Molecules 27 03119

molecules
Review
A Comprehensive Review of Lithium-Ion Capacitor Technology:
Theory, Development, Modeling, Thermal Management
Systems, and Applications
Danial Karimi 1,2, * , Hamidreza Behi 1,2 , Joeri Van Mierlo 1,2 and Maitane Berecibar 1
1 Research Group MOBI—Mobility, Logistics, and Automotive Technology Research Centre,

Vrije Universiteit Brussel, Pleinlaan 2, 1050 Brussels, Belgium; [email protected] (H.B.);
[email protected] (J.V.M.); [email protected] (M.B.)
2 Flanders Make, 3001 Heverlee, Belgium
* Correspondence: [email protected]; Tel.: +32-(499)875895
Abstract: This review paper aims to provide the background and literature review of a hybrid energy
storage system (ESS) called a lithium-ion capacitor (LiC). Since the LiC structure is formed based on
the anode of lithium-ion batteries (LiB) and cathode of electric double-layer capacitors (EDLCs), a
short overview of LiBs and EDLCs is presented following the motivation of hybrid ESSs. Then, the
used materials in LiC technology are elaborated. Later, a discussion regarding the current knowledge
and recent development related to electro-thermal and lifetime modeling for the LiCs is given. As
the performance and lifetime of LiCs highly depends on the operating temperature, heat transfer
modeling and heat generation mechanisms of the LiC technology have been introduced, and the
published papers considering the thermal management of LiCs have been listed and discussed. In
the last section, the applications of LiCs have been elaborated.
Citation: Karimi, D.; Behi, H.; Van
Keywords: lithium-ion capacitor (LiC); lithium-ion battery; electric double-layer capacitor;
Mierlo, J.; Berecibar, M. A
Comprehensive Review of electro-thermal modeling; lifetime modeling
Lithium-Ion Capacitor Technology:
Theory, Development, Modeling,
Thermal Management Systems, and
Applications. Molecules 2022, 27, 3119. 1. Introduction
https://doi.org/10.3390/ Currently, the reduction of carbon dioxide (CO2 ) emissions to decrease global warming
molecules27103119 and the greenhouse gas (GHG) effect is a matter of grave concern, in which the negative
Academic Editor: Jim P. Zheng impacts of oil depletion, GHG, and vehicular emissions are rising annually [1]. In this
regard, by increasing the number of vehicles and rising fuel consumption, there would be a
Received: 30 March 2022
question of the tolerability of environmental pollution. The possible solution has been the
Accepted: 8 May 2022
investigation of zero-emission vehicles to reduce GHG emissions. Towards this direction,
Published: 12 May 2022
conventional internal combustion engines ought to be replaced in the field of mobility.
Publisher’s Note: MDPI stays neutral Environmentally friendly rechargeable ESSs could contribute to this direction, as they can
with regard to jurisdictional claims in adequately supply an electro-motive application such as hybrid, plug-in hybrid, and pure
published maps and institutional affil- electric vehicles [2].
iations. Usually, ESSs are mostly comprised of LiBs and EDLCs as the primary electrochemical
storage systems. LiBs are manufactured in different gravimetric and volumetric charac-
teristics and can meet the increased demands on energy and power as well as lifetime
capabilities [3]. High energy densities and low self-discharge are among the advantages
Copyright: © 2022 by the authors.
of LiBs. Nevertheless, specific LiB chemistries such as NMC (Lithium-Nickel-Manganese-
Licensee MDPI, Basel, Switzerland.
Cobalt-Oxide), widely used in many applications, encounter challenges when dealing with
This article is an open access article
increased charge or discharge current rates [4]. In addition, some deficiencies have been
distributed under the terms and
conditions of the Creative Commons
seen in the case of generating high-power output during acceleration [2]. For instance,
Attribution (CC BY) license (https://
some LiBs supply at least 200 Wh/kg of specific energy, but at the same time less than
creativecommons.org/licenses/by/
350 W/kg of specific power [5].
4.0/).
Molecules 2022, 27, 3119. https://doi.org/10.3390/molecules27103119 https://www.mdpi.com/journal/molecules

Molecules 2022, 27, 3119 2 of 22
On the other hand, EDLCs have high power densities with a long lifetime that can be
charged and discharged quickly but suffer from low energy densities. For instance, some
EDLCs supply at least 10 kW/kg of specific power, but at the same time, less than 5 Wh/kg
of specific energy [6]. Gao et al. [7] used EDLCs along with LiBs. However, the usage of
EDLCs often requires a bulky and highly efficient DC–DC converter, which counteracts
the cost and energy efficiency of the system [8]. The logic system can be based on the
hybridization of LiBs with EDLCs to achieve higher energy and power values within a
longer lifetime [9]. Therefore, the anode electrode material of LiBs and cathode electrode
material of EDLCs were combined in a single ESS to develop a hybrid ESS combining the
high energy of LiBs and high power and long lifetime of EDLCs [10]. In such a context,
lithium-ion capacitor (LiC) came into existence. Despite all the advantages such as high
specific power and energy, and long lifetime, LiCs generate excessive amounts of heat in
high current rates that should be controlled for safety reasons [11]. Therefore, a robust
thermal management system (TMS) is vital for all electrical energy storage systems [12]. In
this context, special attention has been paid to thermal modeling in this paper.
2. Various Types of Energy Storage Systems

2.1. Lithium-Ion Batteries (LiBs)
Lithium-ion batteries (LiBs) consist of four main domains: anode and cathode as the
charge carriers, separator to divide electrodes to avoid short-circuits, and electrolyte to
carry ions [13]. When LiBs are charged and discharged, electrodes generate heat, which
should be controlled to prevent battery malfunction [14]. For example, by damaging the
separator, uncontrolled electrochemical reactions would generate significant amounts of
excess heat [15]. In such uncontrollable cases, the electrolyte will behave as an additional
fuel supply for further heat generation, which will result in thermal runaway. An example
of the working principle of LiBs with Lithium-Cobalt-Oxide (LiCoO2 )/graphite is depicted
in Figure 1. During the charging of LiBs, lithium ions de-intercalate from the cathode and
diffuse into the electrolyte, which leads to ion movement to the separator to be intercalated
into the anode. The electrons move in the same direction as the flow of ions (i.e., from the
positive electrode to the negative electrode or vice versa) in the external circuit. Meanwhile,
the current flows in the opposite direction to the movement of electrons. During discharging
of LiBs, lithium ions move back from the anode to the cathode. The shuttling of lithium
ions during charging and discharging generates excessive heat due to the Joule loss and
chemical loss [16]. Although the heat generated during battery operation is normal, the
battery safety will be compromised if there is no dissipation path to remove the heat loss
during charging and discharging processes [17].
2.2. Electric Double-Layer Capacitors (EDLCs)

