Solid State Ionics 406 (2024) 116471

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Solid State Ionics

journal homepage: www.elsevier.com/locate/ssi

Multiphysics simulation of the effect of compressed separator on

lithium-ion battery
Qingyang Hu a, Lei Sheng b, Xin Xie a, Ling Yang a, Xingxu Gao a, Datuan Li a, Yaozong Bai b,
Gaojun Liu b, Haoyu Dong b, Tao Wang a, Xianli Huang a, Jianping He a, *
a
College of Material Science and Technology, Nanjing University of Aeronautics and Astronautics, 210016 Nanjing, Jiangsu Province, China
b
Sinoma Lithium Battery Separator Co. Ltd, 277500 ZaoZhuang, Shandong province, China

A R T I C L E I N F O A B S T R A C T

Keywords: Owing to these phenomena about intercalation and deintercalation lithium-ion, thermal expansion, and external
Multiphysics simulation pressure in lithium-ion batteries, the interior separators are often subjected to compression stress. In this study,
PE separator we have designed a novel model based on the Thiessen Polygon, which is used to describe 3D porous structure of
Compression stress
polyethylene (PE) separator. It can simulate the structure evolution of separator during compression. The
Lithium-ion battery
simulation results show that when the compression stress is up to 60 MPa, the thickness of the separator de­
Microcosmic model
creases by nearly 50%, and the porosity decreases from 42.6% to 10%, which severely affects the ionic trans­
mission performance. Additionally, the separator with changed porosity structure under different compression
conditions was applied to the electrochemistry-thermal model to simulate the discharge process of the battery. As
results, it is found that the discharge capacity is significantly reduced and the temperature is increased due to the
structural variation of the separator caused by compression stress. This study develops a novel mechanical model
which can be used in the simulation of separator compression process, and involves the simulation of multiple
physical fields. And it successfully correlates the mechanical properties of separator with its battery performance.

1. Introduction
Owing to some advantages such as high energy density, long service
life and no memory effect, lithium-ion batteries (LIBs) have become the
most common energy storage devices, which are widely used in portable
electronic devices and electric vehicles [1–4]. As one of the most
important parts of LIBs, the separator is used to isolate the positive and
negative electrodes to prevent the internal short circuit and meantime
allows the transmission of lithium ions. In order to ensure the electro­
chemical performance and safety performance of LIB, the requirements
for separators are very strict. The separator should have ultrathin
thickness, proper porosity, uniform pore structure, high electrolyte
wettability and strong mechanical properties [5–8]. At present, poly­
olefin (polyethylene (PE) and polypropylene (PP)) separators have
attracted wide commercial applications for their low-cost, adequate
mechanical properties and excellent electrochemical stability. However,
when the battery operating in some extreme circumstances, such as high
temperature or large current, the separator could undergo various
degradation for mechanical stress. For example, the separator needs to
bear the tension generated by winding operation under the battery as­
sembly process [7]. And the volume deformation of the electrode ma­
terials induced from lithium-ions diffusion and thermal expansion
difference during the battery components would produce a certain
squeezing force toward the separator [9]. In addition, acupuncture and
collision caused by external factors will also produce stronger force,
which will cause serious deformation effect of the separator and even
lead to battery short circuit. Therefore, exploring the evolution of sep­
arators under different mechanical stresses is of great significance to
improve the performance of LIB [10–18].
Many researches have been carried out about the mechanical prop­
erties of separators in recent years. For instance, Zhang et al. [19]
explored the deformation and failure modes of four commonly used
separators (PE, PP/PE/PP, ceramic-coated and nonwoven separators)
through uniaxial tension, compression and biaxial stamping experi­
ments. Also, Sheidaei et al. [20–26] studied the mechanical properties of
the separator after immersion in the electrolyte, and it revealed that the
electrolyte greatly weakened the tensile properties of the separator, but
improved the compression properties of the PP separator produced by

* Corresponding author.
E-mail address: jianph@nuaa.edu.cn (J. He).

