Virolainen et al. separated Li, Ni, and Co successfully from spent battery leachate
by extractant-Cyanex 272 (Bis(2,4,4-trimethylpentyl)phosphinic acid). Modified
Cyanex 272 by TOA (trioctylamine, a phase modifier), which helps to abate the for-
mation of unwanted organic phases, was utilized to obtain a Li raffinate, whose purity
was 99.9%. With subsequent scrubbing and stripping, a 99.7% Ni aqueous solution
and a 99.6% Co organic solution were recovered.55

Chemical Precipitation: Similar to solvent extraction, chemical reactions can be used

to separate metals or remove impurities, and these have the ability to precipitate out
diverse metals by strategic tuning of pH numbers. Pinna et al. dissolved Co and Li,
using a leaching solution of H3PO4 and H2O2. Then, by adding oxalic acid and
NaOH, Co was precipitated out as CoC2O4, with an efficiency of 88%, and Li was
recovered as Li3PO4, at an efficiency of 99%.57 A lithium ion-sieve (LIS) can selectively
absorb lithium with a high capacity and is generally employed in lithium extraction
from brine, groundwater, and seawater. Lithium manganese oxide is a good candi-
date material as a LIS. As demonstrated by Guo et al., recycled Li2CO3 can be sin-
tered with MnCO3 to fabricate LMO for usage as a LIS. The content of Na2CO3
impurity in raw Li2CO3 was controlled below 10%, and the Na-doped LMO LIS
was shown to be able to resist the Mn corrosion to a level of 21.07% while maintain-
ing a satisfactory absorption capacity of 40.08 mg/g.58

Co-precipitation: Notably, Ni, Mn, and Co share similar properties and thus require
complex steps to separate them. An effective approach is to coprecipitate them

Joule 3, 2622–2646, November 20, 2019 2633

together and sinter the precursor directly into NMC cathode material. Yang et al.
accomplished this goal via the co-extraction and co-precipitation paths and success-
fully fabricated recycled NMC 111 with good performance. First, a three-stage
extraction with an extractant of D2EHPA in kerosene was employed, and 100%
Mn, 99% Co, and 85% Ni were co-extracted. Separated Li raffinate was treated
with Na2CO3, and a purity of 99.2% Li2CO3 was obtained. Next, transition metals
were stripped with 0.5M H2SO4, and Ni1/3Mn1/3Co1/3(OH)2 was produced in a co-
precipitation reaction. Lastly, recycled NMC 111 was created through calcination
of the mixture of Li2CO3 and metal hydroxide. Co-extraction and co-precipitation
demonstrate a promising path, in which tedious and costly separation steps are
obviated, and a high-quality cathode material is produced.60 A closed-loop LIB
recycling process developed by Worcester Polytechnic Institute (WPI) shared the
same principle of co-precipitation.66,68–72 A hydrometallurgical process is imple-
mented, and different cathode materials are dissolved in the leaching solution.
Then, impurities in the leachate, including Cu, Fe, and Al, are removed through a
series of pH adjustments, leaving the Ni, Mn, Co metal ions. Next, the ratio of Ni,
Mn, Co is tailored to the desired ratio, by adding virgin metal sulfates as needed.
Subsequently, the adjusted metal sulfate solution undergoes the co-precipitation
reaction, and NMC hydroxide precursor powder is produced. After calcination
with recovered lithium carbonate, recovered NMC cathode power is ready for use
in ‘‘new’’ batteries, enabling a closed-loop approach. The group has demonstrated
that the recovered NMC 111 has similar or better electrochemical properties than
the commercial control powder with both coin cells and pouch cells, which have
been independently tested by A123 Systems and Argonne National Laboratory.