Electric double-layer capacitors (EDLC), also known as supercapacitors (SC) or ul-
tracapacitors, store energy in their electric double-layer. In EDLCs, a shorter distance
between plates and larger area plates results in higher effective capacitance. The energy
storage mechanism of EDLCs is achieved via charge separation at electrode–electrolyte
interfaces. The ions are physically absorbed in the surface of electrodes commonly made
of activated carbon (AC), carbon nanotubes (CNT), and graphene. Figure 2 shows the
basic ides for EDLCs, where AC as two electrodes are placed into an electrolyte [18]. As
Figure 2a demonstrates, by applying a power source to AC electrodes, charge layers are
formed; positive and negative. These charge layers are oppositely layered to be formed
into the electrolyte. AC electrode material is porous activated carbon with high electrical
conductivity, high chemical stability, and low cost. In addition, the AC electrode has a large
surface area per specific surface area due to the distribution of pores (Figure 2b) for each
electrode–electrolyte surface (Figure 2c). Pseudocapacitors can be grouped as supercapac-
itors with the storage mechanism of fast surface redox reactions occurring between the
electrode and the electrolyte [19].
Molecules2022,
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Figure 1. (a) A graphical view of the LiB structure for all the different battery types [13]; (b) cylin-
Figure 1. (a) A graphical view of the LiB structure for all the different battery types [13]; (b) cylindrical
drical cell type; (c) prismatic cell type; (d) coin cell type; (e) pouch cell type; (f) the relationship
Figure
cell type;1.(c)
(a)prismatic
A graphical
cellview
type;of
(d)the LiBcell
coin structure forpouch
type; (e) all thecell
different battery
type; (f) types [13]; between
the relationship (b) cylin-
between cells, modules, and battery pack [20].
drical
cells, cell type;
modules, (c)battery
and prismatic
packcell
[20].type; (d) coin cell type; (e) pouch cell type; (f) the relationship
between cells, modules, and battery pack [20].
Figure 2. The EDLC formed by a collector, AC electrodes, and an electrolyte: (a) concept, (b) charg-
ing, (c) and discharging [18].
Figure2.2.The
Figure TheEDLC
EDLCformed
formedbybya collector,
a collector,
ACAC electrodes,
electrodes, andand
an an electrolyte:
electrolyte: (a) concept,
(a) concept, (b) charg-
(b) charging,
ing, (c) and discharging
(c) and discharging [18]. [18].
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2.3.Lithium-Ion
2.3. Lithium-IonCapacitors
Capacitors(LiCs)
(LiCs)
TheLiC
The LiCrepresents
representsan anemerged
emergedtechnology
technologythat thatcombines
combinesthe thepre-lithiated
pre-lithiatedanodeanode
electrodematerial
electrode materialofofLiBs
LiBsandandthe
thecathode
cathodeelectrode
electrodematerial
materialofofEDLCsEDLCs[21].
[21].This
Thiselectrode
electrode
combinationinherits
combination inheritsthethehigh
highpower
powerdensity
densityandandlonger
longerlifetime
lifetimeofofEDLCs
EDLCswith withthethehigh
high
energydensity
energy densityofofLiBs
LiBs[22].
[22].Typically,
Typically,LiCs
LiCsshow
show4 4toto55times
timesmore moreenergy
energythanthanEDLCS
EDLCS
duetotothe
due theutilization
utilizationofofa abulk
bulkmechanism
mechanismtotostore
storethetheenergy
energyininone oneofofthe
theelectrodes.
electrodes.InIn
addition, LiC’s electrolyte material can achieve higher voltage values comparedtotostandard
addition, LiC’s electrolyte material can achieve higher voltage values compared stand-
EDLCs.
ard EDLCs.Therefore,
Therefore,LiCs cancan
LiCs compete withwith
compete EDLCsEDLCsin terms of energy
in terms density.
of energy Nevertheless,
density. Never-
LiCs have
theless, LiCsless
haveenergy density
less energy than than
density LiBs,LiBs,
but but
can can
nevernevercompete
compete with
withLiBs
LiBsinin
terms
termsof
ofenergy
energydensity
density[23].
[23].Although
Although the the energy
energy density
density ofof LiCs
LiCs is is lower
lowerthan
thanthatthatofofLiBs,
LiBs,the
the
power density of LiCs is much higher than LiBs. Figure 3 exhibits the
power density of LiCs is much higher than LiBs. Figure 3 exhibits the performance of LiCs performance of LiCs
ininterms
termsofofenergy
energyandandpower
powerdensities
densitiesasasa aRagone
Ragoneplot plot[24],
[24],ininwhich
whichthe thespecific
specificenergy
energy
of LiCs is in the range of 25–100 Wh/kg, with a specific power
of LiCs is in the range of 25–100 Wh/kg, with a specific power of 1000–10,000 W/kg.of 1000–10,000 W/kg.
Figure
Figure3.3.The
TheRagone
Ragoneplot
plotfor
fordifferent
differentESSs
ESSs[24].
[24].
2.4.Construction
2.4. ConstructionofofLithium-Ion
Lithium-IonCapacitors
Capacitors
Figure4 4shows
Figure showsthe thestorage
storagemechanism
mechanismofofthreethreedifferent
differentESSs,
ESSs,including
includingLiBs,
LiBs,LiCs,
LiCs,
and EDLCs [25], in which the LiC technology stands between LiBs and EDLCs. As can bebe
and EDLCs [25], in which the LiC technology stands between LiBs and EDLCs. As can
observed,although
observed, althoughEDLCsEDLCshavehavea asymmetric
symmetricconstruction,
construction,thetheLiC
LiCbears
bearsan
anasymmetric
asymmetric
configuration as it employs two different types of electrodes. As explained,
configuration as it employs two different types of electrodes. As explained, the charge the charge
and
and discharge processes of EDLCs are based on a non-Faradaic double-layer
discharge processes of EDLCs are based on a non-Faradaic double-layer capacitor [26]. capacitor [26].
Since LiCs combine two types of electrodes, on one side, anions are adsorbed
Since LiCs combine two types of electrodes, on one side, anions are adsorbed into/de- into/desorbed
from the
sorbed positive
from electrode’s
the positive surface, surface,
electrode’s and on the
andother side,
on the ions side,
other of lithium arelithium
ions of intercalated
are
into/de-intercalated from the negative electrode’s body. Faradaic intercalation and non-
intercalated into/de-intercalated from the negative electrode’s body. Faradaic intercala-
Faradaic surface reaction are the main reasons for the high power and energy densities of
tion and non-Faradaic surface reaction are the main reasons for the high power and en-
LiCs. The power (PESS [W]) and energy (EESS [J = W·s]) of an ESS can be expressed as [27]:
ergy densities of LiCs. The power (𝑃𝐸𝑆𝑆 [W]) and energy (𝐸𝐸𝑆𝑆 [J=W.s]) of an ESS can be
expressed as [27]: 1
EESS = CV 2 (1)
12 2
𝐸𝐸𝑆𝑆 = 𝐶𝑉 (1)
2 2
V
PESS = 𝑉 2 (2)
𝑃𝐸𝑆𝑆 = 4R (2)
where C [F], V [V], and R [Ω] denote the cell’s 4𝑅 capacitance, potential, and equivalent
where
seriesCresistance
[F], V [V],(ESR).
and R Figure
[Ω] denote the cell’s capacitance,
5 demonstrates potential,
the characteristics ofand
LiBsequivalent
and EDLCs series
over
resistance (ESR).
six essential Figure
criteria, 5 demonstrates
including the characteristics
energy density, of LiBs
power density, and EDLCs
cyclability, safetyover six
ecology,
operation
essential temperature,
criteria, includingand voltage
energy for electrochemical
density, ESSs. A synergistic
power density, cyclability, impact
safety ecology, op-is
expected
eration by combining
temperature, andEDLCs and
voltage forLiBs to form a hybrid
electrochemical ESSs.ESS
A such as LiCs.impact is ex-
synergistic
pected by combining EDLCs and LiBs to form a hybrid ESS such as LiCs.
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2022, 27,27, x FOR
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3119 PEER
PEER REVIEW
REVIEW 5 of
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24
Figure
Figure
Figure 4. 4.
4. TheThe
The storage
storage
storage mechanism
mechanism
mechanism and
and
and chemical
chemical
chemical structure
structure
structure ofof
of LiBs,
LiBs,
LiBs, LiCs,
LiCs,
LiCs, and
and
and EDLCs.
EDLCs.
EDLCs. The
The
The blue
blue
blue arrows
arrows
arrows
denote
denote thethe discharging
discharging process
process while
while thethe green
green arrows
arrows
arrows denote
denote
denote the
thethe charging
charging
charging process
process
process [25].
[25].
[25].
Figure
Figure 5. 5. Comparison
Comparison ofof LiBs
LiBs and
and EDLCs
EDLCs characteristics
characteristics toto form
form a complementary
a complementary system
system [28].
[28].
Figure
Figure
Figure 66 compares
6 compares
compares the
the potential
the
potential window
potential window
window ofofEDLCs
of EDLCs
EDLCs and LiCs
and
and toto
LiCs
LiCs conclude
to that
conclude
conclude increasing
that
that increas-
increas-
the voltage
ing the will
voltage enhance
will the
enhance energy
the and
energy power
and densities
power as they
densities as carry
they a direct
carry
ing the voltage will enhance the energy and power densities as they carry a direct propor- a proportion.
direct propor-
The operation
tion. The voltage
operation window
voltage for
window two electrode
for two materials
electrode of LiCs
materials of is different
LiCs
tion. The operation voltage window for two electrode materials of LiCs is different since is since
different the
since
electrochemical
the electrochemicalmechanisms are
mechanisms different.
are Thus,
different. the voltage
Thus, the window
voltage is higher
window
the electrochemical mechanisms are different. Thus, the voltage window is higher than than
is EDLCs.
higher than
The negative
EDLCs. The electrode
negative of the LiC
electrode in
of the
the figure
LiC in is
the graphite,
figure is while the
graphite, positive
while
EDLCs. The negative electrode of the LiC in the figure is graphite, while the positive elec-the electrode
positive is
elec-
AC [28].
trode
trode is is
ACAC [28].
[28].
In general, EDLCs use AC for both electrodes. The electrolyte is composed of a salt of
tetraethyl methyl ammonium tetrafluoroborate (TEMABF4 ) in acetonitrile or propylene
carbonate. This commercial EDLC has a maximum voltage of 2.7 V. In contrast, LiCs contain
higher voltage ranges up to 4.0 V. Normally, higher voltages for LiC technology can be
obtained by setting appropriate materials for positive and negative electrodes. Therefore,
the energy density of LiCs is enhanced up to three times compared with EDLCs. In addition,
the selection of an electrolyte with a higher potential window leads to improvement of
the voltage range. For instance, the aqueous electrolytes of LiCs have voltages between
1.0–1.5 V, while the potential range for ionic liquids and organic electrolytes is up to 4.0 V
and 2.5–3.0 V, respectively.
Figure 6 compares the potential window of EDLCs and LiCs to conclude that increas-
ing the voltage will enhance the energy and power densities as they carry a direct propor-
tion. The operation voltage window for two electrode materials of LiCs is different since
Molecules 2022, 27, 3119 the electrochemical mechanisms are different. Thus, the voltage window is higher 6than of 22
EDLCs. The negative electrode of the LiC in the figure is graphite, while the positive elec-
trode is AC [28].
Figure 6. The potential comparison between EDLCs and LiCs [28].
Another essential parameter to enhance the energy density of LiCs is specific capaci-
tance, which can be influenced by the electrode’s extra redox capacitance, the electrolyte
and active material’s electrical conductivity, the electrolyte and active material’s pore size
distribution, and specific surface area [27]. It is worth mentioning that the specific ca-
pacitance calculation directly relates to the effective specific surface area. The effective
specific surface area is calculated by cumulative density functional theory. In this theory,
the diameter of the pores is larger than the ion in various electrolytes [29].
Thus, the fabrication of nano-porous structures with a highly effective surface area is a
practical approach to increasing energy density. In addition, introducing pseudo-capacitive
species with heteroatom doping enables to obtain extra redox capacitance, leading to
an increase in the LiC’s energy density. As was explained, the operating voltage bears
an impact on increasing the energy density, but to increase the power density, ESR is
another critical parameter in addition to the operating voltage. The main factors in the ESR
include the electrolyte and electrode’s conductivity, the electrode material’s rate of ions, the
electrode’s diffusion distance, and the contact resistance between the current collector and
electrode material. Increasing the effective specific surface area reduces the ESR resulting
in power density enhancement. Moreover, increasing the electrode material’s conductivity
and employing an aqueous electrolyte would also increase the power density [30].
3. 1D Electrical, Thermal, and Lifetime Modeling