https://doi.org/10.1016/j.ssi.2024.116471
Received 9 August 2023; Received in revised form 21 December 2023; Accepted 17 January 2024
Available online 24 January 2024
0167-2738/© 2024 Elsevier B.V. All rights reserved.
Q. Hu et al.
dry process to a certain extent. Furthermore, Zhao et al. [27] studied
coupled effect of low temperature and electrolyte immersion on the
tensile properties of separators, and find that separators in low tem­
perature conditions exhibit an increase in strength while showed a sig­
nificant softening behavior when immersion in the electrolyte. Makki
et al. [28] studies the stress distribution in the separator when the bat­
tery cell under mechanical loading inside a battery pack is fast charged,
and the results show a significant amount of damage can be accumulated
in the separator under certain loading in charge-discharge cycling. Ding
et al. [29–31] discussed the effect of compression stress on the me­
chanical properties of separator through compression experiments.
These experiments are to understand the deformation and damage
mechanism of the separator, so as to prevent the battery performance
degradation or even short circuit caused by the mechanical degradation
or crack of the separator. But the mechanical degradation of the sepa­
rator is often inevitable. Even without the influence of external factors,
the mechanical strength of the separator would inevitably decrease with
the battery cycle [32]. Therefore, it is also necessary to consider the
effect of the mechanical degradation of the separator on the battery
performance. Hence, Peabody et al. [33] assembled the compressed
separator into the battery and tested its capacity, the experimental re­
sults uncovered that even a small external stress as low as 1 MPa would
cause measurable attenuation of the battery capacity. Canarella et al.
[34] disclosed the effect of mechanical stress generated by charge-
discharge cycle on the life of LIB, and found that the capacity fade
was caused by the coupling of mechanical and electrochemical. Sun
et al. investigate the effects of compressed separators on the electro­
chemical performance of LIB, and find the key parameter to influence
the performance. [35] Spingler et al. present an analysis of the effects of
non-uniform mechanical loads on the performance of LIB and find that it
can provoke localized lithium plating due to the changed current density
distribution. [36] The above researches are based on experiments which
are difficult to operate and costly. In order to investigate the perfor­
mance of the separator and reduce the research cost, the numerical
simulation method is necessary.
When using the numerical simulation method, the separator model
needs to be developed. At present, many researchers use macroscopic
homogenization model to simulate the mechanical properties of sepa­
rator. This model can predict the macroscopic deformation of the
separator under various stress. When the deformation reaches the
extreme value, the separator will be cracked, which would lead to the
short circuit of battery. Therefore, it is possible to predict the short
circuit of the battery through this model [37–45]. When the separator is
deformed, it displays the variation of thickness and shape on the
macroscale, and the transform of pore structure on the microscale.
Moreover, these transformations of microstructural characteristics are
closely related to the ionic transmission performance. Hence, to un­
derstand the microstructural behavior during separator deformation, it
is worthwhile to develop a micro-geometric model that could effectively
describe the 3D porous structure of the separator. For instance, Xu et al.
[46–48] developed a 3D microstructure model through random recon­
struction algorithm based on 2D microscopic images of anisotropic
separators. The microstructure model successfully captured the anisot­
ropy of the battery separator, and predicted the stress-strain curve and
deformation microstructure. In addition, Lagadec et al. [49] presented a
simple method for PE separator microstructure visualization and
quantification based on focused-ion-beam scanning electron micro­
scopic tomography. Through this method, the pore structure charac­
teristics of PE separator are quantified using porosity and tortuosity
parameters. Based on this structural visualization method, researchers
established a numerical model to predict the changes of mechanical and
electrochemical properties of the separator under compression stress
[50,51]. However, separator properties are ultimately related to the
comprehensive performance of LIB. In order to investigate the effect of
separator deformation on LIB by numerical simulation, it is also neces­
sary to combine the LIB model. Among the LIB models, the P2D (pseudo-
2
Solid State Ionics 406 (2024) 116471
two-dimensions) model developed by Newman et al. [52,53] is a com­
mon model. Many researchers have established new models based on
P2D model. These models can simulate the charge-discharge process of
LIB, obtain the charge-discharge curve of LIBs and the heat value
generated during the work process [54–57].
At present, there have been many investigations to explore the effect
of mechanical compression on separator performance through numeri­
cal simulations, but few have considered the effect of reduced ion
transport performance of separators under pressure on LIB performance.
To address this issue, a novel 3D mechanical model that can reflect the
real structural of the separator has been developed and combined with
the electrochemical-thermal model of the LIB for the analysis of the
Multiphysics simulation. Mechanical models have been used to analyze
the change in separator structure under compression stress, and this
transition has been quantified and applied to electrochemical-thermal
models to predict the discharge properties and temperature changes of
LIB.
2. Methods
Fig. 1 presents the research process in this work. PE separator was
selected as the study object, and its microscopic images were obtained
using the scanning electron microscope (SEM, Japan, Hitachi, S-4800).
Based on the obtained SEM images, a microscopic 3D model of the PE
separator was constructed using parameter modeling in Rhino software.
Then we use the established microscopic 3D model to perform
compression simulations in COMSOL Multiphysics. The structural
change of the separator during compression could be observed through
simulation, and the change of separator porosity and dimension during
compression could be calculated according to the simulation results.
Finally, these structural parameters of separator porosity and dimension
calculated from compression simulations are used in the
electrochemical-thermal model of LIB, and then the effect of separator
deformation caused by compression stress on the performance of LIB
was investigated.
2.1. The establishment of 3D microcosmic model
Fig. 2 exhibits the SEM image of PE separator produced by wet
process. The PE separator has undergone biaxial tension, so it has nearly
circular uniform pores, and its cross section shows a multilayer struc­
ture. This separator has a measured porosity of 40.4%. To build a
micron-scale model consistent with the actual structure of the separator,
the Grasshopper plug-in Rhino software was used for parameter
modeling. Specific modeling ideas are as follows: To save the calculation
cost, we selected the area shown in Fig. 2 (1 um × 1 um) as the reference
object for modeling. The Thiessen Polygon is used as the basic model. It
is a group of continuous polygons composed of vertical bisectors con­
necting two adjacent point segments, and has a porous structure similar
to the separator. The distance from any point in a Thiessen Polygon to
the control point forming the polygon is less than the distance from the
control point of other polygons. The pore in the separator was chosen as
the control point for generating the Thiessen Polygon structure element.
After the Thiessen Polygon structural element is established, it is
necessary to generate pores. Each element can scale relative to its center
point in the same proportion, and this scaling operation can control the
porosity of the generated model. Then curve lifting, combining,
smoothing, and other operations are performed to complete the single-
layer model. Since the PE separator is a multilayer structure in the
thickness direction, four similar structures are constructed. The final 3D
model of the PE separator is shown in Fig. 3.
To facilitate the compression simulation, the protruding filament
structure around the 3D model is truncated to a regular square for the
application of the compression stress. The dimension of the final model
is 1 × 1 × 0.75 um, and the porosity is 42.6% by calculation, which is
close to the true porosity of the separator.
Q. Hu et al. Solid State Ionics 406 (2024) 116471

