CET 96
DOI: 10.3303/CET2296005
Paper Received: 11 February 2022; Revised: 8 July 2022; Accepted: 30 August 2022
Please cite this article as: Latini D., Lagnoni M., Brunazzi E., Mauri R., Nicolella C., Della Posta P., Tognotti L., Bertei A., 2022, Recycling of
Lithium-ion Batteries: Overview of Existing Processes, Analysis and Performance, Chemical Engineering Transactions, 96, 25-30
DOI:10.3303/CET2296005
CHEMICAL ENGINEERING TRANSACTIONS
VOL. 96, 2022
A publication of
The Italian Association
of Chemical Engineering
Online at www.cetjournal.it
Guest Editors: David Bogle, Flavio Manenti, Piero Salatino
Copyright © 2022, AIDIC Servizi S.r.l.
ISBN 978-88-95608-95-2; ISSN 2283-9216
Recycling of Lithium-Ion Batteries: Overview of Existing
Processes, Analysis and Performance
Dario Latinia, Marco Lagnonia,*, Elisabetta Brunazzia, Roberto Mauria, Cristiano
Nicolellaa, Pompeo Della Postab,c, Leonardo Tognottia,*, Antonio Berteia,*
aDipartimento di Ingegneria Civile e Industriale, Università di Pisa, Italy
bDipartimento di Economia e Management, Università di Pisa, Italy
cThe Belt and Road School, Beijing Normal University at Zhuhai, Guangdong, China
*marco.lagnoni@phd.unipi.it, leonardo.tognotti@unipi.it, antonio.bertei@unipi.it
Lithium-ion batteries (LIBs) have become a widespread technology for electrochemical energy storage in the
current era of digitalization and transport electrification, being used as electric stationary storage as well as for
powering electric vehicles, e-bikes and portable electronic devices such as smartphones and laptops. However,
LIBs contain valuable materials, such as cobalt, nickel, lithium and graphite, whose supply has become critical
to meet the increasing demand of batteries. Therefore, proper recycling processes are required in order to
recover these materials from spent batteries and re-use them to produce new batteries in a sustainable cycle.
This contribution provides an extensive survey of the main recycling routes available today, focusing specifically
on pyrometallurgical and hydrometallurgical processes based in Europe, North America and Asia. Attention is
also devoted to the recycling behaviour of individuals and companies and to the possible ways to increase their
recycling rate. The comparison of different processes allows for the ranking of best practices as well as the
drawbacks of different process units, with identification of which materials can be recovered, their recovery rate,
and an assessment of the overall recycling efficiency of the process for different battery sizes (small and large,
for portable electronics and electric vehicles, respectively). The analysis reveals that pyrometallurgical
processes can flexibly treat different LIB chemistries but, since the electrolyte and graphite are burnt in the
process, the global recycling efficiency cannot compete with hydrometallurgical processes, especially for small
format batteries. Nevertheless, hydrometallurgical processes typically require preliminary mechanical
separation treatments to separate the black mass, which contains valuable electrodic materials, as well as
complex precipitation steps, which eventually reduce the material recovery rate and the applicability to diverse
LIB chemistries. Finally, the study reports an analysis of the electrochemical performance of a battery made
with recycled materials, showing that even if recycled cathodic materials had a lower gravimetric capacity and
solid-state diffusivity, the performance of a recycled battery could be compensated by simple minor changes to
the cell design which would ultimately decrease the specific energy density by a few percent compared to a LIB
made with virgin materials.
1. Introduction
The abuse of natural resources and climate change are forcing the society to move towards a sustainable way
of life. The decarbonization of the transport sector points in this direction, witnessing a rapid growth of electric
vehicle (EV) utilization. Lithium-ion batteries (LIBs) are a central component of this electric revolution, powering
different types of EVs, from hybrid and plug-in electric vehicles to EVs powered solely by a battery pack. In
addition, LIBs are increasingly used for large stationary energy storage applications, while being still abundant
in portable electronics and small power tools. However, considering the expected lifetime of a LIB, which is in
the order of 10-15 years, a significant flow of spent batteries is expected in the future, summing cumulatively to
11 Mt in 2030 (Thompson et al., 2020). Such a flow of spent batteries may represent a waste-management
challenge on one hand, while it can be turned into a valuable opportunity to recycle critical raw materials such
as cobalt, lithium and nickel (Harper et al., 2019).
