Journal of The Electrochemical Society, 166 (10) A1769-A1778 (2019) A1769

0013-4651/2019/166(10)/A1769/10/$38.00 © The Electrochemical Society

A Numerical Study of the Effects of Cell Formats on the Cycle Life

of Lithium Ion Batteries
Hong-Keun Kim,1 Jin Hyeok Choi,2 and Kyu-Jin Lee 3,z

1 Dept. of Mechanical & Aerospace Engineering, Seoul National University, Seoul 151-744, Korea
2 Korea Electric Power Corporation, Yuseong-gu, Daejeon, Korea
3 Department of Mechanical Engineering, Myongji University, Yongin 448-728, Korea

The effect of cell format on the imbalance and degradation of Lithium Ion Batteries is investigated using a three-dimensional model
that solves thermal-electrical-electrochemical-coupled physics. A pouch cell, a cylindrical cell and a prismatic cell are modeled to
have the same capacity, the same volume and the same electrode design. Highly nonuniform behavior is observed in the cylindrical
cell due to large electrical resistances in the current collectors and to poor heat transport in the radial direction. Degradation of the
cylindrical cell is also the fastest among the three cells due to the elevation of its cell temperature by the high joule heat generation
and small surface area. The prismatic cell shows the least imbalanced response, and the pouch cell takes advantage of a large cooling
area for degradation. Additionally, the model results for the cells with the continuous tab show that accelerated degradation caused
by the cell design can be considerably mitigated by improving the electrical configuration.
© 2019 The Electrochemical Society. [DOI: 10.1149/2.0261910jes]

Manuscript submitted October 24, 2018; revised manuscript received May 12, 2019. Published May 31, 2019.

As the market for electric vehicles (EVs) or hybrid electric vehicles
(HEVs) has increased in the recent decade, the size and capacity of
a commercial lithium-ion battery (LIB) system have also grown. The
large-format LIB is considered favorable for the HEV or EV systems
because modules or packs with large LIB cells can include fewer ter-
minal connectors and electrical components so that manufacturers can
achieve high energy density at the system level. However, as the LIB
size increases, cell design factors, such as cell shape, tab configuration,
and cooling condition, which have negligible influence in small LIBs,
have shown unexpected response. These cell design factors often cause
high temperature, nonuniform electrical potentials and localized elec-
trochemical reaction in the cell volume, resulting in poor performance
or short life.1–2 Therefore, it is difficult to successfully utilize large
LIBs without understanding the influence of the cell design factors,
even though the electrochemistry for lithium-ion batteries guarantees
good performance, cost and life.
Three major cell formats are used in the current commercial LIB
market: pouch cell, cylindrical cell and prismatic cell. Pouch cells have
stacked layers of electrode-separator-metal current collector compos-
ite connected to electrical tabs in a parallel manner, enclosed by film-
type pouches. Pouch cells have been known to be favorable for heat
management because of the large cooling area and advantages for
packing in modules due to their thin and flat geometries.3 However,
poor durability of the plastic film pouch and low yields from com-
plex manufacturing processes are weak points for using pouch cells.
Cylindrical cells have wound layer structures inside cylindrical metal
cans with good mechanical rigidity. Cylindrical cells are relatively
cost effective due to fast manufacturing processes and are mechani-
cally strong. However, the cylindrical geometry is known to be disad-
vantageous for large cells due to the small surface area per volume.
Additionally, poor thermal conductivity in the radial direction makes
heat management even more challenging. Prismatic cells combining
the benefits of pouch cells and cylindrical cells have wound layer struc-
tures of electrode-separator-metal current collector in prismatic metal
cans. Prismatic geometries allow small dead volumes in modular sys-
tems and a relatively large surface area for cooling. For current EV or
HEV systems, these three-cell formats are widely used: in numerous
small cylindrical cells (18650 type) in the Model S of Tesla, in pouch
cells in GM Golf, and in prismatic cells in BMW i8. No optimized stan-
dard cell format has been proposed in the current automobile market
due to the distinct pros and cons of each cell format. Understanding
of the relationship between cell format and cell behavior has been
lacking. To satisfy the performance, life and cost demand of electric
vehicles, the cell format should be optimized for the large-capacity
z
E-mail: kjlee@mju.ac.kr
systems based on knowledge of the effects of cell geometry on cell
behavior.
To investigate the effects of various cell formats, numerical ap-
proaches have advantages. Complex manufacturing processes for large
cells are difficult to conduct in laboratory-scale experiments, and para-
metric studies for cell designs can be very cost-effective in simulations.
There have been Multiphysics models to predict the behavior of small
LIB cells. A pseudo 2-dimensional model proposed by the Newman
Group mathematically describes the dominant phenomena such as
lithium diffusion transport and charge conservation in a porous elec-
trode inside the lithium-ion battery.4–6 This model has been widely
adopted since it can calculate nonlinear responses of the LIB quite
accurately. However, this model assumes uniform electric potentials
at current collectors and constant temperature to set limits for pre-
dicting the behavior of large-format LIBs. Multidimensional models
including cell geometries have been developed to estimate electrical-
electrochemical-thermally coupled behaviors of large LIBs. Kwon7
and Kim8,9 used a two-dimensional thermal model to solve poten-
tial and current density fields in a large-format LIB, but the model
results were valid for specific load profiles because the electrochem-
ical reaction parameters were fitted from empirical data in certain
DOD (depth of discharge) ranges. Jung2 proposed a multidimensional
model for large LIBs based on an equivalent circuit model (ECM) and
an empirical degradation model. A multiscale multidomain (MSMD)
framework suggested by Kim10 includes three independent modeling
domains to resolve the dominant physics in different length scales
and thus efficiently computates physics-based models for large LIBs.
Guo11 developed a reduced order model (ROM) by applying a lin-
ear approximation to the MSMD model and reduced the calculation
time.
Several degradation models have been suggested based on the
Newman approach. Many of the models calculate degradation by con-
sidering growth of the SEI layer on anode surfaces during the charg-
ing process. Ramadass12 and Ning13 modeled the development of the
SEI layer, limiting kinetic reactions and capturing active lithium irre-
versibly. Diffusion limitation of electrolytes inside the SEI layers was
modeled by Ploehn,14 and Safari15,16 added to the SEI layer growth
model. Yang17 suggested an aging model to simultaneously calculate
lithium plating and SEI layer growth. Awarke18 expanded the SEI layer
growth model for a large pouch cell in three dimensions and observed
effects of nonuniform electric currents on degradation.
Recently, three-dimensional modeling of the batteries is available
through several commercial software such as STAR CCM, COMSOL
and ANSYS. However, it is not easy to use the commercial software
to simulate the response of the wound type cells such as cylindrical
cells or prismatic cells because the wound geometry requires many
computational nodes and long calculation time. Thus, prediction of