Fig. 1. Multiphysics simulation workflow chart.

Fig. 2. Microstructure image of wet process PE separator.

2.2. Finite element simulation of compression process where σ ij is stress tensor, fi is body force, and i and j are spatial vectors.
The constitutive equation of isotropic linear elastic material is given
After the establishment and adjustment of the model, the finite by Hooke's law:
element method is used for compression simulation. Using the solid
mechanics module of COMSOL Multiphysics, a steady-state analysis εij =
(1 + ν) ν
σ ij − σ kk δij (2)
study was conducted. The research shows that the porous separator E E
structure behaves viscoelastic when deformed [58]. In order to simplify
where εij is strain tensor, ν is Poisson's ratio, E is Young's modulus, and
the calculation, based on previous studies [51], the separator is assumed
δij is the Kronecker symbol.
to be isotropic linear elastic material in this study. The substrate mate­
rial is PE with densities and Poisson ratios of 930 kg/m3 and 0.38, The deformation compatibility equation describing the relationship
between displacement and strain is as following:
respectively, and Young's modulus values are those mentioned in ref.
[29]. The compression test results in other study show that the PE 1( )
εij = uij + uji (3)
separator has no yield stage and has always been in the hardening stage. 2
Therefore, the Young's modulus is set to increase linearly in the simu­
lation with reference to the experimental data. where u is displacement.
The basic governing equations for solving structural mechanics After setting the material parameters and determining the control
problems are as follows: equation, the model needs to be constrained. As shown in Fig. 4a, the
The first is the equilibrium equation under steady-state conditions: application of constraint is consistent with the compression test. During
compression, the separator is fixed on the base, and the expansion of the
σ ij + fi = 0 (1) separator around is not limited when the compression stress is applied.