LiC technology is employed at the system level regarding its applications, such as
automotive or stationary. Therefore, a holistic modeling approach is needed to extract its
electrical and thermal parameters, which will then be used for lifetime modeling [31], safety
assessment [32], cell equalization management [33], and thermal management [34]. For
example, an accurate electro-thermal model is required for electrical and thermal issues
in the developed management system [35]. Moreover, an accurate tool is needed for state
of charge (SoC) [36], state of health (SoH) [37], and state of power (SoP) to control the
LiC system [38]. The holistic model of the LiC that is applicable for real-time energy
management and control purposes is shown in Figure 7 [26].
olecules 2022, 27, x FOR PEER REVIEW
Molecules 2022, 27, 3119 7 of 22
Figure
Figure7. The
7. holistic model of the
The holistic LiC is of
model applicable
the LiC for real-time energy management
is applicable and control
for real-time energy ma
purposes [26].
purposes [26].
This section introduces a state-of-the-art review regarding electrical modeling, thermal
modeling, and lifetime modeling of LiCs. The LiC model that is developed should be
This section introduces a state-of-the-art review regarding electr
dedicated to a special aim since the goal of modeling is design, parameter identification,
malestimation,
state modeling, and lifetime
and control. modeling
In this regard, of LiCs.
some models, Theelectrical,
including LiC model that is d
thermal,
and lifetime models of LiC technology, are presented. The most developed models are
dedicated to a special aim since the goal of modeling is design, param
electrochemical [39], fractional-order [40], and equivalent circuit models (ECM) [41]. The
state
LiC’s estimation,
electrical parametersand control.
highly depend on Intemperature,
this regard,currentsome models,
rate, and including
SoC. In addi-
tion,
andalmost all of the
lifetime LiC’s characteristics
models change over the are
of LiC technology, cell’s presented.
lifetime [42]. Therefore,
The most a de
holistic approach should be considered for electrical, thermal, and lifetime modeling under
electrochemical
various [39], fractional-order [40], and equivalent circuit mod
operating conditions.
LiC’s electrical parameters highly depend on temperature, current rat
3.1. Electrical Modeling
tion, almost all of the LiC’s characteristics change over the cell’s lifetim
The first modeling method is the electrochemical model, which is counted as a power-
holistic
ful approach
tool considering both theshould be chemistry
physics and considered for[43].
interfaces electrical,
Although thermal,
electrochemi-and lif
cal
dermodels are accurate,
various their computational
operating conditions. time is high due to modeling of the reaction
process by partial differential equations (PDE), which hinders the applicability of these
models in energy management and real-time control [44]. Moreover, they can simulate the
3.1. trend
aging Electrical Modeling
of the cell (lifetime estimation) under various working conditions for different
ESSs [45,46].
The first
However, modeling
this requires method
a thorough is the
knowledge of electrochemical
the aging mechanism, model, which i
limiting the
applicability of such modeling tools. The most used electrochemical
erful tool considering both the physics and chemistry interfaces [43 modeling approaches
are the lumped parameter model [47] and porous electrode theory [48]. The first approach
chemical
uses models equations
differential-algebraic are accurate, their the
(DAE) to model computational time isinside
electrochemical phenomena high due
reaction
the processthebychemical
cell by considering partial differential
products equations
as a uniform (PDE),The
spatial distribution. which
secondhinder
approach uses PDE to define the electrochemical processes based on Fick’s law, Ohm’s law,
these
and models
the Nernst in energy management
and Butler–Volmer equations [49]. and real-time control [44]. Mor
ulate theother
On the aging
hand,trend
ECMs are ofdeveloped
the cellunder
(lifetime estimation)
certain conditions under various
from experimental
tests, applicable in real-time energy management owing to precision and simplicity [50].
for different ESSs [45,46].
They include RC networks (resistor–capacitor) and utilize ordinary differential equations
(ODE) to However, this requires
model the electrical behavior ofa LiC
thorough
cells [51]. knowledge
The main items of the aging
to enhance the mec
precision of ECMs are
applicability circuit configuration
of such modeling and component
tools. The most number [52].electrochemical
used The developed m
are the lumped parameter model [47] and porous electrode theory [48
uses differential-algebraic equations (DAE) to model the electrochem
side the cell by considering the chemical products as a uniform spat
Molecules 2022, 27, 3119 8 of 22
ECMs for the LiC technology are illustrated in Figure 8, in which Figure 8a shows the
simplest
Molecules 2022, 27, x FOR PEER REVIEW ECM, including a resistor for overall resistance and a capacitor for the known
9 of 24
capacitance impacts, connected in series [24].
Figure 8. The developed ECMs for the LiC technology [26]: (a) Rint, (b) Rint-Rp, (c) Advanced Rint-Rp,
Figure 8. The(e)developed
(d) Hybrid, ECMs for the
PNGV (Partnership for LiC
Newtechnology
Generation[26]: (a) Rint , (b)
of Vehicles), (f)RAdvanced
int -Rp , (c) Advanced
PNGV, (g)
RThevenin,
-R
int p , (d) Hybrid,
(h) 2-RC.(e) PNGV (Partnership for New Generation of Vehicles), (f) Advanced PNGV,
(g) Thevenin, (h) 2-RC.
The variations of capacitance and ESR are evaluated by performing some experi-
Figure 8b depicts a classical ECM for which a parallel resistor is added to the previous
mental tests. This model poorly reflects the LiC behavior in diffusion steps and charge
ECM to consider the self-discharge phenomenon [53]. Figure 8c illustrates the same
transfer, which is the main shortcoming of the first-order Thevenin model. Therefore, the
topology, in which the overall resistance was split up to the charge/discharge resistances,
second-order Thevenin model is proposed to cope with this problem to predict the LiC’s
while three capacitors (C0 , C1 , C2 ) are available in the model in parallel connection [54].
transient behavior [59]. This model is shown in Figure 8h. For almost all the mentioned
C0 , C1 , and C2 correspond to the initial LiC, capacitor variations at various currents, and
models, the parameters of the models significantly depend on temperature, current rate,
and SoC [60]. Moreover, the model’s number of RC branches defines its complexity [61].
If the parameters of ECMs are identified through experiments, the model is called a semi-
empirical model [62].
However, other approaches for modeling can be found in the literature [63]. Charac-
terization and parameter identification is the most significant step to develop an ECM
[64]. In this context, online and offline methods should be used to identify the electrical
Molecules 2022, 27, 3119 9 of 22
capacitor variations at different SoC values. Another critical parameter in the model is the
parallel resistance (Rp ) that is employed for the self-discharge phenomenon:
OCV 2 tdischarge
Rp = (3)
Whbe f ore − Wh a f ter
Whbe f ore and Wh a f ter , and tdischarge denote the available energy of the full-charged cell
before starting the test, the available energy after the cell is stored at 25 ◦ C for seven days,
and discharge time. The main drawback of this ECM is depiction of the cell dynamics
only for a short period of several seconds. Figure 8d demonstrates an ECM for power
electronics applications that consist of five parameters [55]. One of the model parameters
is the capacitance that depends highly on voltage variations to reduce the simulation
time. The influence of the internal resistance in series connection with the RC component
would be a variation of open-circuit voltage (OCV) at the end of each pulse. The internal
capacitance was replaced by a voltage source that is highly dependent on the SoC values
to update the model [56]. Figure 8e illustrates the FreedomCAR model that combines the
voltage source with the internal capacitor.
Figure 8f illustrates an advanced model of the FreedomCAR for which the current
direction is considered. The first-order Thevenin model is one of the most popular ECMs
used for various ESSs [57]. This ECM is seen in Figure 8g for LiCs [58].
The variations of capacitance and ESR are evaluated by performing some experimental
tests. This model poorly reflects the LiC behavior in diffusion steps and charge transfer,
which is the main shortcoming of the first-order Thevenin model. Therefore, the second-
order Thevenin model is proposed to cope with this problem to predict the LiC’s transient
behavior [59]. This model is shown in Figure 8h. For almost all the mentioned models,
the parameters of the models significantly depend on temperature, current rate, and
SoC [60]. Moreover, the model’s number of RC branches defines its complexity [61]. If
the parameters of ECMs are identified through experiments, the model is called a semi-
empirical model [62].
However, other approaches for modeling can be found in the literature [63]. Charac-
terization and parameter identification is the most significant step to develop an ECM [64].
In this context, online and offline methods should be used to identify the electrical and
thermal parameters of the cell. Offline methods use lookup tables to store the extracted
parameters [65], or the parameters should be fitted using fitting techniques [66]. Among