Sol-Gel: Sol-gel synthesis is another approach to synthesize cathode material while

avoiding separation steps, and it is generally operated after the ratio of metal ions
has been adjusted to the desired number. Initially, metal ions are homogeneously
distributed in sol states. Then, by hydrolyzing the mixture of precursors, the sol
gradually transforms into a gel state. The generation of final solid cathode powder
requires a drying step, to remove any remaining solvent, and an additional sinter-
ing step. Li et al. treated spent mixed cathode batteries with citric acid and
hydrogen peroxide. Then, recycled NMC 111 was synthesized from leachate, via
the sol-gel process, in which citric acid was the chelating agent. For comparison,
virgin NMC 111 was also synthesized by the same sol-gel method but with pure
materials. Recycled cathode outperformed the virgin material in cell tests, and it
was speculated that this was because trace amounts of Al performed a doping
function, which was conducive to stabilizing the structure during the insertion
and extraction of Li.62 This same group also experimented by using the sol-gel
method with lactic acid, and the capacity retention of recycled NMC 111 was
96% after 100 cycles at 0.5C.63

For most cathode materials, hydrometallurgical recycling processes are economi-

cally viable, particularly for cathodes high in cobalt and nickel. For this reason, LFP
and LMO pose a challenge for traditional business purposes, due to the low intrinsic
value of the cathode material components (Fe and Mn).73

Industry Demonstrations: In North America, Retriev uses a hydrometallurgical pro-

cess to recycle LIBs. After the battery packs come in, they are manually dismantled,
to the module or cell level, then fed into a flooded hammer-mill (immersed in lithium
brine) for crushing, so as to lower the reactivity of the batteries, neutralize the elec-
trolyte, and prevent gas emissions.22,32,35–37,43,74–76 The Retriev process produces
three streams of materials: metal solid, metal-enriched liquid, and plastic fluff. The

2634 Joule 3, 2622–2646, November 20, 2019

metal solid may contain black mass, Cu and Al foils, and the metal-enriched liquid
primarily includes lithium-ion, which is precipitated and filtered.77 The filter cake
and metal solid are sold to down-stream smelters (Glencore) that are interested in
the cobalt or nickel content. Plastics can be directly recycled or disposed. Here,
lithium can be recycled as lithium carbonate.21,22,31,34–36,40,43,74–76,78–80

Batrec Industrie AG employs a hydrometallurgical process to recycle LIBs. The used

batteries are sorted and crushed in a CO2 atmosphere, and the released lithium is
then neutralized by moist air. Following crushing and neutralization, the protective
CO2 gas is purified in a gas scrubber before being exhausted. The remaining scrap
materials are processed in acidified aqueous liquid, and the resultant leaching liquor
and solid fraction are separated for further purification.21,31,34

Recupyl’s hydrometallurgical process for LIB recycling, named Valibat, consists of a

mechanical treatment of spent batteries, implemented under an inert gas mixture
(CO2), and the physical separation of steel, copper, and plastics. Subsequent
leaching of the fine powders yields an alkali solution of lithium, mixed metal oxides,
and carbon. Lithium is precipitated out as Li2CO3 or Li3PO4, and metal oxides
undergo a second leaching. After the Cu and other impurities are removed, NaClO
is added in order to precipitate cobalt as cobalt (III) hydroxide.34

The LithoRec project, funded by the German Federal Ministry of Environment, aimed
to develop an economically viable and ecological beneficial recycling process with
high recycling rates. Active materials that separated in the recycling stream are
sent to Albemarle Germany GmbH (Rockwood Lithium GmbH) for hydrometallurgi-
cal treatment, and the recovered lithium and transition metal salts can be used for
the synthesis of new cathode material.37,75,76,81

The hydrometallurgical process is also primarily deployed in China. As a leading

battery recycling enterprise, Brunp processes spent LIBs by acid leaching (sulfuric
acid and hydrogen peroxide), and the produced metal hydroxides can be utilized
for cathode fabrication.31,82–85 Other major LIB recyclers (GEM, GHTECH, TES-AMM
China, and Highpower International) also adopted a similar route to recycle LIBs.

SungEel HiTech is a hydrometallurgical recycling facility located in South Korea and

offers the capability of recovering Ni, Mn, Co, Li, and Cu from spent LIBs. The recov-
ered materials (metal sulfate and lithium phosphate) are supplied to LIB manufac-
turers to synthesize new batteries.86

Battery Resourcers, located in Worcester, Massachusetts, has developed a closed-

loop process to recycle LIBs. Here, a hydrometallurgical process is utilized to
dissolve the cathode powder. The leaching solution is used to synthesize different
LiNixMnyCozO2 (NMC). SMCC and American Manganese are also actively devel-
oping a hydrometallurgical process in order to recycle LIBs.