3
Q. Hu et al. Solid State Ionics 406 (2024) 116471

Fig. 3. Modeling process of PE separator.

Fig. 4. (a) Schematic diagram of constraints; (b) Schematic diagram of model grid division.

In order to obtain a unique solution, it is necessary to limit the six de­
grees of freedom of the model. First, the specified displacement
constraint of z = 0 is applied to the bottom surface of the model so that
the bottom surface does not move in the vertical direction. And then two
points are selected on the bottom surface, one of which is subject to a
fixed constraint, and the other is to limit its displacement in the direction
perpendicular to the line between the two points, thus limiting the
rotational freedom of the model. Next, the model was meshed. Due to
the complexity of the model and the fact that the defective parts of the
model had been corrected during the modeling process, it was decided to
automatically mesh the model based on the physical field. The mesh size
range was 0.018 μm − 0.1 μm, and the final mesh count was approxi­
mately 1.66 million, as shown in Fig. 4b. The legend on the right of
Fig. 4b represents the grid quality. The larger the value, the better the
grid quality. Judging from the color in the figure, the grid quality is
generally acceptable. After the constraint and mesh division is
completed, the compression stress is applied along the normal direction
of the upper surface, and the change of separator structure under the
compression stress of 10–100 MPa is simulated at the interval of 10 MPa.
2.3. Electrochemical-thermal model
In order to explore the effect of separator pressure on battery per­
formance, the electrochemistry-thermal coupling model is used in this
study which was proposed by Newman et al. [48]. This model describes
the electrochemical process in LIBs, including material transfer and
charge transfer, the schematic diagram of the model is shown in Fig. 5.
Material transfer occurs in the electrode particles (solid phase) and
electrolyte (liquid phase). The control equation is given by Fick's second
law, in which the liquid phase also contains the electromigration term:
∂cs
= ∇⋅(Ds ∇cs ) (4)
∂t
∂ce ( ) 1 − t+0 Li
= ∇⋅ Deff
e ∇ce + j (5)
∂t F
where cs and Ds are the lithium-ion concentration and the diffusion co­
efficient of the solid phase, respectively; and ce and Deff
e are the lithium-
ion concentration and the diffusion coefficient in the liquid phase,

4
Q. Hu et al. Solid State Ionics 406 (2024) 116471

Fig. 5. P2D model of lithium-ion battery.