the offline methods, hybrid pulse power characterization (HPPC) [67] and electrochem-
ical impedance spectroscopy (EIS) [68] are the main approaches. As mentioned earlier,
the electrical parameters of an ECM highly depend on the SoC values. Therefore, SoC
estimation methods should be employed as well to characterize the cell [69]. Coulomb
counting method is one of the simplest SoC estimation methods with high accuracy that
uses charge and discharge capacity tests to calculate the cell’s capacity [70]. Nevertheless,
offline methods are incapable of including the temperature and aging conditions [71]. In
contrast, online methods extract the parameters in real-time operation [72]. Among the
online methods in the literature, the Kalman Filter (KF) [73], Extended KF (EKF) [74], Adap-
tive KF (AKF) [75], least square method (LSM) [76], Relevance Vector Machine (RVM) [77],
Support Vector Machine (SVM) [78], Neural Network (NN) [79], and Particle Filter (PF) [80]
are the most widely used.
The third modeling approach is the fractional-order model (FOM) developed to en-
hance models’ precision [81]. FOMs are non-integer order differential equations that can
better extract the parameters compared with the integer-order ECMs. Figure 9 illustrates
FOMs reported in the literature. Figure 9a demonstrates a basic FOM including a series and
a parallel resistance, a constant phase element, and a Warburg-lie element [38]. Figure 9b
depicts an ECM consisting of three components in series [82]. The impedance behavior of
the LiC is complex due to some kinetic steps. Thus, ZP was employed in this model. The
diffusion process and the porous nature of electrodes are the main factors for this trans-
Molecules 2022, 27, 3119 10 of 22
fer impedance. Figure 9c shows the same model with four parallel impedance branches
(ZP ) [83]. Figure 9d exhibits a developed FOM, in which the impedance is modeled by
considering the ambient temperature at various currents [84]. Figure 9e shows an enhanced
FOM regarding the influence of the cell’s temperature [85]. Figure 9f demonstrates an ad-
vanced FOM that models impedance behavior in the frequency domain that was validated
for low current rates [86].
Figure
Figure 9.
9. The
The developed
developed fractional-order
fractional-order models
models [26].
[26]. (a)a
(a) abasic
basicFOM,
FOM,(b)ECM with
(b) ECM three
with compo-
three compo-
nents in series, (c)the same ECM with four parallel impedance branches, (d)developed FOM, in
nents in series, (c) the same ECM with four parallel impedance branches, (d) developed FOM, in
which the impedance is modeled by considering the ambient temperature at various currents (e)
which the impedance is modeled by considering the ambient temperature at various currents (e) an
an enhanced FOM regarding the influence of the cell’s temperature, (f)an advanced FOM that
enhanced
models FOM regarding
impedance theininfluence
behavior of the domain.
the frequency cell’s temperature, (f) an advanced FOM that models
impedance behavior in the frequency domain.
3.2.
3.2. Lifetime
Lifetime Modeling
Modeling
The
The lifetime of
lifetime ofESSs
ESSshashasananessential
essentialimpact
impactononEVs, as the
EVs, totaltotal
as the cost,cost,
safety, and reli-
safety, and
ability of each
reliability EV EV
of each strictly depend
strictly dependon the
on lifetime of itsofESS
the lifetime [87].[87].
its ESS Thus, SoHSoH
Thus, estimation and
estimation
prediction
and prediction of the remained life of ESSs under real-time driving profiles represents es-
of the remained life of ESSs under real-time driving profiles represents an an
sential
essentialstep
steptoto
avoid
avoidissues
issues[88].
[88].Lifetime
Lifetimemodels
modelshave
havebeenbeendeveloped
developedin in the
the literature
literature to
to
evaluate
evaluate thethe long-term
long-term behavior
behavior of of ESSs [89,90]. Therefore,
ESSs [89,90]. Therefore, developing
developing aa precise
precise lifetime
lifetime
model
model is is of
ofhigh
highimportance
importancefor forESSs
ESSsthat
that aim
aim to to operate
operate under
under various
various working
working condi-
conditions
tions
for anforexpected
an expected duration.
duration. TheThe lifetime
lifetime model
model helpsestimate
helps estimatethetheESSs
ESSs characteristics
characteristics
and
and determine the most severe working conditions during their predicted lifetime
determine the most severe working conditions during their predicted lifetime [91].
[91].
For this aim, developing a robust lifetime model requires a thorough understanding of
aging processes and ESSs characteristics. Nevertheless, such comprehensive knowledge
to predict the lifetime of ESSs is feasible for a limited number of applications [92]. Thus,
understanding the main aging processes would be enough for lifetime modeling to pre-
dict the LiC’s end of life.
Molecules 2022, 27, 3119 11 of 22
For this aim, developing a robust lifetime model requires a thorough understanding of
aging processes and ESSs characteristics. Nevertheless, such comprehensive knowledge
to predict the lifetime of ESSs is feasible for a limited number of applications [92]. Thus,
understanding the main aging processes would be enough for lifetime modeling to predict
the LiC’s end of life.
Almost all the LiC characteristics such as impedance parameters and capacity change
over the lifetime of the cell. The main reason for this change is the aging of the cell under
calendaring or cycling [31]. LiCs suffer from ESR rise and capacity fade when are exposed
to calendaring and cycle aging processes. The main factors that influence the lifespan
of LiCs include the type of anode material, the pre-lithiation level, inconsistency of the
lithiated anode, and range of electrode potential [93]. The LiCs lifetime is reported as more
than ten years [94]. However, the mentioned factors highly impact the lifetime of LiCs. The
main factors that affect the degradation mechanism of LiCs are temperature, equivalent
number of cycles (eq-cyc), depth of discharge (DOD), and current rate in charging and
discharging scenarios. The main criteria to indicate the end of life degradation of LiCs are
capacity reduction for 20% and ESR increase for 100% [95]. El Ghossein et al. [96] evaluated
the aging mechanism of LiC for 20 months at high temperatures and various voltage levels,
but the lifetime model was not developed. A lifetime model based on accelerated aging
was developed that was capable of estimating the end of life. Nevertheless, the developed
lifetime model was not comprehensive as the impact of the current rate was not applied in
the modeling phases. Omar et al. [97] evaluated the impact of ESR growth and capacity
reduction and concluded that ESR has more influence than capacity.
As is seen, the number of research articles is limited in LiCs degradation mechanisms
and lifetime modeling, so an enormous potential can be seen here to fill this gap. The
effect of temperature on the LiC cell’s components, including electrode materials and the
electrolyte, should be investigated to thoroughly understand the impact of the operational
temperature on the LiC cell’s performance. The target LiC cell in this dissertation has
Lithium-Titanate-Oxide (LTO) as anode material. LTO is commonly used as the negative
electrode, which features good capacity [26]. LTO, as the LiB anode, has high interfacial
side reactivity with the electrolyte, which can lead to gas generation and poor cycling
stability [98].
Huang et al. [99] investigated the temperature dependence of LTO degradation in LiBs.
They have shown that the cell’s capacity retention would decrease at elevated temperatures;
LTO could deliver up to 87.1% capacity retention in low C-rates (1C, 60 ◦ C, 500 Cycles).
However, with raising the C-rate, the capacity retention had drastically dropped to 20.9%
(5C, 60 ◦ C, 500 Cycles). Considering that high C-rates are in the interest of LiC applications,
it is expected that controlling the temperature and keeping that in lower values could cause
the LiC lifetime’s amelioration. Within another investigation, Yang et al. [100] evaluated
the rate capability of LTO in a LiB cell at different temperatures from 0.5 ◦ C to 20 ◦ C and
depicted 35 ◦ C as the most efficient temperature for different C-rate values.
The electrolyte is also a vulnerable component against heat. Many common LiC elec-
trolytes are based on carbonate solvents. Handel et al. [101] investigated the effect of high
temperature on the degradation of pure Lithium-Hexafluoro-Phosphate (LiPF6 )/carbonate-
based electrolyte stored for 28 days at 60 ◦ C and demonstrated that the electrolyte’s total
impurity content had increased by about 2.5 times compared with the fresh electrolyte.
Smart et al. [102] also reported degradation of LiPF6/carbonate-based electrolytes at ele-
vated temperatures. To understand the aging factors, El Ghossein et al. [103] performed
calendar accelerated aging tests on LiC cells cycled at 70 ◦ C followed by a post-mortem
study and concluded that pore-blocking at the positive electrode could decrease the ca-
pacitance values of the LiC cell and the main aging mechanism of the positive electrode is
reported as the pore blocking of the activated carbon due to parasitic reactions between
the functional groups present on its surface and the components of the electrolyte. Accord-
ing to what was mentioned, it could be concluded that internal heat, which would raise
Molecules 2022, 27, 3119 12 of 22
the operating temperature, is the most crucial factor in the LiC’s lifespan. Therefore, the
application of LiCs requires a proper robust cooling system to extend the cell’s lifetime.
3.3. Thermal Modeling