The Direct Recycling Process. Direct recycling is a recovery method proposed to

directly harvest and recover active materials of LIBs, while retaining their original
compound structure.87,88 In this process, battery constituents are separated, primar-
ily using physical separation methods, magnetic separation, and a moderate thermal
processing, in order to avoid chemical breakdown of the active materials, which are
the main recovery ‘‘target’’. The active materials are purified, and both surface and
bulk defects are repaired by re-lithiation or hydrothermal processes. However, cath-
odes may be a mixture of more than one active materials, and separating them may

Joule 3, 2622–2646, November 20, 2019 2635

Table 3. Technical Advancements in Direct Recycling Processes in Recent Literature
Direct Recycling Process Performance Significance
Hydrothermal: 220 C 4 h; LiCoO2; 91.2% capacity A nondestructive and simple
Short annealing: 800 C 4 h retention after 100 cycles at 1C renovation process; mixed
(3–4.3V); 141.9 mAh/g at 2C cathode can be processed
and 130.3 mAh/g at 5C together87
Hydrothermal: 220 C 4 h; NMC 111: First-discharge Cathode with higher nickel
Short annealing: 850 C 4 h capacity of 158.4 mAh/g at 1C content is more sensitive to
in O2 and 122.6 mAh/g after 100 oxygen partial pressure during
cycles; NMC 532: 128.3 mAh/g solid state regeneration88
after 100 cycles
Solid phase sintering: LiFePO4; 144 mAh/g at 0.1C Simple regeneration process;
700 C 8 h; Doping ratio (2.5–4.1V); 135 mAh/g after satisfactory electrochemical
between spent LFP 100 cycles performance89
with new LFP: 3:7
Solid phase heat treatment: LiFePO4; First-discharge A green recycling process
650 C 1 h under Ar/H2 flow; capacity of 147.3 mAh/g offering high yields; impurity
Li2CO3 as lithium source (2.5–4.2V); 140.4 mAh/g phases are fully converted90
after 100 cycles at 0.2C and
capacity retention is 95.32%
Solid phase sintering: LiCoO2; First-discharge A high total recovery rate of
850 C; Li2CO3 as lithium capacity of 150.3 mAh/g 95.78%; undesired phases are
source (3.0–4.3V) at 0.1C; converted back to layer
140.1 mAh/g after 100 structure; Al and Cu impurities
cycles favor electrochemical
performances91
Electrochemical: cycle LiFePO4; 150–155 mAh/g An innovative electrochemical
spent cathode coating method to regenerate the
with pure lithium metal; cathode; decrease of 50%
Chemical: immerse spent embodied energy, compared
cathode power in lithium with virgin material
containing solution production92
Hydrothermal: 80 C 6 h; LiCoO2; First-discharge capacity Ultrasonic radiation is used
Ultrasonic power: 600W of 133.5 mAh/g; 99.5% capacity to facilitate the renovation
retention after 40 cycles process93

not be economically or technically feasible. Furthermore, inputs containing multiple

NMC chemistries cannot yet be separated and thus present significant sorting chal-
lenges. The main advantages of the direct recycling approach include: (1) a relatively
simple process, (2) that active materials could be directly reused after regeneration,
and (3) significantly lower emissions and less secondary pollution, in comparison
with pyrometallurgy and hydrometallurgy.43 The main disadvantages of the direct
recycling process include: (1) that it requires a rigorous sorting/pre-processing,
based on exact active material chemistry; (2) that it is a challenge to guarantee
consistent high purity and pristine crystal structure, which may not meet rigorous
standards required by the battery industry; (3) an unproven technology that, thus
far, exists only at lab scale; (4) significant sensitivity to input stream variations; and
(5) an inflexible process: what goes in comes out, and thus the process may not be
appropriate to meet the reality of changing cathode chemistry (active materials
recovered at EOL will be ‘‘old technology’’ and may no longer be relevant). In the
near term, this technology is more likely to be adopted by battery manufacturers
for recycling electrode scrap, where the chemistry is known and current.