0
respectively; t+ is the lithium-ion transfer number, F is the Faraday thermal model is 293 K. Some parameters of the electrochemical ther­
constant, and jLi is the Current density of electrochemical reaction. mal model are shown in Table 1 [54,60].
The charge transfer process also occurs in the solid phase and the
liquid phase, and is described by the change of the solid phase potential 3. Results and discussion
and the liquid phase potential. The governing equation is given by Ohm's
law: This section mainly includes compression simulation of mechanical
( ) model and simulation of battery discharge process of electrochemistry-
∇⋅ σ eff ∇ϕs − jLi = 0 (6) thermal coupling model. The stress distribution and displacement dis­
( ) ( ) Li tribution of the separator under compression stress are obtained from
∇⋅ κeff ∇ϕe + ∇⋅ κeff
D ∇lnce + j = 0 (7) the compression simulation, and the dimension and porosity variations
of the separator during compression are calculated from the displace­
where σeff is the effective electron conductivity, κeff and κeff
D are the ment distribution diagram, and the results are presented in Sections
lithium-ion conductivity coefficient and the effective lithium-ion diffu­ 3.1–3.2. The discharge process of the battery is simulated, and the
sion conductivity, respectively; ϕs and ϕe are the solid phase potential discharge capacity and temperature variations are obtained for different
and the liquid phase potential, respectively. discharge rates are obtained when the separator is compressed, and the
The Butler–Volmer equation is used to calculate the local current at results are presented in Sections 3.3–3.4.
the electrode interface area:
[ ( ) ( )]
jLi = i0 exp
αN F αF
η − exp p η (8) 3.1. Stress and displacement distribution
RT RT
Taking 30 MPa compression stress as an example, the stress distri­
where R is the Gas constant, αN and αp are the electrochemical reaction bution of the separator under the compression stress is analyzed in
transmission coefficient of positive and negative electrodes, respec­ Fig. 6, and the stress value gradually increases from blue to red. The
tively; i0 is the exchange current density of electrochemical reaction, porous part of the separator is defective when subjected to stress, so that
and η is the overpotential. the phenomenon of stress concentration during the compression of the
The heat transfer control equation is as following: separator is very remarkable. Due to the stress concentration, the high
∂T stress values are mostly concentrated around the pores in the thickness
ρC p = ∇⋅(λ∇T) + q (9) direction, which leads to the gradual closing of the pores in the thickness
∂t
direction during the separator compression.
where ρ is the mixed average density of battery components, Cp is the
specific heat value of battery components, λ is the thermal conductivity, Table 1
and q is the heat generation rate of battery. Parameters used in the simulations.
The calculation of heat generation rate in electrochemical models is
Parameter Anode Separator Cathode
mainly based on the chemical battery heat generation rate model pro­
Thickness, Li(μm) 100 Lsep 183
posed by Bernardi et al. [61]. The heat generation rate of batteries
Battery sectional area, A(m2) 1
during charging and discharging is: Porosity, εe 0.503 εsep 0.63
( ) Active material volume fraction, εact 0.471 0.297
∇ce ∂Uo
q = Qohm + Qr = σ eff ∇ϕs ⋅∇ϕs + κeff ∇ϕe + κeff
D ⋅∇ϕe + IT (10) Bruggeman exponent, B 3.3 3.3 3.3
ce ∂T Particle radius, Ri(μm) 12.5 8
13
Solid phase Li diffusion coefficient, Ds(m2 / 3.9 × 1 × 10−
where Qohm is ohmic heat, Qr is electrochemical heat, I is the charge and S) 10− 14
11
discharge current, T is the battery temperature, and Uo is the open cir­ liquid phase Li+ diffusion coefficient, 7.5 × 10−
cuit voltage. De(m2 /S)
Solid phase conductivity, σs(S/m) 100 3.8
This simulation type is a transient study(time-dependent), using the Li+ transference number, t+ 0.363
above model to simulate the discharge process of a LiMn2O4|LiPF6|LiC6
0
Initial temperature, T (K) 293
battery with a capacity of 17.5 Ah at different discharge rates (1C = Mixture Density, ρ (Kg/m3) 2300
17.5 A/m2), with a cut-off voltage set at 2.4 V. Heat transfer under Mixture specific heat capacity, cp (J/kg K) 2400
adiabatic conditions is considered, and the initial temperature of the Mixture thermal conductivity, k (W/m K) 3