All ESSs, including LiBs, EDLCs, and LiCs, produce heat during their operation [104,105].
Temperature is one of the most vital parameters that affect the performance of LiCs [106] by
causing irreversible effects, including accelerated aging [107], impurity production [108],
and solvent evaporation [109–111]. LiCs generate more heat with smaller ESR since they
have been used in high power applications under high current rates [112]. Therefore, the
lifetime and performance of LiCs significantly depend on their working temperature. In
this context, an accurate thermal model is quite essential to design an optimized system to
control the thermal behavior of LiCs [113]. An interdisciplinary knowledge of both thermal
and electrical fields is required to develop an optimized LiC management system [114,115].
This work aims to develop a holistic 1D electro-thermal model for LiC technology coupled
to 3D computational fluid dynamics (CFD) thermal model for further investigation of the
temperature behavior of LiCs.
3.3.1. Heat Transfer Modeling of LiCs

Before explaining the heat generation mechanism of LiCs, a thorough literature study
on the LiC thermal model development is of high importance. Heat transfer modeling
aims to determine the temperature evolution across the spatially discretized LiC, for which
the thermal and geometric characteristics were identified [116]. Various heat generation
types can be assumed, including conduction, convection, and radiation [117]. The heat
conduction equation specifies the conduction, which is employed to model the temperature
of the LiC’s surface and inside its layers [118]. In contrast, the dissipated heat from the
LiC surface to the environment is due to convection heat transfer [119], and finally, the
Stefan–Boltzmann law expresses the heat radiation [120].
This section deals with the heat transfer models developed for LiCs at the cell level or
module level. The general equation for the heat dissipation of batteries was explained by
Bernardi in 1985 [121]:
∂U
Ploss = I (OCV − Vt ) − I T (4)
∂T
where I [A], OCV [V], Vt [V], and ∂U∂T [V/K] represent current, open-circuit voltage (OCV),
the terminal voltage of the cell, and the entropy coefficient (U denotes the cell’s voltage).
The 1D thermal model for a cell stack was introduced by Pals and Newman in 1995 [122]:
∂2 T ∂2 T ∂2 T