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 A1770 Journal of The Electrochemical Society, 166 (10) A1769-A1778 (2019)

the long-term life response of the wound type cells in affordable cal-
culation time is hardly achievable for the commercial software.
To date, the effect of cell shape on cell behavior has been reported
in several reports. A few studies reported that pouch-type cells suffer
from large electric potential gradients and high temperature in near-tab
regions because electrical currents in current collectors converge near
the narrow tabs.8–11 Kim et al.10 simulated pouch cells with different
shapes and showed significant effects of the cell design on the imbal-
ance of electrochemical reaction rate and temperature. Awarke et al.18
and Kim et al.19 also conducted a modeling analysis to investigate
effects of nonuniform electric currents in a large-format pouch cell
and found that high temperatures near the tabs accelerate cell degra-
dation. However, compared to the number of studies on pouch cells,
the number of reports on cylindrical or prismatic cells having wound
structures has been small. Lee et al.20 developed a wound cell model
that can resolve electrical paths along wound current collectors to sim-
ulate discharging cases of a 20 Ah cylindrical cell with different tab
designs and found that the number of tabs and electrical paths along
the current collectors has significant effects on cell output voltage and
imbalance over the cell volume. Zhao21 and Cleary et al.22 also in-
vestigated a cylindrical and prismatic wound cell by using numerical
models and showed that current density and temperature are strongly
coupled in those cells and that tab configurations affect cell response.
The effects of the electrical tab designs on cell imbalance have been
detected in experiments showing that cell degradation becomes more
severe in LIB cells with fewer electrical tabs.23
We have known that, for large-format LIBs, the choice of cell de-
sign among the three different types, pouch cell, cylindrical cell and
prismatic cell, determines the nonuniform phenomena affecting cell
performance and life. However, noncomparative studies have shown
how much cell degradation is accelerated in a specific cell shape. This
study investigates the effects of cell shapes on imbalance and degrada-
tion by simulating three cells that have different shapes but an identical
electrode design such as material or capacity.
The simulation is conducted by a three-dimensional model includ-
ing an electrical, electrochemical, and thermal calculation.

Mathematical Model
The MSMD framework10 used in this study solves coupled physics
behavior in the large-format LIB. Three computational domains,
which are particle domain, electrode domain, and cell domain, are
separated in the MSMD for computational efficiency. Each model do-
main has different geometries and independent coordinate systems,
as shown in Fig. 1. In the hierarchical structure of the model do-
mains, the microscale physics such as electrochemical reactions at
the electrode surface are calculated in the lower domain, while the
macroscale physics such as heat transport are resolved in the upper
domain. Solution variables in each independent domain are solved
in a coupled manner by exchanging information between neighboring
domains in the hierarchy. The model developed in this study includes a
full-physics model proposed by the Newman group to be the lower hi-
erarchical model in the particle domain and the electrode domain. For
the cell domain, three cell models are established to adapt the differ-
ent cell formats: pouch, cylindrical and prismatic cells. All governing
equations in each submodel are summarized in Table I. Figure 1. Model domains in the MSMD framework and calculations of the
physics in each domain.
Particle domain model and electrode domain model.—The par-
ticle domain submodel adapts a 1D spherical particle model in which
all active material particles in the electrodes are considered to be
spherical. In this submodel, lithium transport in the solid active
materials and charge transfer reactions taking place at the interface carbonate(EC) and lithium ions in the negative electrode. The rate of
between the active materials and electrolyte are calculated. Heat SEI formation is calculated by making several assumptions: 1) the side
generation is considered from the electrochemical reactions to the reaction follows the Tafel equation (Eq. 3 of Table I), 2) there is no
entropy change of the active materials.24 The particle domain also en- limitation for consuming lithium and electrolyte in the liquid phase,
gages the aging mechanism, modeling the SEI layer development in 3) the electrolyte molecules are transported through the SEI layer by
the anode material based on the calculation of the parasitic reaction diffusion, as shown in Eq. 4 of Table I, and 4) the lithium loss is irre-
rate.25 The SEI growth is considered as formation of lithium ethylene versible, 5) lithium ions in the electrolyte are not directly involved in
dicarbonate(CH2 OCO2 LI)2 by the parasitic reaction between ethylene the side reaction.

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 Journal of The Electrochemical Society, 166 (10) A1769-A1778 (2019) A1771

Table I. Solution variables and governing equations of the sub-models.