5
Q. Hu et al.
Fig. 6. Stress distribution of the separator under the compression stress of
30 MPa.
The displacement distribution of the separator under the compres­
sion stress of 10–60 MPa is showed in Fig. 7. Since the compression
stress acts directly on the upper surface, the displacement at the top of
the separator is larger than the displacement at the bottom. As the
compression stress increases, the pores in the thickness direction of the
separator are squeezed and collapse. When the compression stress is
increased to 60 MPa, the pores in the thickness direction almost disap­
pear. When the compression stress is sufficiently large, the pores in the
thickness direction of the separator close and the filaments of the
separator expand laterally, thus gradually filling the transverse pores.
With the increase of compression stress, the displacement of each part in
the separator correspondingly increases. When the compression stress is
10–60 MPa, the average displacement in the z direction of the separator
is − 0.148 um, − 0.235 um, − 0.296 um, − 0.337 um, − 0.367 um, and −
0.388 um, respectively, and which is 19.7%, 31.3%, 39.4%, 44.9%,
48.9%, and 51.7% of the model thickness (0.75 um), respectively.
The ratio of the displacement of the upper surface of the separator
(the surface under compression stress) relative to the initial thickness of
the separator is defined as the strain during compression. The corre­
sponding separator strain values under different compression stresses
are calculated by using the displacement distribution diagram, and the
stress-strain curve during separator compression is obtained. The
simulated and experimental values of the separator compression stress-
strain curves are illustrated in Fig. 8a. The experimental results are from
Fig. 7. Displacement distribution under different compression stresses.
6
Solid State Ionics 406 (2024) 116471
the literature [28], and the simulation results are consistent with the
experimental results. As the compression stress increases, the separator
strain increases continuously. Since the separator has a porous structure,
the first parts to be compressed are the pore of the separator and a few
parts of the separator body. Thus, during the initial stage of compres­
sion, the separator can generate relatively large deformations with small
stress increases. As the compression process proceeds, the pores of the
separator in the thickness direction gradually disappear, while the
transverse pores are gradually filled by the expanded separator fibers. At
this point, the solid part of the separator is compressed, so that it is
difficult for the separator to deform at the later stage of compression,
and the deformation corresponding to the same stress increment is
significantly reduced compared to the initial stage of compression.
In this section, the stress and displacement distribution of the sepa­
rator under the compression stress are obtained. The change in the
dimension of the separator during compression can be understood
through the displacement distribution diagram, including change of
separator cross-sectional area and thickness. The variation of cross
section area is small and negligible, so the change of dimension is mainly
reflected in the decrease of the separator thickness.
3.2. Porosity and ionic transmission performance
The porosity is changed with the compression of the separator. As the
compressive stress increases, the separator's porosity decreases signifi­
cantly. The corresponding porosity of the separator under different
compression stresses could be calculated by Eq. (11):
V0 − V
P= (11)
V0
where P is the porosity of separator, V0 is the sum of the pore volume and
the actual volume (the volume of cuboid), and V is the actual volume of
separator. When there is no compression stress, V0 is 0.75 um3. After the
separator is compressed, the displacement distribution diagram can be
used to calculate the absolute value of the size variation of the cuboid
surrounding the separator in the x, y and z directions under the
compression stress, and V0 can be calculated form the displacement
distribution diagram. The initial value of the V of the separator is 0.43
um3. The change value Δ V of the separator can be obtained by volume
integral of the volume strain value in the post simulation processing. The
value of V is obtained by subtracting the change value from the initial
value. The dimension variation and Δ V value in x, y and z directions are
listed in Table 2.
Fig. 8b demonstrates the calculated curve of porosity versus
Q. Hu et al. Solid State Ionics 406 (2024) 116471

Fig. 8. Curves obtained from structural mechanics simulation: (a) Compressive stress-strain curve; (b) Porosity under different compressive stresses.

Table 2
Physical size variation under compression stress.
Stress (MPa) 10 20 30 40 50 60

Dimensional variation(um) X direction 0.0546 0.0869 0.109 0.125 0.135 0.144

Y direction 0.0536 0.0853 0.108 0.122 0.133 0.141
Z direction 0.148 0.235 0.296 0.337 0.367 0.388
Volume variation(um3) ΔV 0.0139 0.0223 0.028 0.0319 0.0348 0.0367

compressive stress. The initial porosity of the separator is 42.6%. The

Table 3
porosity decreases continuously with increasing compressive stress, and
Porosity and ionic transmission performance under compression stress.
its trend of variation is consistent with that of the separator strain: at the
initial stage of compression, the separator is relatively easy to deform, Stress (MPa) 10 20 30 40 50 60