dT
ρC p = λ x 2 + λy 2 + λz 2 + Ploss (5)
dt ∂x ∂y ∂z
where ρ [kg/m3 ] denotes the density, C p [J/kg·K] is the heat capacity, T [K] is the tem-
perature, λ [W/m·K] represents thermal conductivity, and Ploss [W/m3 ] represents the
volumetric heat generation. Then, the heat flux from the cell to the ambient can be ex-
pressed as:
∂2 T ∂2 T ∂2 T

− λ x 2 + λy 2 + λz 2 = h( T − Tamb )|boundaries (6)
∂x ∂y ∂z boundaries
where h [W/m2 ·K], T [K], and Tamb [K] represent the heat transfer coefficient, cell tempera-
ture, and ambient temperature. All the mentioned thermal parameters can be estimated
using various methods, including the empirical approach, the electrical model for thermal
behavior, and calorimetric evaluation. The first two methods have been used for LiCs, but
the last one has never been employed for LiCs. For LiC cells, Equation (7) was updated to
extract the thermal parameters of a 3300 F LiC [112]. Nevertheless, the heat source’s entropy
change was not included. The same method was employed for a 1500 F LiC to predict the
observed. Ts1, Ts2, Ts3, and Ts4 are the surface temperature for the lateral sides. Ts_back and
Ts_front are the surface temperature of the back and front sides. Tint and Ta are the internal
and ambient temperatures. Rth(i) and Rconv(i) are the thermal resistance from the middle
Molecules 2022, 27, 3119 13 of 22
point to side i, and convectional thermal resistance from side i to the ambient. The same
model has been used in another work for thermal conductivity calculations in various
directions for a prismatic 2300 F cell [123]. The extracted parameters were then utilized in
temperature of LiCs [58]. However, the model was unable to mimic the temperature of the
another work for temperature uniformity analysis of LiCs [6].
cell for charging and discharging.
It can be observed
An RC branch was used that
forathe
fewfirstmodels have[59]
time in LiCs developed
for thermala 1D thermalestimation
parameters model for LiCs.
However,
using the least their 1D fitting
square modelmethod.
has not been coupled
Reversible to a 3Dheat
and irreversible thermal
sources model to main
were the evaluate the
accuracy of the extracted
factor for temperature rise inparameters.
this empiricalOnly one study
approach. has developed
Nonetheless, a 1D model
the load profile was notcoupled
high,
to a 3Dshowing
thermal the applicability of the modelthe
model to investigate for thermal
high-power applications.of
performance Figure 10 depicts
a module of 12 LiCs
the RC abranch
under used to
forced-air predictsystem
cooling the thermal[124].behavior
However, of LiC
the3300 F cell.performance
thermal In the presented of the pro-
first-order
posed TMS thermal model, six branches
was investigated underofa lumped thermal rate
100 A current parameters
that isarenotobserved.
consideredTs1 , a high-
Ts2 , Ts3 , and Ts4 are the surface temperature for the lateral sides. Ts_back and Ts_front are the
power application for LiCs, as the temperature of the 2300 F prismatic LiC that was inves-
surface temperature of the back and front sides. Tint and Ta are the internal and ambient
tigated reaches around 40 °C after an hour of continuous operation. Therefore, a high cur-
temperatures. Rth(i) and Rconv(i) are the thermal resistance from the middle point to side
rent rate should bethermal
i, and convectional appliedresistance
to such afrom cell side
to obtain theambient.
i to the highest The
peak samepower deliverable
model has by
the
been2300
usedFinLiC cell. work for thermal conductivity calculations in various directions for a
another
prismatic 2300 F cell [123].isThe
The LiC structure made for heavy-duty
extracted parameters were applications, where
then utilized high power
in another work is de-
manded. Therefore,
for temperature TMS analysis
uniformity development of LiCsand[6]. modeling are indispensable to ensure the safe
and Itreliable
can be observed
operationthat of asuch
few models have developed
technology. a 1D thermal
Another critical modelconcerning
challenge for LiCs. LiCs
However, their 1D model has not been coupled to a 3D thermal
would be the temperature non-uniformity, which is the main reason for electrical model to evaluate the imbal-
accuracy of the extracted parameters. Only one study has developed a 1D model coupled
ance and SoC mismatch among the module cells [39]. Therefore, special attention should
to a 3D thermal model to investigate the thermal performance of a module of 12 LiCs under
be given in designing a robust 3D thermal model to manage the temperature rise of LiCs
a forced-air cooling system [124]. However, the thermal performance of the proposed TMS
during high charging
was investigated under aand 100 A discharging.
current rate that Table 1 lists
is not all the adeveloped
considered high-power3D models for LiC
application
cells. As can
for LiCs, as thebetemperature
observed, there of theis2300
a massive potential
F prismatic in 3D
LiC that wasthermal modeling
investigated for LiCs in
reaches
high-power ◦
around 40 C applications.
after an hour of As is seen inoperation.
continuous the literature studyaof
Therefore, LiCs,
high the 3D
current ratethermal
should behav-
ior of the LiC
be applied to suchcellaiscell
notto analyzed and optimized
obtain the highest peak power comprehensively.
deliverable by the 2300 F LiC cell.
Figure 10.The
Figure 10. TheRCRC branch
branch usedused to predict
to predict the thermal
the thermal behaviorbehavior of FLiC
of LiC 3300 cell 3300 F cell that
that consists consists of
of four
four lateral sides (S 1, S2, S3, and S4) front and back sides [59,125].
lateral sides (S , S , S , and S ) front and back sides [59,125].
1 2 3 4
Molecules 2022, 27, 3119 14 of 22
The LiC structure is made for heavy-duty applications, where high power is demanded.
Therefore, TMS development and modeling are indispensable to ensure the safe and reliable
operation of such technology. Another critical challenge concerning LiCs would be the
temperature non-uniformity, which is the main reason for electrical imbalance and SoC
mismatch among the module cells [39]. Therefore, special attention should be given in
designing a robust 3D thermal model to manage the temperature rise of LiCs during high
charging and discharging. Table 1 lists all the developed 3D models for LiC cells. As can
be observed, there is a massive potential in 3D thermal modeling for LiCs in high-power
applications. As is seen in the literature study of LiCs, the 3D thermal behavior of the LiC
cell is not analyzed and optimized comprehensively.
Table 1. The developed 3D models for LiCs in the literature with their type of TMS.
Ref. Application Cell/Module Active Passive Hybrid

[123] Thermal behavior analysis Cell - X -
[126] Cooling system design Cell - X -
[124] Cooling system design Module X - -
[127] Cooling system design Cell & Module - X -
[128] Cooling system design Cell X - -
[129] Uniformity analysis Cell - X -
Cooling system design,
[131] Cell X X X
uniformity analysis
[42] Lifetime analysis Cell X X -
[132] Cell - X X
uniformity analysis
Holistic 1D/3D model,
[133] Cell - X X
cooling system design
[134] Cell & Module X - -
uniformity analysis
[135] Cell & Module X - -
uniformity analysis
[136] Cell & Module X X X
uniformity analysis
3.3.2. Heat Generation Mechanism of LiCs

A summary of heat generation modeling methods for LiCs is listed in Table 2. By
assuming the heat generation as non-uniform, the heat generation process can ideally be
described by PDEs [138]. Nevertheless, solving such equations would be computationally
inefficient since obtaining the microscopic parameters requires structural and material
knowledge. On the other hand, by assuming the heat generation as uniform, the heat
generation calculation is more straightforward since acquiring the equivalent macroscopic
parameters is easier than the non-uniform heat generation [139]. Thus, uniform heat
generation assumption is more suitable to investigate the EESs, since the heat flux per area
has not been changed and our method is constant heat flux.
Molecules 2022, 27, 3119 15 of 22
Table 2. The heat generation estimation methods for LiCs in the literature.
Heat Generation Heat Generation

