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Keywords: In order to solve the problems of thermal safety and thermal reliability of the battery, a method of thermal
Lithium-ion battery reliability assessment and reliability sensitivity analysis for an 18,650 cylindrical lithium-ion battery is proposed.
P2D model The finite element analysis (FEA) software is used to establish an electrochemical-thermal coupling model of the
Thermal model
lithium-ion battery. By comparing the expected and experimental results, the accuracy of the proposed model is
Experiment
verified, and the model is subsequently used to analyze the thermal reliability. The adaptive Kriging method is
Reliability
used to establish the thermal reliability performance function model and assess the thermal reliability of the
lithium-ion battery. Additionally, in order to study the influence of the material parameters on the thermal
reliability of the battery, gradual reliability and reliability sensitivity analyses are conducted. The results show
that when the density is 3150 kg/m3, the reliability reaches 0.993, which is 14.4 % higher than that of the
existing battery, while the sensitivity value decreases. When the specific heat capacity is 1310 J/kg⋅K, the
reliability of the battery reaches 0.986, which is 13.6 % higher than that of the existing battery, while the
sensitivity value decreases. Lastly, the thermal conductivity has little influence on the thermal reliability of the
battery.
1. Introduction problem between the number of redundant battery cells and their reli
ability. Xia et al. [1] proposed a reliability design method considering
With the increasing risk of environmental pollution and the deep the thermal disequilibrium based on cell redundancy. For the problem of
ening of the global energy crisis, the transition from traditional energy predicting and evaluating remaining useful life and reliability, Wang
vehicles to electric vehicles has become increasingly imperative. et al. [9] established a reliability model considering the dependency
Lithium-ion batteries have been widely used in electric vehicles due to among cells, Zhu et al. [10,11] realized the real-time reliability evalu
their properties of high voltage, low self-discharge rate, large specific ation of the battery using the based-performance degradation Wiener
energy and relatively long life [1,2]. process model. Based on a response surface methodology and a multi-
Lithium-ion battery is an important part of electric vehicle. A failure physics coupling simulation, Xia et al. [12] proposed a novel reli
of the battery directly affects the safety of vehicles [3]. With the wide ability optimization method for a battery pack. From the above research,
spread use of lithium-ion batteries in electric vehicles, the reliability and it can be seen that the safety and reliability of the lithium-ion batteries
safety of batteries have become an important factor in the performance are crucial and urgent for the development of electric vehicles.
evaluation of electric vehicles [4]. Chen et al. [5] proposed a novel Thermal runaway is the key scientific problem in battery thermal
electro-thermal coupling model for temperature prediction and safety safety research, which has been widely investigated by multiple scholars
analysis under external short circuit fault. Li et al. [6] conducted a in recent years. Thermal runaway is related to a temperature rise orig
reliability analysis of primary battery packs using the universal gener inating from external or internal heat generation during abnormal abuse
ating function method. Ran et al. [7] proposed a strategy to enhance the [13]. Possible abuse conditions of lithium-ion batteries include electrical
reliability of lithium-ion batteries based on a statistical analysis and abuse [14–16], thermal abuse [17–20] and mechanical abuse [21,22]. A
study of the macro-mechanism of product failures. Based on the thermal runaway event can occur when the temperature of the cell
degradation of the battery pack, Liu et al. [8] research the trade-off reaches a certain degree which triggers the breakdown of the solid-
* Corresponding author.
E-mail address: yangzhou@mail.neu.edu.cn (Z. Yang).
https://doi.org/10.1016/j.est.2022.106504
Received 27 July 2022; Received in revised form 18 December 2022; Accepted 20 December 2022
Available online 27 December 2022
2352-152X/© 2022 Elsevier Ltd. All rights reserved.
Z. Yang et al. Journal of Energy Storage 59 (2023) 106504
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Z. Yang et al. Journal of Energy Storage 59 (2023) 106504
the chamber. The battery charge and discharge process are controlled by
the battery test system. The battery is charged at a constant current of
1.2A to the cut-off voltage of 4.2 V, and then charged at a constant
voltage of 4.2 V to the cut-off current of 0.048A, and then stood for 2 h.
After the charging is complete, the battery is left disconnected for 2 h, so
that the internal balance of the battery is restored. The battery is then
discharged at a discharge rate of 3C to the cut-off voltage of 3 V,
disconnected from the load, and left for 10 min. Throughout the
experiment, the current, voltage and temperature changes of the battery
are recorded.
3. Model development
Table 2
Governing equations and boundary condition of the P2D model.