Recent Progress: Direct recycling processes can restore the structure of active mate-
rials directly, and some recent technical innovations are listed in Table 3. Capacity
degradation of spent LIBs is associated with lithium loss due to the thickening of
the solid-electrolyte interface (SEI) and undesired phase change.88 In earlier studies
of direct recycling, researchers principally focused on relithiation to regenerate

2636 Joule 3, 2622–2646, November 20, 2019

cathode materials. Solid-phase sintering with a lithium source is a versatile tool to
supplement deficiency. Song et al. doped spent LiFePO4 (LFP) materials with new
LFP, at a ratio of 3:7 and calcinated at 700 C. Results showed that the recycled
LFP offered a discharge capacity of 144 mAh/g (commercial LFP: 150 mAh/g).89
Li2CO3 can also be added and mixed with the spent cathode to compensate for
lithium loss. Li et al. regenerated spent LFP, by calcinating it with Li2CO3 for 1 h,
at 650 C. The end product delivered a high first-discharge capacity of 147.3 mAh/
g and kept a capacity retention of 95.32% after 100 cycles (commercial LFP require-
ment: >92.43%).90 A key challenge for the direct recycling approach relates to the
levels of impurities. While aluminum and copper have been shown to improve the
electrochemical performance of regenerated cathode material, there remains a
threshold impurity limit. Chen et al. verified this conclusion when regenerating Li-
CoO2 by direct recycling with solid-state sintering. With an Al content less than
0.4 wt %, or Cu content less than 0.6 wt %, the electrochemical reaction was not hin-
dered by impurities but, in fact, improved. With an optimal quantity of Li2CO3, fol-
lowed by a heat treatment at 850 C, the regenerated cathode displayed a good
discharge capacity of 150.3 mAh/g (commercial LCO: 150 mAh/g) and a capacity
retention of 93.2% after 100 cycles.91

In addition to the aforementioned solid-state sintering, relithiation can also be

achieved via hydrothermal, electrochemical, and chemical processes. Electrochem-
ical relithiation uses an electrochemical method to restore the cathode powder’s lost
lithium, whereas the chemical method involves soaking the cathode powder in a so-
lution with an excess lithium source, and the hydrothermal technique employs the
same steps as the chemical method but with added thermal treatments. Ganter
et al. evaluated the electrochemically and chemically regenerated LFP by SEM,
XRD, and electrochemical testing, finding that it exhibited identical performance
and characteristics as the new LFP. It can thus be said that both electrochemical
and chemical lithiation processes show promising results for future applications.92
Zhang et al. regenerated LiCoO2 hydrothermally, assisted by ultrasound. The re-
paired LCO had a discharge capacity of 133.5 mAh/g (theoretical capacity: 137
mAh/g for Li0.5CoO2) and approached the specifications of commercial cathodes.
Ultrasonic waves produce cavitation effects and thereby accelerate relithation.93 Hy-
drothermal lithiation can partially restore the structure of the cathode, and when fol-
lowed by an annealing process, the structure restoration is further enhanced. Shi
et al. also successfully regenerated spent LiCoO2 cathode by hydrothermal lithia-
tion, followed by short-duration annealing, which resulted in better crystallinity,
less cation disordering, and fewer defects. The hydrothermally renovated LCO
showed a discharge capacity of 153.1 mAh/g (commercial LCO: 150 mAh/g) at
0.1C and capacity retention of 91.2% at 1C after 100 cycles. This result was
compared with another LCO sample recovered by sole heat treatment (850 C, 12
h), and the hydrothermally repaired sample showed superior rate capability. Unlike
sole heat treatment, where the amount of added lithium sources must first be calcu-
lated by testing the level of lithium loss, the proposed hydrothermal method can
accommodate any degradation level of spent cathode materials, and the ratio of
Li to the delithiated cathode does not have to be tightly controlled.87 This group
also demonstrated its feasibility in direct regeneration of NMC cathode particles.
Degradation mechanisms related to cycled NMC cathode materials are complex,
compared with LCO, incurring more challenges during the regeneration process.
In addition to the lithium loss due to the solid-electrolyte interphase (SEI) formation,
spinel and rock salt phase changes also exacerbate this capacity loss. Shi et al. used a
hydrothermal treatment, followed by a short annealing, and the recovered NMC
cathode was converted back to a layered structure. The rejuvenated NMC cathode