25
There exist different routes for LIB recycling. The most established one is pyrometallurgy, which consists of
smelting the battery at high temperature to recover an alloy of precious metals among which nickel, copper and
cobalt; instead, lithium is lost in the slag while graphite, plastics and electrolyte solvents are burnt (Harper et al.,
2019). The hydrometallurgical route replaces the smelting step with the leaching of the battery components after
crushing and mechanical separations; the resulting metal ions in solution are selectively precipitated and/or
extracted to recover high-quality metal salts or even precursors ready for LIB manufacturing (Harper et al.,
2019). Thus, different recycling strategies allow for diverse capabilities of material recovery and quality of
recycled outputs, affecting both the potential of closed-loop recycling solutions and the overall sustainability of
the lithium-ion battery chain.
This study is meant to provide an updated overview of LIB recycling processes from an engineering perspective
in order to give a preliminary quantitative assessment of recycling efficiency of different processes, with
concurrent identification of best practices and bottlenecks. Finally, the potential of a closed-loop battery chain
is discussed by assessing which design strategies at the cell level can be adopted to compensate for the
reduced performance of recycled cathode active materials.
2. Overview and analysis of LIB recycling strategies
The format and size of LIBs are not standardized. From a recycling viewpoint, they can be classified into two
broad categories: i) large format LIBs, as those used in EVs, which comprise system peripheries such as cables,
external plastics, aluminium or steel casing in addition to the battery cells, and ii) small format LIBs, as those
used in power electronics, which basically consist of the battery cell only. In any case, the battery cell is the
basic unit of both formats. A battery cell contains several materials within a relatively thin case (typically of
aluminium), such as copper and aluminium current collector foils, graphite, organic solvents and LiPF6 as liquid
electrolyte, a polypropylene porous separator and particles of cathode active materials, among which the most
common ones nowadays are LiNixMnyCo1-x-yO2 (NMC), LiNixCoyAl1-x-yO2 (NCA), LiFePO4 (LFP) and LiCoO2
(LCO) (Schröder et al., 2017).
Figure 1 reports a schematic representation of the principal recycling strategies, where the different steps are
marked with a different colour to distinguish mechanical, pyrometallurgical, hydrometallurgical and co-
precipitation operations. The pyrometallurgical route (Figure 1a) starts with a manual disassembly of cables,
casing and other system peripheries, which sum up to ca. 45 % of the weight of large format batteries (Dai et
al., 2019). The disassembled cells are merged with small format ones and sent to a furnace to operate the
smelting of the battery. Sand, limestone, coke, other reducing agents and slag formers are added to LIB cells,
in a ratio that can vary from 50 to 200 % weight compared to the battery input depending on the cell casing
(steel or aluminium, respectively) (Cheret and Santen, 2007). A vertical shaft furnace is typically used: the feed
enters a pre-heating zone at 300 °C to evaporate electrolyte solvents, then a temperature increase to 700 °C in
the second zone causes plastic pyrolysis, followed by a final zone at 1200-1400 °C at the bottom of the furnace
where smelting and reduction take place (Tanong et al., 2014). Two fractions are produced from the furnace: i)
a metal alloy containing Cu, Ni, Co and Fe, and ii) a slag fraction which contains Li, Al, Mn and other elements
such as Si and Ca in oxidised state (Velàzquez-Martínez et al., 2019). The metal alloy is typically refined via
hydrometallurgical steps of leaching and selective precipitations or solvent extractions to recover single metal
salts such as CuS, Ni(OH)2, CoCl2 and Fe(OH)3, which can re-enter in the LIB manufacturing chain. The slag
can potentially follow a similar hydrometallurgical refining process to recover Li, Al, Mn and Fe salts (Li et al.,
2019); however, currently the value of such end products is not sufficient to make slug refining economically
attractive, thus the slug is typically downcycled by selling it as an additive for the construction industry.