Domain Solution Variable Governing Equation Boundary Conditions

1D spherical particle model

∂cs Ds ∂ 2 ∂cs ∂cs ∂cs 
Particle domain (X,Y,Z cs (r, x, X, Y, Z) ∂t = r 2 ∂r
(r ∂r ) (1) ∂r |r=0 =0 ∂r |r=Rs = − Dis F
for SPPC) (R,θ,Z for cs (r, x, R,θ, Z)
WPPC) i r (r = rs , x, X, Y, Z) i = i r + i para (1), η = ϕs + ϕe − Uocv − i RSE I (For negative)
i r (r = rs , x, R,θ, Z) ir = F ki (ce )αa (cs,max − cs,e )αa (cs,e )αc η = ϕs + ϕe − Uocv (For positive)
× {exp[ αRT aF
η] − exp[ αRT cF
η]} (2),
i para = −i para,init ex p[− αRT
cF
η para ](i para,init = Fk0,SE I CsEC ),
ηpara = ϕs + ϕe − Upara − i Rpara (3)
CsEC −C0EC −i para ∂δSE I i para MSE I δSE I
−DEC δSE I = F (4), ∂t =− ρSE I F (5), RSE I = κSE I (6)
1D porous electrode model
∂ (εe ce ) ∂ ∂ +  1−t 0
i e +  ∂t 0 ∂ce ∂ce
Electrode domain (X,Y,Z ce (x, X, Y, Z) ∂t = ∂x e ∂x ce ) + F j x − F ∂x (7)
(Deff ∂x |x=0 =0 ∂x |x=la+ls+lc =0
for SPPC) (R,θ,Z for ce (x, R,θ, Z)
∂ eff ∂ ∂ eff ∂  ∂ϕe ∂ϕe
WPPC) ϕe (x, X, Y, Z) ∂x (κ ∂x ϕe ) + ∂x (κD ∂x lnce ) + j x = 0 (8) ∂x |x=0 =0 ∂x |x=la+ls+lc =0
ϕe (x, R,θ, Z)
∂ eff ∂  ∂ϕs,a
ϕs,a (x, X, Y, Z) ∂x (σ ∂x ϕs ) − j x = 0 (9) ϕs,a |x=0 = − ∂x |x=la =0
ϕs,c (x, X, Y, Z) ∂ϕs,c
∂x |x=la+ls = 0 ϕs,c |x=la+ls+lc = +
ϕs,a (x, R,θ, Z)
ϕs,c (x, R,θ, Z)
3D Single Pair Potential Continuum (SPPC) model for Pouch cell
(ε− σ− ∂∂X2 + ε− σ− ∂∂Z2 + j − ) = 0 (10)
2 2
Cell domain − (X, Y, Z)

(ε+ σ+ ∂∂X2 + ε+ σ+ ∂∂Z2 + j + ) = 0 (11)

2 2
+ (X, Y, Z)
∂ (ρCP T) ∂ T ∂ T ∂ T  2 2 2
T(X, Y, Z) ∂t = (kX ∂X 2 + kY ∂Y2 + kZ ∂Z2 ) + q  (12)
3D Wound Pair Potential Continuum (WPPC) model for Cylindrical and Prismatic cell
( ε−Rσ− ∂∂θ ∂2
2
− (R,θ, Z) 
Cell domain 2 + ε− σ− ∂Z2 + j − ) = 0 (13)

( ε+Rσ2+∂2
+ ε+ σ+ ∂∂Z2 + j + ) = 0 (14)
2
+ (R,θ, Z) ∂θ2
∂ (ρCP T) ∂ ∂T kin ∂ 2 T ∂ T 2

T(R,θ, Z) ∂t = ( R1 ∂R (ktr R ∂R )+ R2 ∂θ2
+ kin ∂Z 2 ) + q  (15)

The electrode domain model adapts a 1D porous electrode model
for resolving the electrochemical behavior across the anode electrode,
the separator and the cathode electrode. The electrode domain sub-
model is regarded as a one-dimensional problem by assuming that
the solid matrix electrodes are a composite mix of active material,
conductors and binders are homogeneous. The lithium-ion transport
in the liquid electrolyte (Eq. 7), the charge conservation in the elec-
trolyte (Eq. 8) and the solid electrodes (Eq. 9) are calculated in the
electrode domain. Joule heat due to electrical currents flowing through
the solid matrices calculated in the electrode domain is summed up
with heat generating from the lower domain (the particle domain) and
then transferring to the upper domain (the cell domain).
Cell domain model.—The cell domain submodel resolves the
macroscopic physics with characteristic lengths of the cell volumes
such as electrical potential fields in metal current collectors and tem-
perature distribution. To solve the electrical potentials in the positive
and negative current collectors, the design of the electrical tabs is con-
sidered the boundary conditions for Eqs. 10, 11, 13, 14) of Table I, and
the structure of the metal current collectors is also modeled to reflect
electric current paths. The temperature distribution is calculated from
the cooling condition of the cell and the heat sources in Eqs. 12, 15
of Table I. The heat generated in the cell domain by ohmic resistance
of the current collectors is summed up with the heat transferred from
the lower domains (the electrode domain).
In this study, individual cell domain models for each cell format are
developed and applied to the MSMD model framework. The pouch
cell having a stacked structure of electrodes and current collectors
has a single potential-pair continuum (SPPC) model that counts a
single pair of electric potential and a single temperature in an arbitrary
finite volume of the cell.10 The single potential-pair continuum can be
implemented for the pouch cell where the difference of the electric
potential fields between the neighboring metal current collectors is
relatively small. The SPPC model also assumes orthotropic thermal
conductivities in the homogeneous cell volume, as shown in Fig. 2. Due
to the assumptions of the continuum, the computational mesh in the
cell domain model can be generated by ignoring the layer structures;
therefore, the better computational efficiency can be achieved.
For the cylindrical cell and the prismatic cell, the cell domain mod-
els are developed with a wound potential-pair continuum (WPPC).20
In a cylindrical cell and a prismatic cell having a wound structure of
electrodes and current collectors, the long and wide electrical paths
can appear in the winding direction of the current collectors, and an
electrical potential of neighboring current collectors cannot be consid-
ered to be similar. Thus, the wound potential-pair continuum counts
a single pair of electric potential and a single temperature for a finite
cell volume containing a single pair of current collectors. Due to the
restraint for generating the mesh of the wound layer structure, the
WPPC loses some of the computational efficiency. Detailed informa-
tion about the MSMD model framework and the cell models of SPPC
and WPPC is available in Refs. 10 and 20.
Results and Discussion
By using the multidimensional model, three different types of
large-format LIBs with 20 Ah are simulated, as shown in Fig. 1. The
pouch cell model has the same features as the reference cell that is a
commercial cell with NCM/Graphite (20 Ah, Top battery Korea), and
the detailed information of the electrode design of the reference cell
is also emulated by the model, as shown in Table II. The size of the
pouch cell is 185 mm×147 mm×5.74 mm, and the electrical tabs with
a width of 45 mm are located on the same side, as shown in Fig. 2a.
Since there is no actual reference cell whose shape is cylindrical or
prismatic and the electrode design is also identical to that of the pouch
cell, the cylindrical cell model and the prismatic cell model are set to
have similar shapes as those in the commercial market. The cylindrical