and therefore the porosity decreases rapidly; As the porosity of the
separator decreases, the area under pressure gradually becomes to the
separator body. As a result, the porosity decreases slowly due to the
difficult deformation of the separator at the late stage of compression.
When the compression stress is 60 MPa, the porosity of the separator
decreases to 10%; and when the compression stress is 100 MPa, the
porosity of the separator is close to 0.
The effect of compression stress is not only reflected in the porosity of
separator, but also reflected in the tortuosity of the pore structure. The
transmission characteristics of electrolyte in porous structure are
affected by porosity and tortuosity, which can be expressed by Eq. (12)
[55]:
ε ε
keff = k ，Deff = D
τ τ
where keff and Deff are the effective conductivity and the effective
diffusion coefficient, respectively, k and D are the conductivity and
diffusion coefficient of electrolyte, respectively, ε is the porosity of
porous structure, and τ is the tortuosity of porous structure. The rela­
tionship between ε and τ can be expressed by Bruggeman relationship:
τ = ε1− α
where α is the Bruggeman exponent, in this study α is set as 3.3 [59].
Through Eqs. (12) and (13), the relationship between the ionic
transmission characteristics of electrolyte in porous structure and
porosity can be obtained:
keff = kεα ，Deff = Dεα
According to Eq. (14), the reduction of porosity in the process of
separator compression would affect the ionic transmission performance,
thus adversely affecting the performance of LIBs. The change in ionic
conductivity under pressure calculated by Eq. (14) is shown in Table 3.
The results show that it decreases to 0.04 mS/cm under compression
stress of 60 MPa. Ding et al. [29] tested the ionic conductivity of com­
pressed separator-electrolyte systems and found that when the
Porosity(%) 33.7 27.7 22.3 17.7 13.5 10
Ionic conductivity(mS/cm) 0.28 0.20 0.15 0.11 0.07 0.04
compression stress was 20 MPa, the ionic conductivity decreased to
0.15, and when the compression stress was 40 MPa, the discharge ca­
pacity attenuation reached 52.9%, illustrating the adverse impact of the
compressed separator on the performance of the battery.
3.3. Lithium-ion battery performance
In order to explore the effect of separator compression on the elec­
trochemical performance of LIBs, the changes of the size and pore
(12)
structure of the separator after compression are parameterized and
applied to the electrochemistry-thermal model to simulate the discharge
process of LIBs. The simulation related parameters are shown in Table 1.
In the simulations, LIBs are discharged to the cut-off voltage at constant
currents of 0.2C, 1C, 3C and 5C respectively.
The voltage-capacity curves when the separator is subjected to 0–60
MPa compression stress are depicted in Fig. 9. The battery is discharged
at different C-rates, and the effect of compression stress on battery
(13)
performance becomes obvious with the increase of discharge rate. The
discharge voltage of the battery decreases slightly with the increase of
compression stress when discharging at 1C. With a discharge rate of 3C,
not only the discharge voltage of the battery is significantly reduced, but
also the discharge capacity of the battery is slightly reduced. When
discharged at 5C, the discharge voltage and capacity of the battery
(14) decreased significantly with the increase of the compression stress.
Fig. 9d shows the change curves of the battery capacity loss with
compression stress at 3C and 5C. At a compression stress of 60 MPa, the
capacity loss is 12.3% at 3C discharge and 30.2% at 5C discharge. This
result indicates that the compression stress of the separator has a
negative effect on the rate capability of the battery. It could be ascribed
that the compression stress could cause the separator structure to
change, and significantly reduce the number and size of the ion trans­
port channels. As a result, the ionic transport rate would be

7
Q. Hu et al. Solid State Ionics 406 (2024) 116471

Fig. 9. Voltage-capacity curves under different discharge rates: (a) 1C, (b) 3C, (c) 5C; (d) Discharge capacity loss under different compression stresses.

correspondingly retarded. This weakens the ability of the ion to reach
the reaction site under the specified current, thus weakening the utili­
zation efficiency of the active material of the electrode, resulting in the
loss of discharge capacity, especially in the case of large current
discharge [33]. The compression stress acting on the separator increases
the impedance, and during high-current discharge, the ohmic polariza­
tion effect (including the ohmic resistance caused by compression) is
amplified, causing the battery to reach the cut-off voltage faster,
resulting in a significant loss of discharge capacity during high-current
discharge.
3.4. Thermal effect
Compressive stresses on the separator not only affect the discharge
capacity of the LIB, but also its safety. After the separator is compressed,
the internal resistance and polarization resistance of the battery will
increase, which will lead to the increase of ohmic heat and polarization
heat during battery discharge. The heat generated during the discharge

Fig. 10. Discharge temperature-capacity curves at different discharge rates: (a) 0.2C, (b) 2C, (c) 3C, (d) 5C.