Figure 1b shows the principal steps used by a hydrometallurgical process (Kwade and Diekmann, 2018). The
first section of the process comprises mechanical treatments to obtain the black mass, which is the powder
containing the valuable cathodic and anodic materials. Hence, after discharging and disassembly of large
battery packs, LIB cells are crushed under inert atmosphere to reduce the risks associated to electric sparks
and flammable electrolyte. The liquid electrolyte is then removed by adopting different techniques, among which
thermal drying, extraction with organic solvents or with sub/super-critical CO2 (Nowak and Winter, 2017). A
series of mechanical separations, comprising air classification with zig-zag sifters, crushing, sieving, magnetic
and optical separations, enable for the recovery of different streams, such as a light plastic fraction, Al foils
fraction, Cu foils fraction, steel fraction and the black mass (Kwade and Diekmann, 2018). The black mass,
which contains graphite, cathode active material and impurities of metal scraps, is leached typically with H2SO4
and H2O2 as reducing agent, so that the metals contained in the cathode active material are dissolved in solution
while graphite remains unleached and can be separated by filtration (Gratz et al., 2014). The resulting solution
containing Ni, Co, Li, Mn ions, with impurities of Fe, Al and Cu ions, can either be processed by classical
hydrometallurgical steps of selective precipitations and extractions to recover single metal salts (blue steps at
the bottom of Figure 1b) or can undergo a co-precipitation process (green steps in Figure 1b). The latter is an
26
innovative strategy particularly suited for NMC input streams, where a ternary hydroxide of Ni, Co and Mn can
be co-precipitated and then sent to the sintering step, along with Li2CO3 (or LiOH) recovered via precipitation at
high pH from the leached solution, in order to re-synthetize the cathode active material in oxide form (Kwade
and Diekmann, 2018).
Figure 1: Schematic block diagram of LIB recycling strategies based on: a) pyrometallurgy, with optional
hydrometallurgical refining, b) hydrometallurgy, comprising preliminary mechanical separations and two
alternative hydrometallurgical/co-precipitation routes of the black mass.
Table 1 summarizes the main companies which operate LIB recycling across three different continents. As the
table shows, in Europe there are several companies which carry out only mechanical separations (i.e., the first
steps in Figure 1b) up to the black mass; only a few companies follow the hydrometallurgical route, while the
most established companies with higher capacities carry out battery smelting as in the pyrometallurgical
strategy, often followed by a hydrometallurgical refining of the metal alloy as in Figure 1a. In North America and
in Asia the company distribution is different: North America is characterized by LIB recyclers which tend to
achieve a closed loop of cathode materials via hydrometallurgical processes, while in Asia there is a significant
recycling capacity provided by different companies, which mainly treat production scraps from LIB
manufacturing giga-factories via hydrometallurgical processes.
Table 1: List of LIB recycling companies in different continents classified according to the main recycling strategy
Recycling route Companies in Europe Companies in North America Companies in Asia
Pyrometallurgical Umicore, Accurec,
Glencore, SNAM,
Valdi
Glencore, Inmetco Sony Sumitomo, Kobar,
Nippon Recycle Centre
Corp.
Hydrometallurgical or co-
precipitation
Recupyl Valibat,
Neometals, Northvolt,
Stena
Retrieve, Ascend Elements,
American Manganese Inc.,
Lithion Recycling, Li-Cycle
Hunan BRUNP, Shenzen
Green Eco (GEM),
SungEel, Huayo
Mechanical separations Duesenfeld, Akkuser
Oy, Batrec, Euro
Dieuze, Redux,
Fortum Oyj, uRecycle
In any case, different recycling processes enable for different recycling efficiencies and material recovery rates.
In a pyrometallurgical process some materials contained in the LIB cells are burnt, including graphite, plastic
separator and the electrolyte. As such, considering the mass composition of a LIB cell (Dai et al., 2019), the
recycling efficiency of a pyrometallurgical process is in the order of 55 % for small format LIBs, where the
recycling efficiency is calculated as the mass of recovered materials compared to the mass of the input stream;
Pre-treatments
and disassembly
Crushing
Electrolyte
removal
Mechanical
separations
Leaching
Selective precipitations
& solvent extraction
Leaching Co-precipitation Sintering
Electrolyte
Casing and
peripheries
Al foils, Cu foils
Al/Fe fraction,
plastic fraction
Spent large
format LIBs
Spent small
format LIBs Cathode active
material
Al, Cu, Fe salts
(low purity)
Co, Ni, Mn, Li salts
(high purity)
Black mass
Mechanical steps
Hydrometallurgical steps
Co-precipitation steps
Mechanical steps
Pyrometallurgical steps
Hydrometallurgical steps
Co-precipitation method steps
Smelting
Pre-treatments
and disassembly
Spent large
format LIBs
Casing and
peripheries
Incineration
electrolyte,
graphite, plastics
Spent small
format LIBs
Slag
(Li, Al, Mn, Fe)
Alloy
(Co, Ni, Cu, Fe)
Leaching
Selective precipitations
& solvent extraction
Leaching
Selective precipitations
& solvent extraction
Hydrometallurgical refining (optional) Pyrometallurgical steps
Co, Ni salts
(high purity)
Cu, Fe salts
(low purity)
Al, Fe salts
(low purity)
Li, Mn salts
(high purity)
a)
b)
27
the recycling efficiency can achieve 70 % and beyond in case of large format LIBs since the casing and other
peripheries can be disassembled and easily recovered. Valuable metals, such as Ni, Co and Cu, can be
effectively recovered in high-quality streams with material recovery rates in the order of 90-95 %; in particular,
ca. 60 kg of critical cathodic elements as Ni and Co can be recovered from a ton of mixed batteries (75 % large
format, 25 % small format). However, all the Li ends in the slag phase and cannot be recovered as a high-quality
product, thus it cannot re-enter the LIB manufacturing chain. In any case, the pyrometallurgical route stands out
as the most mature strategy, being flexible to accommodate different battery chemistries.