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 A1772 Journal of The Electrochemical Society, 166 (10) A1769-A1778 (2019)
Figure 2. a) Geometries of the three cell models, b) tab configurations and c) tab locations in the unrolled cylindrical and prismatic cells.
cell has an outer diameter of 44 mm, an inner diameter of 8 mm and a
height of 110 mm. A pair of current collectors is wound 43 turns, and
the length of the unrolled cell is approximately 3.49 m. The locations
of the electrical tabs with a 10 mm width are distributed at uniform
distances along the unrolled current collectors, and the locations of 8
positive tabs are set to be on the top sides, while 8 negative tabs are on
the bottom sides, as shown in Fig. 2c. The prismatic cell has a size of
100 mm×22 mm×80.45 mm, 25 turns of the wound current collec-
tors and an unrolled length of approximately 4.5 m. The electrical tabs
20 mm in width are located on the same side as the current collectors,
as shown in Fig. 2b. The cell models exclusively consider the volume
of the electrode composite, the so-called jelly roll, neglecting con-
tainers and electrically connecting components such as the outer film
of the pouch cell, the metal can of the cylindrical cell, and the metal
connectors. For the pouch cell, the convective cooling conditions are
applied on the top and bottom surfaces with a heat transfer coefficient
of 25 W/m2 K and an ambient temperature of 25°C. For the cylindrical
cell and the prismatic cell, the side surface excluding the top and bot-
tom faces is cooled by convection. The pouch cell has a surface cooling
area of 0.054 m2 , which is approximately 3∼4 times larger than those
of the other cells (0.015 m2 for the cylindrical cell and 0.018 m2 for
the prismatic cell). The numbers of the computational nodes in the cell
domains are approximately 2000 for the pouch cell and approximately
10000 for the cylindrical and the prismatic cell. Since a single node
in the cell domain has 25 electrode domain nodes and a single node in
the electrode domain has 10 particle domain nodes, the total numbers
of the computational mesh are approximately 240,000 for the pouch
cell and approximately 1,200,000 for the cylindrical and the prismatic
cell. The multidimensional model in this study was solved by the fi-
nite volume method, the Gauss-Seidel method and implicit scheme.
Also, to reduce computation time, the calculations were performed by
OPENMP parallel computing.
Model parameter calibration.—Before the comparison of the
three cell models is made, the model parameters of the particle do-
main model and the electrode domain model are calibrated by the
measured data of the pouch cell by a battery cycler (MACCOR, series
4000). During the test operation, the temperature in the environmental
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chamber is set to 25°C and the cell temperature is almost steady and
uniform because a highly convective condition is applied on the large
surface of the pouch cell. Fig. 3a shows the comparisons of the output
voltages of the measured data with the simulation results during con-
stant current discharging at 1C, 2C, 3C, 4C, 5C and 10C. Ion diffusivity
in the solid phase and kinetic reaction coefficients in the electrode do-
main model, which are difficult to determine experimentally, are fitted
by the test data. Ion diffusivities in the solid phase are determined to
be 1.35e−14 m2 /s in the anode and 8e−14 m2 /s in cathode, which are
similar (in the ranges of 10−14 to 10−15 m2 /s for the anode and 10−13 to
10−14 m2 /s for the cathode) to values in the literature.26–28 Kinetic re-
action coefficients for both electrodes are determined to be 6e-11m/s,
which are similar (order of 10−11 m/s) to values in the literature.13,15
The cycling test data for 1200 cycles are measured to calibrate
the aging parameters. The operating cycle includes 5 stages: constant
current discharge at 4C rate (80A) with a cutoff voltage of 2.8 V,
rest for 30 minutes, constant current charge at 4C rate (80A) with a
cutoff voltage of 4.2 V, constant voltage charge until the charge current
becomes less than 0.05C (1A), and rest for 30 minutes. The capacity
retention of the simulation results and test data are plotted in Fig. 3b,
and the output voltage curves at discharge stages during the cycle
operation are compared in Fig. 3c. The exchange current density for
the parasitic reaction of Eq. 3 is estimated at 2.05e−7 A/m2 , which is
within the range of 10−8 to 10−6 A/m2 reported in the literature.13,18
The activation energy parameter related to temperature effects is also
chosen from literatures.20,30 The other aging parameters calibrated are
shown in Table II.
Effects of cell formats on performance.—The responses of the
three cells at constant current discharge conditions are compared by
the simulation results. The voltage curves and the average-temperature
profiles for discharges at 1C, 3C and 5C are presented in Figs. 4a−4c.
The voltage curves of the three cells are very similar during the dis-
charge at 1C in Fig. 4a, but the voltage drop of the cylindrical cell
is clearly shown during the discharges at 3C and 5C. The pouch cell
shows slightly lower voltage than the prismatic cell for the initial stage
of the discharges. To compare the internal resistances of the three cell
formats, the voltage differences between the output voltage and the
 Journal of The Electrochemical Society, 166 (10) A1769-A1778 (2019) A1773