Ref. Advantage Disadvantage
Mechanism Assumption
Low computational effort, easy
[34] Irreversible heat Uniform Low Precision
parameters extraction
High precision, heat Heavy computational effort,
[140] Reversible heat Non-uniform
distribution description good harder parameter extraction
[121] Reversible heat Uniform Low Precision
High precision, heat Heavy computational effort,
[140] Reversible heat Non-uniform
distribution description good harder parameter extraction
During the operation of LiCs, the temperature varies due to ion migration. This ion
activity inside LiCs should be defined to measure the quantity and distribution of the
heat generation. All the influenced factors in the heat generation of the LiC cell should
be considered to develop a precise model to be able to estimate the electrical and thermal
parameters of the cell. Moreover, the model should be able to estimate the end of life of the
LiC since its lifetime is long and hard to reach within the experimental tests.
Based on the Bernardi equation [121], the generated heat of the cell incorporates the
Joule loss, side reaction loss, and electrochemical reaction loss. The side reaction loss is
neglected when the cell operates at reasonable temperature conditions [141]. To model the
heat generation of the LiC, it should be considered that the cell’s generated heat consists of
irreversible heat and reversible heat. The first part arises from the internal resistances of the
electrolyte, electrodes, and collectors. In contrast, the second part stems from the entropy
change of ions, plus Faradaic and non-Faradaic reactions [142]. In LiCs, the proportion
of the reversible heat source is more extensive than the irreversible heat source due to
Faradaic reactions, thus it cannot be neglected. In contrast, the proportion of reversible heat
in EDLCs is significantly smaller than irreversible heat sources so that it can be neglected
in the heat generation equations [125]. This would be the main difference between EDLCs
and LiCs in terms of heat generation modeling. Thus, the Bernardi equation for LiCs can
be written as:
. . ∂U
Ploss = qirr + qrev = I (OCV − Vt ) − I T (7)
∂T
As the temperature distribution of LiCs is non-uniform, the LiC’s heat sources are used
separately for the tab domain and the cell domain. Equation (8) explains the heat source
equation for the cell domain. For the tab domain, the heat generation can be explained
as follows:
R I2
Ploss = (8)
Vtab
l
R = ρ0 (9)
S
where R [Ω], I [A], Vtab [V], ρ0 [Ωm], l [m], and S [m2 ] denote the tab resistance, current,
volume, resistivity, length, and cross-sectional area.
4. Application of LiCs
Currently, LiCs are employed for different applications such as electric vehicles
(EVs) [143], flywheels for pulsed power applications [144], lightweight transportation
systems [145], wind power plants [146], photovoltaic (PV) panels [147], power electron-
ics [82], grid applications [55], railways [148], spacecraft and satellites [149], and power
conditioning units (PCU) [150]. One of the most promising technologies counted as the
Molecules 2022, 27, 3119 16 of 22
end-user of LiC technology is the regenerative braking system (RBS), which collects energy
from the braking of EVs or HEVs, trains, trams, and other types of automotive vehicles, as
shown in Figure 11. The RBS bears low capabilities to restore the braking energy due to the
limits of LiBs and EDLCs. However, LiCs can help this system regenerate and store higher
amounts of energy for delivery to the vehicle’s traction based on the driver’s demand.
Figure The
11.11.
Figure Energy
The flow
Energy with
flow and
with without
and RBS
without [151].
RBS [151].
5. Conclusions
5. Conclusions
In this review paper, the working principle of LiBs, EDLCs, and LiCs was presented,
focusingIn this
on thereview paper,
storage the working
mechanism andprinciple
chemicalof LiBs, EDLCs,
structure andThen,
of LiCs. LiCs was presented,
the literature
focusing on the storage mechanism and chemical structure of LiCs. Then,
review was presented regarding the electrical, thermal, and lifetime models developed the literature
for
review was presented regarding the electrical, thermal, and lifetime models
LiCs. Various modeling methodologies, including the electrochemical modeling method, developed for
LiCs. Various modeling methodologies, including the electrochemical
equivalent circuit models (ECM), and fractional order models (FOM), were listed for modeling method,
equivalent
electrical circuit
model models (ECM),
development. andfactors
Aging fractional
and order modelsmechanisms
degradation (FOM), wereof listed
LiCsfor elec-
were
reviewed for the lifetime model development. Thermal model development, includingre-
trical model development. Aging factors and degradation mechanisms of LiCs were
viewed
1D/3D for themodels,
thermal lifetime model
were development.
reviewed, and heatThermal model development,
transfer modeling including
and heat generation
1D/3D thermal
mechanisms models,
of LiCs were were reviewed,
presented. In theand
end,heat
the transfer modeling
application of LiCsand
washeat generation
introduced.
mechanisms of LiCs were presented. In the end, the application of LiCs was introduced.
Author Contributions: Conceptualization, methodology, formal analysis, investigation, writing—
Authorjournal
original Contributions: Conceptualization,
draft by D.K.; writing—review methodology,
and editing formal
by H.B.;analysis, investigation,
supervision, writing—
writing—review
original
and journal
editing draft and
by J.V.M. by D.K.;
M.B.writing—review
All authors have and editing
read and by H.B.;tosupervision,
agreed writing—review
the published version of
and
the editing by J.V.M. and M.B. All authors have read and agreed to the published version of the
manuscript.
manuscript.
Funding: This research received no external funding.
Funding: This research received no external funding.
Institutional Review Board Statement: Not applicable.
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: Not applicable.
Data Availability Statement: Not applicable.
Acknowledgments: We acknowledge Flanders Make for supporting the MOBI group.
Acknowledgments: We acknowledge Flanders Make for supporting the MOBI group.
Conflicts of Interest: The authors declare no conflict of interest.
Conflicts of Interest: The authors declare no conflict of interest.
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molecules

1 Research Group MOBI—Mobility, Logistics, and Automotive Technology Research Centre,

Molecules 2022, 27, 3119. https://doi.org/10.3390/molecules27103119 https://www.mdpi.com/journal/molecules

2. Various Types of Energy Storage Systems

2.2. Electric Double-Layer Capacitors (EDLCs)

Molecules 2022, 27, x FOR PEER REVIEW 3 of 24

Figure 6. The potential comparison between EDLCs and LiCs [28].

3. 1D Electrical, Thermal, and Lifetime Modeling

3.3. Thermal Modeling

3.3.1. Heat Transfer Modeling of LiCs

Ref. Application Cell/Module Active Passive Hybrid

3.3.2. Heat Generation Mechanism of LiCs

Heat Generation Heat Generation

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