Hydrometallurgical and co-precipitation processes enable for higher recycling efficiencies due to the absence
of the smelting step. More than 80 % of the LIB mass can be recovered from small format batteries, value which
can potentially increase to more than 90 % in case of large format LIBs. Such an increase in recycling efficiency
is basically due to the recovery of electrolyte, graphite and the light plastic fraction. However, typically the quality
of electrolyte and graphite is not sufficient to be reused in the manufacturing of a new battery, although some
companies as OnTo Technologies and Lithion claim that, thanks to additional treatments, these components
can be considered as battery-grade. Thus, the main benefit of recycling routes based on leaching of the black
mass consists in the recovery of lithium, achieving a material recovery rate of ca. 75 % (i.e., ca. 7 kg of Li
recovered from a ton of spent batteries). On the other hand, the main limitations of the hydrometallurgical route
lie in the mechanical separation section, where part of the cathode active materials is lost due to the strong
adhesion to current collector foils given by the organic binders used in all battery formulations (Harper et al.,
2019). Moreover, the co-precipitation steps are susceptible to the presence of phosphates, which cause
undesired precipitation of Ni, Co and Mn phosphates, thus limiting the applicability of such a recycling strategy
to spent batteries which should not contain LFP as a cathode material (Kwade and Diekmann, 2018).
3. Guidelines to compensate performance limitations of recycled materials
The overview of recycling strategies reported in the previous section highlights that there is a concrete potential
for achieving a closed loop of materials in the LIB recycling chain, thus enabling for the manufacturing of a
second generation of batteries with materials coming from recycled streams rather than from virgin sources, at
least for the cathode materials. While secondary raw materials resulting from pyrometallurgical and
hydrometallurgical recycling processes may arguably entail the same properties of virgin ones, recycled cathode
active materials obtained via co-precipitation may have decreased electrochemical properties due to the
presence of impurities (Beaudet et al., 2020). Therefore, modifications to the electrode design must be
conceived to compensate the performance loss introduced by recycled cathode active materials.
Figure 2 summarizes the main design strategies suggested for compensating a reduction in the gravimetric
accessible capacity of recycled cathode materials (namely, NMC111 in this specific case), which is in the order
of max 10 % of capacity loss (Zhao et al., 2020). Such a gravimetric capacity loss can be due to either a decrease
in maximum concentration of lithium intercalated in the cathode material (Figure 2a, yellow box) or by a decrease
in solid-phase diffusivity of lithium ions in the cathode material (Figure 2a, green box), estimated in the order of
-10 % and -50 %, respectively (Lagnoni et al., 2022). In both cases, the reduced accessible capacity can be
compensated by an increase in cathode thickness; alternatively, the reduced solid-phase diffusivity can be
compensated by a decrease in the particle size of cathode particles. These compensation measures do not
have, in general, any effect on the design of the anode, except for the case where a reduction in solid-phase
diffusion at the cathode is compensated by an increase in cathode thickness, where the anode thickness must
be increased too in order to keep a balanced anode-to-cathode nominal capacity ratio.
Figure 2b reports the results of the compensation measures by using a physics-based thermo-electrochemical
battery model (Lagnoni et al., 2021) tuned to replicate the electrochemical response of the graphite-NMC111
Samsung SDI 94 h battery used in the BMW i3 electric vehicle (Lagnoni et al., 2022). Figure 2b shows that,
compared to the electrode thicknesses of the reference battery made with virgin materials (namely, 90.5 m for
the cathode, 98 m for the anode), different compensation measures lead to different designs of LIBs produced
with recycled materials. If a recycled cathode active material features a 10 % loss in nominal capacity (yellow
box in Figure 2a), a corresponding increase by 10 % in cathode thickness has to be foreseen (Figure 2b) to
guarantee the same accessible capacity during operation. On the other hand, a decrease in solid-phase
diffusivity (green box in Figure 2a) can be compensated by either a minor increase in cathode and anode
thicknesses (less than 2 % increase cumulatively, Figure 2b) or by a reduction in the diameter of cathode
particles from 8 m to 6 m. The latter strategy may arguably reduce the battery life because of the increased
specific surface area of cathode particles, which may trigger parasitic reactions. On the other hand, the
strategies based on increasing the electrode thicknesses appear to be totally feasible since the volume increase
of the jelly roll is minimal and can be accommodated within the cell casing, resulting only in a marginal reduction
in energy density at the pack level (from 142 Wh/kg to 137 Wh/kg as a minimum), which is still suitable for
electric vehicle applications.