Joule 3, 2622–2646, November 20, 2019 2637

exhibited good electrochemical performances, approaching pristine materials, with
NMC 111 showing a capacity of 158.4 mAh/g in the first cycle, at 1C, and 122.6 mAh/
g after 100 cycles; concurrently, NMC 532 maintained a capacity of 128.3 mAh/g af-
ter 100 cycles. In contrast with NMC 111, solid-state regeneration of NMC 532 was
more sensitive to oxygen partial pressure and cannot fully recover the desired micro-
phases/layer structure of NMC 532 in air.88

Industry Demonstrations: Because of the low intrinsic value of LFP, it is not econom-
ically feasible to recycle LFP by hydrometallurgical methods. In industry, utilizing
direct recycling to recover LFP can be potentially profitable, as claimed by BYD in
China.73 OnTo Technology is located in Bend, Oregon, and recycles LIBs via a
direct-recycle methodology at bench scale. EOL LIBs are discharged and opened
to harvest the electrode, after which the cathode material is gained by blending
the electrode in an aqueous alkaline solution and detaching it from the current col-
lector. With the utilization of hydrothermal and additional heat treatment, the
degraded cathode material can be regenerated and used in new cells.94 The com-
pany claims that its recycling process is economically viable and has started working
with a US-based EV manufacturer. OnTo Technology also recycles electrolyte, using
liquid CO2, either by circulating CO2 or soaking spent batteries in supercritical fluid.
After discharging and shredding, 90% of the electrolyte is extracted in 48 h.34,95
However, this electrolyte recycling process is not practically adopted, due to its
intrinsic high cost. Farasis, a lithium-ionbattery manufacturer, has also been devel-
oping a direct recycling process to recycle LIBs under a USABC contract and has
claimed some success in its report included in the Department of Energy Annual
Merit Review Report.

Summary, Challenges, and Future Outlook

The EV LIB market is expected to grow to over $90B USD by 2026.96 The rapid, ever-
increasing adoption rates of EVs pose a concern for the materials supply chain, as
evidenced by the fluctuating price of raw materials, especially lithium and cobalt.
There is no doubt that LIB recycling will play an important role in strategic materials
supply. The US Department of Energy (DOE) has identified LIB recycling as a critical
need, to enable long-term material availability and to stabilize the LIB supply chain.
In fact, recycling is viewed as a lever that has the potential to decrease future battery
costs and energy use, alleviate pristine material prices, and reduce reliance on im-
ported materials. The DOE recently announced the establishment of a Lithium Ion
Recycling Center, ReCell, which will house a multi-institution effort led by Argonne
National Laboratory. The objective of the center is to develop a closed-loop recy-
cling R&D process, focused on novel materials and processes, in order to improve
the economic viability of battery recycling.

As described above, pyrometallurgical, hydrometallurgical, and direct recycling

processes each have their respective advantages and disadvantages. Both pyromet-
allurgical and hydrometallurgical processes have been commercialized, and their
business models depend largely on the high cobalt concentration of LIBs for
portable electronics. However, these business models may become increasingly
challenging for EV batteries, as they trend toward lower and lower cobalt content.
Direct recycling processes remain at the lab-scale level and require further develop-
ment in order to generate a meaningful impact. As such, the need for flexible pro-
cessing techniques to extract as much material value as possible from current, and
future generations of batteries is critical to the sustainability of EVs. Unfortunately,
none of the above recycling processes presently provides an economical solution
to the very dynamic input streams of current and future LIBs, and better recycling

2638 Joule 3, 2622–2646, November 20, 2019

technologies are needed. It is widely accepted that a value-based ‘‘pull system,’’
whereby extracted value exceeds recycling costs, is the necessary engine for effi-
cient collection and, in turn, sustainable closed-loop recycling.