Table II. Model parameters in the sub-models.

Negative electrode Positive electrode

Particle domain parameters (Graphite) (NCM523)

Diffusion coefficient, Ds,a , Ds,c (m2 /s) 1.35×10−14 ad 8.0×10−14 ad

Activation energy for solid phase Li diffusion, EDs,a , 3529 3929
EDs,c , (kJ/mol)
Reaction rate constant ka , kc , 6.0×10−11 ad 6.0×10−11 ad
(mol. s−1. m−2 [(mol. m−3 )−1.5 )
Activation energy for kinetic reaction, Ek,a , Ek,c , 2029 1329
(kJ/mol)
Charge-transfer coefficients, αa , αc 0.5 0.5
Average particle radius, Rs,a , Rs,c (m) 5.0×10−6 2.5×10−6
Concentration solid maximum, Cs,max,a , Cs,max,c 30555 45000
(mol/m3 )
SEI layer molecular weight, MSEI (kg/mol) 0.113 –
SEI layer density, ρSEI (kg/m3 ) 210013 –
Equilibrium potential of parasitic reaction, Upara , (V) 0.4012,15,17
SEI layer conductivity, κSEI (S/m) 5×10−615,17 –
0 (·m2 )
Initial SEI layer resistance, RSEI 0.00115 –
Concentration of EC (mol/L) 4.54114,15,17
Initial exchange current of parasitic reaction, ipara,init , 2.05×10−7 ad –
(A/m2 )
Activation energy for parasitic reaction, Ea,para , (kJ/mol) 5830
Electrode Domain Parameters Negative electrode separator Positive electrode
(Graphite) (NCM523)
Electrode thickness (μm) 88 – 82
Separator thickness (μm) 20
Conductivity, σs,a , σs,c (S/m) 10031 – 1031
Porosity, εi 0.397 0.43 0.401
Volume fraction AB, ε f ,i 0.007 – 0.066
Volume fraction PVDF, ε p,i 0.044 – 0.043
Initial salt concentration, ce, (mol/m3 ) 120010,20
Electrolyte diffusion coefficient, De (m2 /s) 3.0×10−1032
Electrolyte ionic conductivity, κi (S/m) κi = 10−4 ce,i × 1.2544 (−8.2488 + 0.053248T − 0.00002987T2 + 0.26235 × 0.001
ce,i −0.0093063 × 0.001ce,i T + 0.000008069 × 0.001 ce,i T 2 + 0.22002x10−6 ce,i 2
− 0.0001765x10−6 ce,i 2 T)233
Activation energy for electrolyte phase Li+ diffusion, 26.629
EDe (kJ/mol)
Transport number, t+0 0.36332
Faraday’s constant, F, (Cmol−1 ) 96487
Gas constant, R (Jmol−1 K−1 ) 8.314
Cell Domain Parameters
Thickness, δ− , δ+ (μm) 10 20
Electric conductivity for σ− , σ+ (S/m) 59.6×10610,20 37.8×10610,20
Heat transfer coefficient, hconv (W/m2 ·K) 25
Electrode plate area(m2 ) 0.76146
Mass density of jelly roll, ρ (kg/m3 ) 240010,20
Specific heat of jelly roll, Cp (J/kg·K) 85010,20
Thermal conductivity in ×& y direction, kx , ky (W/m·K) 2710,20
Thermal conductivity in planar direction, kp (W/m·K)
Thermal conductivity in z direction, kz , (W/m·K) 0.810,20
Thermal conductivity in transversal direction, kt ,
(W/m·K)
Initial temperature, T0 (°C) 25
Atmospheric temperature, Tamb (°C) 25

es: estimated, f: fitting

OCV at the beginning of the discharges are calculated and divided
by the operating current. The internal resistances are approximately
1.66 mOhm in the prismatic cell, 1.72 mOhm in the pouch cell, and
2.12 mOhm in the cylindrical cell. Thus, as the discharge current in-
creases, the voltage loss becomes more severe in the cylindrical cell
than in the prismatic cell.
The average temperature in the cylindrical cell increases more
rapidly than in the pouch cell or the prismatic cell. These different
thermal responses of the three cells are influenced by the cooling con-
ditions and the heat generation rates. At the end of discharge for the 5C
rate, the average temperature is approximately 47°C in the cylindrical
cell, while it is approximately 34°C in the pouch cell, which has a large
cooling area (approximately 178% larger than that of the cylindrical
cell) and a relatively small internal resistance area (approximately 29%
that of the cylindrical cell). Fig. 4c shows that the cylindrical cell with
a high internal resistance discharges more capacity at the end of the