28
Figure 2: a) Strategies to cope with reduced properties of recycled cathode active materials via increase of
electrode thickness or reduction of particle size; b) effect of compensation measures on electrode thickness and
size of cathode particles to ensure the same battery capacity.
Hence, the numerical analysis reported in Figure 2 indicates that recycled cathode active materials, even with
reduced electrochemical properties, can be accommodated in the manufacturing of secondary lithium-ion
batteries by adopting marginal changes to the electrode design, enabling for a closed loop of materials in the
battery chain.
4. Conclusions
This paper gave an overview on the status of recycling processes for lithium-ion batteries from an engineering
perspective, assessing the current limitations and the feasibility of reusing recycled cathode materials in the
manufacturing of new cells.
The survey of LIB recycling companies in different continents indicates that in Europe a large fraction of recyclers
performs only mechanical separation treatments to obtain the black mass; however, the black mass cannot be
considered as an end product from a recycling viewpoint. The alternative strategy adopted mostly in Europe is
pyrometallurgy, which has the clear benefit of being only marginally affected by the chemical composition of
spent batteries in the input stream. However, since graphite, electrolyte and plastics are burnt, the recycling
efficiency of pyrometallurgy lies in the order of 55-70 % for small format and large format batteries, respectively;
moreover, Li is downcycled in the slag and currently its recovery via hydrometallurgical refining processes is not
economically feasible. In North America and Asia recyclers adopt mostly the hydrometallurgical and co-
precipitation recycling routes. While the leaching phase is not problematic in terms of material recovery rate, the
preliminary mechanical separation steps limit the recovery of valuable cathodic metals. Nevertheless, the overall
recycling efficiency can potentially be up to 90 %, along with the possibility to recover ca. 75 % of lithium in
battery-grade products such as Li2CO3 and LiOH. Therefore, the hydrometallurgical and co-precipitation
strategies should be promoted at industrial level, especially in Europe, to cope with the expected lack of lithium
from natural sources, by investigating better mechanical separations, refining operations for electrolyte and
graphite to make them battery-grande, and the use of water-soluble binders.
The use of recycled materials in the manufacturing of new batteries was also investigated in this study. In
particular, compensatory measures in electrode design were suggested in case of reduced electrochemical
properties of cathode active materials. The numerical results showed that a 10 % decrease in nominal volumetric
capacity of the cathode active material can be compensated by a 10 % increase in cathode thickness, resulting
only in a 3.5 % reduction in gravimetric energy density at the pack level, which is still suitable for electric vehicle
applications. A similar strategy is suggested in case of reduced solid-phase diffusivity of the cathode active
material, which produces an even smaller loss in energy density (< 1 %). On the other hand, decreasing the
size of recycled cathode active particles does not seem to be a viable alternative because the battery life might
be negatively affected.
In summary, the survey of existing LIB recycling processes and the compensatory measures suggested in the
study indicate that a close loop of materials in the lithium-ion battery chain is technically feasible, at least for Ni,
Co, Cu, Al and Mn, while the recycling of Li, graphite and electrolyte still needs further technological
advancements before being adopted at industrial scale.
0 5 10 15
Reference cell
85 90 95 100
10 % capacity
comp.: thickness
−
Electrode thickness [μm]
50 % diffusivity
comp.: thickness
−
50 % diffusivity
comp.: diameter
−
Electrode thickness variation [%]
8μm
8μm
8μm
6μm
Cathode
particle
diameter
[μm]
Anode
Cathode
Decrease particle
diameter cathode
Increase cathode
thickness
Li max concentration
decrease
No impact on anode
design
Increase anode
thickness
10 %−
Solid-phase
diffusivity decrease
50 %−
a) b)
29
Acknowledgments
This research was supported by the University of Pisa through the funding program “Progetti di Ricerca di
Ateneo PRA 2020–2021”, project no. PRA_2020_48.
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Recycling of Lithium-Ion Batteries: Overview of Existing Processes, Analysis and Performance