Although various battery recycling technologies are available today, as yet none of
them offer the perfect solution, and continued efforts are needed. LIBs recycling
research must keep pace with rapidly evolving LIB materials research, which is
bringing new materials and designs to the market. This requires LIB recycling tech-
nologies that are flexible, economically feasible, robust, and which offer high recy-
cling efficiencies. The authors see the following research needs and challenges for
various recycling processes. Note: different recycling processes may have the
same or similar research needs.

1. Sorting and separation technologies: The spent LIBs most likely include vari-
ations in shape, size, and chemistry. Sorting and separation technologies
could increase the efficiency of recycling.
A. LIBs separation, based on different chemistries. Recycling facilities nor-
mally receive EOL LIBs without knowing the interior chemical constituents.
Proper labeling of LIBs by battery manufacturers would help the separation
of LIBs, based on chemistry. Then, single-chemistry LIBs can be sorted and
recycled, which is more effective and efficient. For example, the Society of
Automotive Engineers (SAE) has developed labeling standards (J2936) for
LIBs. This standard gives labeling recommendations for energy storage de-
vices, including cell, battery, and pack-level products during the entire life
spectrum.
B. Material separation. Various chemistries and form factors of spent LIBs
make the pretreatment of EOL LIBs challenging. Safe and effective separa-
tion of battery components needs to be developed. For example, if cell
size and shape are standardized to a few designs, auto-dismantling and
separation become more feasible.
2. The Pyrometallurgical process: The pyrometallurgical process is the most
mature technology and has been primarily deployed in Europe and North
America.
A. Slag recycle. During the smelting process, most of the materials (graphite,
separator, organic electrolyte, plastics) are burned and not recovered.
Slag, including lithium, is produced. In most traditional pyrometallurgical
processes, the lithium and aluminum in slag is not recovered. However,
the gradually increasing price of lithium renders this unsustainable; the
lithium must be recovered or not be sent to slag. Developing practical
technologies to recover lithium in the slag could be one of the important
research directions for the pyrometallurgical process.
B. Adaptation to the rapidly developing LIB industry (high nickel and low co-
balt). The LIB industry is evolving very quickly. Trends are moving toward
increasingly higher nickel and lower cobalt content cathode materials,
with the ultimate objective of ‘‘no-cobalt’’ cathodes. The pyrometallurgical
process relies on reasonably high cobalt concentrations for economic
feasibility. However, as cobalt concentrations are reduced, the business
model will be strained. Innovation is needed to enable pyrometallurgical
processors to adapt their business model to emergent generations of
LIBs, notably low-cobalt or no-cobalt cathode materials. For example,
developing roasting conditions to allow easier purification and separation
of different chemicals could be one possible direction. In addition,