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 A1774 Journal of The Electrochemical Society, 166 (10) A1769-A1778 (2019)
Figure 3. Comparisons between the modeling results and the experimental
results, showing: (a) voltage curves with different currents, (b) capacity change
with cycle numbers and (c) voltage curves at different cycles.
discharge. The elevated temperature affects electrokinetic phenomena
in the electrodes such as the lithium diffusion and the kinetic reaction,
to which the Arrhenius equation is applied, resulting in more active
electrochemical reaction and an increase in discharge capacity. Thus,
a cell with a high internal resistance stays at a high temperature at the
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Figure 4. Output voltages and temperatures of the three cells at discharge rates
of (a) 1C, (b) 3C, (c) 5C; (d) heat generation during discharge.
end of the discharge and has a higher discharge capacity. As shown in
Fig. 4a, the discharge capacities of the three cells are nearly identical
at the 1C rate when the temperature increases are not severe; however,
when the discharge current is at the 5C rate, the cylindrical cell with a
high temperature discharges more capacity than the other cell and the
pouch cell with the prismatic cell.
Fig. 4d shows the total heat generation of the three cells during the
1C, 3C and 5C discharges. Total heat generation is calculated by sum-
ming up the heat from multiple sources, including the kinetic reaction,
joule heat from the electron transfer inside the electrodes, reversible
heating due to entropy change and joule heat caused by the current
flowing in the metal current collectors. The amounts of heat generation
during the discharges are in the increasing order of the prismatic cell,
the pouch cell and the cylindrical cell. The average heat generation
rates at the 5C rate are 9.95 W for the prismatic cell, 10.98 W for the
pouch cell and 13.59 W for the cylindrical cell. Although the pouch
cell generates more heat than the prismatic cell, the average temper-
ature of the pouch cell is lower than the average temperature of the
prismatic cell because of the large cooling surface area (approximately
150% larger than that of the prismatic cell). Since the electrode design
and the material of the three cells are identical, the additional heat gen-
erated in the pouch cell and the cylindrical cell is probably produced
at the cell level where joule heat in the metal current collectors is cal-
culated. Table III shows the heat generations in the current collectors
during the discharges and their percentages of the total heat genera-
tion. The amounts of heat generated from the sources except joule heat
in the current collectors are estimated to be approximately 0.42 W at
the 1C rate in the three cells. However, the percentages of joule heat
in the current collectors are quite different for the three cells. In the
cylindrical cell, the percentage of joule heat in the current collectors
is over 30% of the total heat generated and approximately 4 times
as large as the percentage of joule heat in the current collectors in the
prismatic cell. The high electrical resistance in the current collectors of
 Journal of The Electrochemical Society, 166 (10) A1769-A1778 (2019) A1775

Table III. Heat sources of the three cells during 1C, 3C and 5C constant current discharge.

Heat sources Cell type 1C (20A) 3C (60A) 5C (100A)

Heat from the current collectors (W, %) Pouch 0.06W (12.67%) 0.55W (13.02%) 1.51W (13.71%)
Cylindrical 0.20W (31.64%) 1.79W (33.74%) 4.96W (35.80%)
Prismatic 0.03W (7.08%) 0.28W (7.42%) 0.79W (7.92%)
Heat from the other sources (W, %) Pouch 0.42W (87.33%) 3.65W (86.98%) 9.48W (86.29%)
Cylindrical 0.42W (68.36%) 3.42W (66.26%) 8.63W (64.20%)
Prismatic 0.42W (92.92%) 3.54W (92.58%) 9.16W (92.08%)

the cylindrical cell clearly leads to high heat generation. Additionally,
as discharge currents increase, the percentages of joule heat are ele-
vated in all three cells; for example, joule heat in the cylindrical cell is
approximately 4% higher during the 5C discharge than during the 1C
discharge. The effect of electrical resistance in the current collectors
can therefore be magnified for high current operations of LIBs.
The spatial imbalance in the cell volume is another major factor
affecting the performance and life of large-format LIB cells. However,
it has not been easy to predict the nonuniform phenomena over a cell
volume and to quantitatively determine the effects of cell imbalance on
performance because of complex relationships among coupled elec-
trochemical, electrical and thermal physics. Thus, this study defines
a nonuniformity factor (NUF) for quantitating cell imbalances over
the cell volume during the operation time. Thanks to the fully cou-
pled calculation with 3-dimensional resolution of the MSMD model
framework, NUF can be calculated for all physicochemical variables
in the models, such as current density f  [Am−2 ], SOC, and tempera-
ture T[°C], as shown in Eqs. 16−18.
      