8
Q. Hu et al.
process is calculated using the electrochemical-thermal coupling model,
and the temperature variation during the discharge process of the bat­
tery under the adiabatic condition was obtained through the heat
transfer simulations.
Fig. 10 depicts the curves of the average surface temperature of the
battery with the discharge capacity under different compression stress
when discharging at 0.2C, 1C, 3C and 5C, respectively. As the
compression stress is increased from 0 to 60 MPa, the heating rate and
maximum temperature of the battery are correspondingly increased.
When the discharge rate is increased from 0.2C to 3C, the heating rate
and maximum temperature of the battery are also increased. Due to
excessive polarization and short discharge time, the final accumulated
heat at 5C is slightly lower than 3C, but the temperature rise rate
(heating power) is higher than 3C. When discharge at 3C, the battery
temperature at the end of normal discharge is 41.8 ◦ C, but when the
separator is subjected to 60 MPa compression stress, the battery tem­
perature is 51.5 ◦ C. The compression stress on the separator causes the
temperature of the battery to rise significantly, which will have a
negative impact on the safety and performance of the battery when
exceeding the operating temperature range.
4. Conclusion
In this study, the effects of mechanical compression on the separa­
tor's solid mechanics and transport performance, as well as the perfor­
mance of LIBs was investigated through Multiphysics simulation. We
first build a 3D microscopic model of the PE separator based on the
microscopic morphology of the PE separator based on the Thiessen
Polygon, and then we simulate the change of the separator structure
under compressive stress using structural mechanics simulations. At
compression stresses of up to 60 MPa, the separator thickness is reduced
by nearly 50%, and the porosity is reduced from 42.6% to 10%, which
severely affects the ion transport performance. Finally, the effect of the
compression separator on the electrochemical performance of the LIB is
simulated by the electrochemistry-thermal model of the LIB. At a
discharge rate of 5C, a compression stress of 60 MPa acting on the
separator reduces the LIB capacity by 30.2%. And at discharge rate of
3C, the compression stress of 60 MPa increases the maximum discharge
temperature of the LIB by nearly 10 ◦ C, which will seriously affect the
safety of the LIB. There also have some limitations in this study. The
failure of the separator was not considered in the simulation, and the
change in tortuosity of the separator was described by an empirical
formula. In future research, the failure of the separator and the method
of tortuosity calculating need to be considered. While, we should use
more appropriate experiment method and numerical model to describe
the changes structure of the separator.
CRediT authorship contribution statement
Qingyang Hu: Investigation, Software, Writing – original draft. Lei
Sheng: Investigation, Writing – review & editing. Xin Xie: Writing –
review & editing. Ling Yang: Writing – review & editing. Xingxu Gao:
Data curation. Datuan Li: Investigation. Yaozong Bai: Funding acqui­
sition. Gaojun Liu: Writing – review & editing. Haoyu Dong: Funding
acquisition. Tao Wang: Supervision. Xianli Huang: Writing – review &
editing. Jianping He: Writing – review & editing.
Declaration of competing interest
The authors declare that they have no known competing financial
interests.
Data availability
The authors are unable or have chosen not to specify which data has
been used.
9
Solid State Ionics 406 (2024) 116471
Acknowledgements
This author was grateful for the financial support from the Natural
Science Foundation of Jiangsu Province (BK20160795), the National
Natural Science Foundation of China (51372115 and 11575084), and A
Project Funded by the Priority Academic Program Development of
Jiangsu Higher Education Institutions (PAPD). Meanwhile, thank
Sinoma Lithium Battery Separator Co. Ltd. (China) for providing us with
raw materials.
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