Joule 3, 2622–2646, November 20, 2019 2639

 combining hydrometallurgical processes to allow further purification is
another direction (a few companies are beginning to employ this practice).
C. Secondary waste treatment: The waste in the pyrometallurgical process in-
cludes gases and solids. Gas (mainly CO2) is due to the battery-burning
process, and non-recycled materials become slag. In industry, gas is puri-
fied before emission. However, CO2 is emitted directly into the air.
Methods devised to reduce CO2 emission recover the solid waste, for
example, graphite (in addition to Co, Ni, and Cu) or convert that waste
into valuable materials will further increase the economic benefits of the
pyrometallurgical process.
3. The hydrometallurgical process: The hydrometallurgical process is also a
commercialized technology and has been primarily deployed in China.
A. Recovery of electrolyte and anode. Right now, the major focus in hydro-
metallurgical processing is the recovery of cathode material, due to its
high value. Other materials are not recovered or recycled, given that
they are low-value materials. Developing technologies to enable the re-
covery of the electrolyte and graphite anode as high-value materials will
further increase the economic feasibility of the recycling process.
B. Recycling of LiFePO4 batteries: Many e-buses use LIBs with LiFePO4 cath-
odes. Also, some EVs (especially in China) also use LIBs with LiFePO4
cathodes. Although LiFePO4 is a relatively expensive material, the intrinsic
elements are cheap. In fact, synthesizing LiFePO4 is very costly. There is no
economical way to recycle LiFePO4 cathode-containing LIBs, using a hy-
drometallurgical process. Direct recycling of LiFePO4, if shown to be tech-
nically feasible, may present a viable solution.
C. Secondary waste treatment: The waste in the hydrometallurgical process is
water and chemicals from the leaching step, co-precipitation, and washing,
which increase recycling costs. Further research on purifying the waste-
water, reusing the water, or reducing the amount of water in the process
is needed to reduce or eliminate waste water and associated costs.
4. The direct recycling process: The direct recycling process is still in the labora-
tory stage, and much work needs to be done in order to commercialize it.
A. Pre-processing steps to obtain pure materials: The principle of direct recy-
cling is to directly regenerate and reuse the cathode materials. However,
typical LIBs include many different materials (anode, cathode, copper,
aluminum, plastics, etc.). Creating a means to effectively and efficiently
separate cathode materials from other materials and each other automat-
ically could be one important research area for direct recycling. In addition,
the purity of the recovered cathode materials is also a critical research area.
B. Recover other materials in addition to cathode materials: Currently, the
direct recycling process is mainly focused on cathode powder, which
accounts for 30%–40% of material cost. As with the pyrometallurgical
and hydrometallurgical processes, it is also important that the direct recy-
cling process recycle other materials as much as possible.
C. Demonstrate recovered materials at scale: In order for the industry to
adopt the direct recycling process, the recycling process needs to reach
a certain scale to support meaningful impact. In addition, the recovered
materials need to be independently tested by industry.
D. Recover mixed cathode materials: The spent LIBs may include different
cathode materials. Furthermore, a given battery may use a mixture of cath-
ode chemistries. This is especially challenging for the direct recycling
process. Research into how to separate different cathode materials is crit-
ical, particularly in view of the many ratios of NMC comingled in the waste

2640 Joule 3, 2622–2646, November 20, 2019

 stream. Another option is trying to find a scenario in which the mixture can
be utilized directly.
E. Combine different recycling processes: Since each recycling process has
its advantages and disadvantages, it may be necessary to combine
different recycling processes to enable the most effective recycling. For
example, the cathode materials can be recovered via the hydrometallurgi-
cal process, and other materials can be recovered via a direct recycling
process.

In addition to the research needs outlined above, the following areas also need to be
addressed.

1. Establish a viable business model: Currently, unlike lead-acid batteries, a

viable business model has not been established for LIB recycling, due to low
collection rates, immature technology, and relatively low volumes, among
other reasons. Argonne National Laboratory has developed a recycling strat-
egy assessment tool, which models the economics and environmental impacts
of the aforementioned recycling approaches. The model considers each
process from the initial point of battery extraction from the vehicle to its final
recycling through the user-selected process. The model also offers a compre-
hensive comparison of different recycling technologies,97 which helps deter-
mine both the economic and environmental impacts of a particular recycling
process.
2. Recycling or pretreating locally: Because of the hazardous nature of LIBs,
transportation accounts for a large percentage of the recycling cost. Figure 3
shows the main LIB recycling facilities worldwide. As shown in the figure, recy-
cling facilities are only located in a few countries (United States, Canada,
France, Switzerland, Germany, Belgium, China, Japan, South Korea, and
Singapore). For example, in the United States, LIB recycling facilities are
concentrated on the east and west coasts. Spent LIBs in the middle of the
country must be transported a great distance in order to be recycled. Once
spent LIBs reach sizable volumes, establishing distributed recycling facilities
across the country will most likely be justified for optimized economic and
logistical gains.
3. Design for remanufacturing/repurposing/recycling: EV battery designs are
currently optimized for performance, safety, and cost. Remanufacturing/ re-
purposing/recycling should play a more significant role in EV pack design.
4. Solid-state LIB recycling: In order to further increase the energy density,
considerable research and development is being conducted for solid-state
LIB. The key challenge for solid-state LIB recycling will be how to properly
and safely handle lithium metal. Many steps of the current recycling process
are not appropriate for lithium metal—for example, discharging and shred-
ding. Discharging LIBs using a salt solution is a very common method to
release the remaining energy. However, lithium metal can have a very aggres-
sive reaction with water. In addition, lithium metal can easily adhere to the
shredder due to its soft nature. Therefore, innovations for recycling solid-state
LIBs will also be needed.