1 1  j − j  avg 
NUF j  =     dV dt [16]
dt dV  j  avg 
     
1 1  SOC − SOCavg 
NUFSOC =     dV dt [17]
dt dV  SOCavg 
     
1 1  T − Tavg 
NUFT =     dV dt [18]
dt dV  T  at 1st cycle (solid line) and 1200th cycle (dashed line) in Fig. 6b. At
avg
The spatial imbalances of the variables are influenced mainly by the
electrical configuration in the current collectors and the heat transfer
in the cell volume. Figs. 5a–5c shows the contours of current density,
SOC, and temperature deviation after 5 minutes of discharging at 5C
(100 A). The current density distribution in Fig. 5a indicates that the
electrochemical reaction is activated near the tabs in all three cells. In
the contours of the unrolled cylindrical and prismatic cells, the kinetic
reaction is slightly facilitated near the cell core due to high temperature
because the thermal conductivity of the wound-type cells is poor in
the radial direction. In Fig. 5d, NUFs of current density are elevated
in the three cells as the output current increases, and the prismatic
cell has the lowest NUFs of electrochemical reaction (approximately
40% of the NUF of the cylindrical cell and approximately 67% of the
NUF of the pouch cell). The distribution of SOC shown in Fig. 5b
is closely related to the distribution of current density in Fig. 5a. As
current density maintains a similar spatial distribution for 5 minutes
of 5C discharge, SOC far from the tabs where the kinetic reaction
is less activated is higher than SOC near the tabs. Additionally, in
the cylindrical cell and the prismatic cell, SOC near the cell core is
relatively low because of the high temperature near the cell core. Thus,
NUFs of SOC of the three cells are similar to those of current density
in Fig. 5d.
In the contours of temperature deviation in Fig. 5c, hot spots are
found near the tabs because of the locally concentrated electric current
near the narrow tabs in the current collectors. For all the three cells,
the temperature near the negative tabs is slightly higher than the tem-
perature near the positive tabs because the thickness of the negative
copper foil is half that of the positive aluminum foil corresponding to
high electrical resistance. The hot spots are repeated along the wind-
ing direction in the cylindrical cell and the prismatic cell due to the
thermal conduction in the radial direction. The cylindrical cell shows
a large imbalance of temperature because of its small cooling area
and long thermal path in the radial direction. Temperature deviation
in the pouch cell appears only between the near-tab region and the far-
from-tab region. In the prismatic cell, temperature distribution is quite
uniform because the cell has a relatively large surface area (approxi-
mately 1.2 times the area of the cylindrical cell) and a short thermal
path (approximately half the thickness of the cylindrical cell). There-
fore, the NUFs of temperature for the prismatic cell, the pouch cell
and the cylindrical cell are raised, as shown in Fig. 5d. For discharges
at low currents (1C and 2C), NUFs of temperature of the pouch cell
and the prismatic cell are similar to each other; however, as discharge
current increases, the pouch cell shows a larger imbalance in tempera-
ture than the prismatic cell. This imbalance seems to happen because
the large cooling area of the pouch cell is capable of suppressing the
increase in temperature at the hot spots at the low current discharges.
Effects of cell formats on aging.—Aging of the three cells is
compared by simulating a cycling operation of 4CD4CCCV for 1200
cycles. Fig. 6a shows the model results of capacity retention as cy-
cles; the total capacity losses are approximately 5% for the pouch cell,
approximately 7% for the prismatic cell and approximately 10% for
the cylindrical cell. The voltage curves of the three cells are plotted
the 1st cycle, the voltage loss of the cylindrical cell is large due to the
high internal resistance, but its discharge capacity is slightly larger
than those of the other cells due to the high temperature. At the 1200th
cycle, the output voltage of the cylindrical cell at the beginning of the
discharge is approximately 76 mV lower. The prismatic cell has an
output voltage that is slightly higher than that of the pouch cell at the
1st cycle but is degraded faster, showing a lowered output voltage of
approximately 54 mV at the beginning of the discharge at the 1200th
cycle. In Fig. 6c, the internal resistances of the three cells calculated at
the beginning of the discharges are presented with the cycle number.
The prismatic cell is confirmed to experience faster degradation than
the pouch cell although it starts with a lower internal resistance than the
pouch cell. In the Effects of cell formats on performance section, the
prismatic cell is under a higher temperature than the pouch cell since
it has a cell design with thermal disadvantages such as smaller surface
area and larger thickness. Thus, the impact of internal resistance on
degradation is relatively weak compared to that of temperature. The
SEI layer growth mainly occurring in charging operations is clearly
accelerated under high temperature since the rate of the parasitic re-
action is dependent on temperature, as shown in Eq. 3. In Fig. 6d,
which shows the averaged SEI film resistances, it can be seen that the
cell with high temperature presented in Fig. 4 degrades rapidly. The
cylindrical cell with a high internal resistance experiences the fastest
degradation since it is thermally stressed by high joule heat generation
and has a small cooling area.
Degradation does not occur uniformly over the cell volumes, and
the imbalanced degradation can accelerate the aging of the LIB cells.

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 A1776 Journal of The Electrochemical Society, 166 (10) A1769-A1778 (2019)

Figure 5. Contours of (a) current density, (b) SOC, and (c) temperature deviation in the three cells after 5 minutes of discharging at 5C (100A). (d) Comparisons
of nonuniformity factors (NUFs) for current density, SOC, and temperature.

Fig. 7a presents the mean deviations of SEI layer resistances in the
three cells at the end of the 1200th cycle. In the pouch cell, regions near
the tabs are degraded slightly more than the other regions. The elevated
temperature near the tabs indicated in Fig. 5c induces the activation
of the local parasitic reaction. In the cylindrical cell and the prismatic
cell, degradation is clearly accelerated near the cell cores and is also
caused by the elevated temperature at the cell core. Fig. 7b shows the
NUFs of SEI film resistances, which represent spatial nonuniformity
of degradation; the imbalance of degradation in the cylindrical cell
is the largest among the three cells and is approximately four times
larger than that in the pouch cell. The NUF of SEI film resistance of
the prismatic cell is approximately 1.6 times larger than the NUF of
SEI film resistance of the pouch cell. Although other factors such as
electrical overpotentials over the current collectors can influence the
spatial distribution of degradation, the main factor driving the different
NUFs of degradation in the three cells seems to be temperature distri-
bution. The side reaction occurs actively at the CV charging process
taking a significant time at high SOCs. At this stage, the current den-
sity is relatively small and, thus, the kinetic phenomena such as charge
transfer and electric current flow is hard to influence the spatial devi-
ations of degradation. The smallest NUF of degradation of the pouch
cell is further evidence of the effect of temperature deviation on the
spatially imbalanced degradation because the pouch cell operating at
small input currents, for instance at 1C, has the smallest temperature
deviation, as shown in Fig. 5d.
The continuous tab design in the three cell formats.—The model
results in the Effects of cell formats on aging section show that the
decrease in capacity of the three cells is affected by their thermal
condition. The electrical resistances in the current collectors do not
seem to have a direct impact on degradation. However, it should be
noted that the high electrical resistance results in high joule heat gen-
eration and likely results in high temperature if the cooling capacity
is not large enough. Thus, for a cell with a poor electrical configu-
ration and correspondingly high electrical resistance, it is not easy
to avoid rapid degradation. Rapid degradation of the cylindrical cell
in the Effects of cell formats on aging section is a good example
of that phenomenon because the cell has a small number of elec-
trical tabs and long current flow paths in the current collectors. In
other words, degradation of an LIB cell can be delayed by improv-
ing the electrical configuration without changing the cooling strategy.
In this section, we investigate how much the aging process is de-
layed if a cell has the best possible electrical configuration for its cell
format.
As the improved electrical configuration for the three cells, the
continuous tabs are suggested as shown in Fig. 8a. The purpose of
the continuous tabs is to maximize the area of the electrical tabs in
the given cell geometry and to minimize the electrical paths in the
current collectors. The continuous tabs can be considered extended
current collectors at certain sides of the cells, and the positive and
negative tabs are places in the opposite sides of the cells. Conditions

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 Journal of The Electrochemical Society, 166 (10) A1769-A1778 (2019)
Figure 6. Comparisons of the cycling result of the three cells: (a) capacity
retention, (b) output voltage at 1st cycle and 1200th cycle, (c) internal resistance
and (d) SEI layer resistance.
Figure 7. (a) Distributions of SEI film resistance in the three cells, (b) nonuni-
formity factors (NUFs) of SEI film resistance in the three cells.
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A1777
Figure 8. (a) Cell designs with the continuous tabs for the pouch cell, the
cylindrical cell and the prismatic cell and improved (b) capacity retention, (c)
internal resistance after the 1200th cycle and (d) the maximum temperatures
during 1200 cycles.
of the cycling simulation are the same as those of the operating condi-
tions in the Effects of cell formats on aging sections performed for the
three cells with the continuous tabs. Fig. 8b shows the comparisons
of capacity retentions of the three types of cells with the discrete tabs
and the continuous tabs at the end of the 1200th cycle. Comparison
between the cells with the continuous tabs and the cells with the dis-
crete tab cell shows that capacity retention is approximately 5% high
in the cylindrical cell, approximately 0.3% high in the prismatic cell
and almost the same in the pouch cell. In Fig. 8c, there is not much
improvement in internal resistance in the pouch and prismatic cells
with the continuous tabs. However, in the cylindrical cell, the internal
resistance is reduced by approximately 27% by the continuous tabs
at the 1st cycle, and the difference grows to approximately 32% af-
ter 1200 cycles. Fig. 8d compares the peaks of the volume-averaged
temperatures of the cells during the cycles. For the pouch cell and the
prismatic cell, the peak temperatures are not changed by implementing
the continuous tabs but decrease by approximately 5°C for the cylin-
drical cell. The model results indicate that the tab configuration of the
 A1778 Journal of The Electrochemical Society, 166 (10) A1769-A1778 (2019)
cylindrical cell is particularly poor and that its impact on degradation
is considerable.
From the model results in this study, the cell design of large LIBs
can clearly deteriorate performance and life. The pouch cell design
and the prismatic cell design seem to provide better advantages for
the scale-up of LIBs than the cylindrical cell design thanks to a large
cooling area. However, if the electrical configuration of the cylindrical
cell can minimize the joule heat generation in the current collectors,
the disadvantage of the cylindrical cell design can be reduced.
Conclusions
Simulations for investigating the effects of LIB cell formats on
imbalance and degradation are conducted by using a multi-physics
model. Three cells with different formats, the pouch, cylindrical and
prismatic cells are modeled with a same capacity of 20Ah and an iden-
tical electrode design for comparisons. The model results show that
the imbalance and degradation can be significantly affected by the cell
format and the cell temperature is the key factor deciding the aging
rate of the large LIB cells. The cylindrical cell experiences severely ac-
celerated degradation because of the large electrical resistance and the
poor heat transfer condition rising cell temperature. Serious imbalance
in the cell volume also appears in the cylindrical cell because of the
long electric paths in the current collectors. Competing effects of the
joule heat generation and the convective cooling on degradation are ob-
served in the simulation results of the prismatic cell and the pouch cell.
The prismatic cell with a small electrical resistance produces the rela-
tively small joule heat in the current collectors compared to the pouch
cell. However, degradation of the prismatic cell is slightly faster than
that of the pouch cell because the smaller surface area of the prismatic
cell results in the higher cell temperature. With the improved electrical
configurations of the continuous tabs, the negative effects of the cell
designs on degradation are considerably mitigated. For the cylindrical
cell with the continuous tabs, the capacity retention is increased about
5% and the operating temperature is decreased by about 5°C. It indi-
cates that an optimum tab design is important to achieve better LIB
life.
Acknowledgments
This research was supported by Korea Electric Power Corpora-
tion [No. KEPRI-15-30]; the Korea Institute of Energy Technology
Evaluation Planning [No. 20172410100140].
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ORCID
Kyu-Jin Lee https://orcid.org/0000-0002-5631-6608
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