In addition to the technical considerations, collection, storage, logistics, and trans-

portation are also critical in order to develop viable business practices for spent LIBs.
Although these are beyond the scope of this paper, the recently announced Recy-
cling Prize (DOE) strives to spur advancements in these enabling areas. Moreover,
government policy and regulations also need to be implemented globally for LIB

Joule 3, 2622–2646, November 20, 2019 2641

Figure 3. Lithium-Ion Battery Recycling Facilities Worldwide
The locations of LIBs recycling facilities are listed and marked on the world map. With most of the facilities being concentrated in a few countries or
locations within a country, the challenges arise from the transportation when the quantity of spent LIBs becomes significant.

recycling. The European Union has stringent laws regarding LIB recycling, whereby
recycling efficiencies must meet 50% by 2030.98 In China, after August 2018, all EVs
are given a specific ID, which will help track the batteries from the first production to
second use and, finally, to recycling.99 However, in the US, there are still no national
regulations for the collection and recycling of large-format LIBs. Even though na-
tional policies regarding LIBs recycling have not been established, some existing
state policies are intended to promote the sustainability of xEV LIBs. California is a
forerunner in promoting vehicle electrification, and it will continue to be a national
leader in LIB recycling. In 2016, an EV action plan in California set a new goal to
develop new market opportunities for battery recycling.100,101

In fact, the policy can be initiated for manufacturing LIBs, EOL LIB collection
and transportation, recycling processes, and reuse of recycled materials. The
manufacturing standardization recommendations could include stipulations
regarding module design (energy, size, and voltage), the joining mechanism (revers-
ible to enable disassembly of packs), and adhesives, and these could effectively pro-
mote the acceptability of recycling. If there are fewer variants, the disassembly and
separation processes during recycling would require less labor, and appropriate

2642 Joule 3, 2622–2646, November 20, 2019

automation techniques could be developed. Also, regulations covering the entire
life span of recycling could be raised, from collection, storage, logistics, and trans-
portation to the actual recycling process in the facility. The principles or targets of
policy could include responsibility for EOL LIBs treatment (manufacturers, distribu-
tors), collection rates, and recycling efficiencies.98 The European Union (EU) has
enacted a union-wide extended producer responsibility (EPR) for LIBs, which re-
quires manufacturers to collect and manage EOL LIBs. Also, a deposit-refund system
could encourage users to properly recycle or dispose of EOL batteries.100,102 The
concern regarding recycled material rests on its performance and long-time and
reliable testing should be proposed to foster assurances. Policies and regulations
for standardized evaluation of EOL LIBs could facilitate the global use of recycled
materials.

ACKNOWLEDGMENTS
The authors acknowledge the financial support of the Department of Energy, the Na-
tional Energy Technology Laboratory under award number DE-EE0006250 with the
United States Advanced Battery Consortium LLC (USABC LLC). The authors also
thank Worcester Polytechnic Institute (WPI) Division of Marketing Communications
for creating figures.

Disclaimer

This report was prepared as an account of work sponsored by an agency of the

United States Government and USABC, LLC. Neither the USABC, LLC, the United
States Government, nor any agency thereof, nor any of their employees, makes
any warranty, expresses, implies, or assumes any legal liability or responsibility for
the accuracy, completeness, or usefulness of any information, apparatus, product,
or process disclosed or represents that its use would not infringe privately owned
rights. Reference herein to any specific commercial product, process, or service by
trade name, trademark, manufacturer, or otherwise does not necessarily constitute
or imply its endorsement, recommendation, or favoring by the United States Gov-
ernment or any agency thereof. The views and opinions of authors expressed herein
do not necessarily state or reflect those of the United States Government or any
agency thereof or those of USABC, LLC.

AUTHOR CONTRIBUTIONS
Conceptualization, Y.W.; Visualization, M.C.; Original Writing, M.C., R.A., and Y.W.;
Review & Editing, M.C., R.A., Y.W., X.M., B.C., P.K., and N.S.

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