Description Governing equation Boundary condition
⎧ ⃒
∂ce,n ⃒⃒
Negative electrode solution phase diffusion ∂c ∂2 ce,n ⎪
⎪ =0 (1)
εe,n e,n = Deff
e,n + an (1 − t+ )jn ⎨ ∂l ⃒
⎪
l=0
∂t ∂l2 ⃒ ⃒
⎪
⎪ ∂ce,n ⃒⃒ ∂ce,n ⃒⃒
⎩ Deff
⎪
e,n = Deff
e,sep
∂l l=l−n
⃒ ∂Il ⃒l=l+n
⎧ ∂c ⃒⃒
e,p ⃒
∂ce,p ∂2 ce,p ⎪
⎪ =0
Positive electrode solution phase diffusion εe,p = Deff + ap (1 − t+ )jp
⎪
⎨ ∂l ⃒l=ln +ls +lp (2)
e,p
∂t ∂l 2 ⃒ ⃒
⎪
⎪ ∂ce,p ⃒⃒ ∂ce,p ⃒⃒
⎩ − Deff
⎪
e,p = − Deff e,sep
∂l ⃒l=(ln +ls )− ∂l ⃒l=(ln +ls )+
⎧ ⃒ ⃒
⎪ ∂ce,sep ⃒⃒ ∂ce,p ⃒⃒
2
⎪
⎪ Deff = Deff
Separator area solution phase diffusion ∂ce,sep eff ∂ ce,sep
⎪
⎪
⎪
e,sep
∂l l=(ln +ls )
⃒ e,p
∂l ⃒l=(ln +ls )+ (3)
= De,sep
−
εe,sep ⎪
⎨
∂t ∂l 2 ⃒ ⃒
⎪ ce,n l=l− = ce,sep l=l+
⃒ ⃒
⎪ n n
⎪
⎪ ⃒
⎪
⎪ ⃒ ⃒
⎩ ce,p ⃒l=(ln +ls )+ = ce,sep ⃒
⎪
⃒ l=(ln +ls )−
( ) ⎧ ∂cs,n ⃒
Negative electrode solid phase diffusion ∂cs,n 1 ∂ 2 ∂cs,n ⎪
⎪
⎨ ∂r ⃒r=0
⃒ = 0 (4)
= Ds,n 2 r
∂t r ∂r ∂r ⃒
⎩ ∂cs,n ⃒ jn
⎪
⎪ ⃒
=−
( ) ∂r ⃒r=Rn Ds,n
Positive electrode solid phase diffusion ∂cs,p 1 ∂ 2 ∂cs,p (5)
= Ds,p 2 r
∂t r ∂r ∂r
⎧ ⃒
∂ϕohm ⃒
s,n ⃒ I
∂2 ϕohm ⎪ eff
Negative electrode solid phase Ohm's Law
⎪
⎪ − σ n ⃒ = (6)
σeff
n
s,n
= an Fjn ⎪
⎨ ∂l ⃒ A0
l=0
∂l 2 ⃒
⎪
⎪ ∂ϕohm ⃒
⎪ s,n ⃒⃒
⎪
⎩ =0
∂l ⃒ (7)
l=ln
⎧ ⃒
2 ohm ⎪
⎪ eff
∂ϕohm ⃒
s,p ⃒ I
Positive electrode solid phase Ohm's Law eff ∂ ϕs,p
⎪ − σ p ⃒ =
σp = a p Fj
⎪
⎪
⎨ ∂ l ⃒ A0
p l=l
∂l 2 n +ls +l p
⎪ ∂ϕohm ⃒⃒
⎪
⎪
⎪ s,p ⃒⃒
⎪
⎩ ∂l ⃒ =0
( )0.5 ( )0.5 [ ((1 − β )F ) ( l=ln +l)s ]
Butler-Volmer equation ji = ki cs,i
surf
cmax
surf
ce 0.5 exp i β F
ηi − exp i ηi , i = n, p (8)
s,i − cs,i
RT RT
3
Z. Yang et al. Journal of Energy Storage 59 (2023) 106504
creases to different levels. The temperature of a lithium-ion battery in There are three forms of heat transfer, namely heat transfer, heat
creases faster as the discharge current increases. The high battery tem convection and heat radiation. In the heat transfer process of lithium-ion
perature can affect the battery operation and even cause permanent battery, thermal radiation usually has a little influence on the battery, so
damage to the battery itself. The lithium-ion battery model contains it is usually ignored in the electrochemical heat generation model of
multiple sources of heat, as follows [43–45] lithium-ion battery. In the simulation process, the FEA software is used
to establish the three-dimensional thermal model of lithium-ion battery
Q = Qer + Qp + Qohm + Qsr (9)
[47].
where Qer is the heat of the electrochemical reaction, Qp is the polari ∂T ∂2 T ∂2 T ∂2 T
zation heat, Qohm is the ohmic heating, Qsr is the heat of secondary ρC P = λx 2 + λy 2 + λz 2 + q (11)
∂t ∂x ∂y ∂z
reaction.
When the lithium-ion battery is discharged normally, the tempera where λx, λy, λz are the anisotropic thermal conductivity, and q is the
ture of the battery will be below 90 ◦ C. In this case, the polarization heat battery heat generation rate.
generation, electrochemical heat generation and ohmic heating gener
ation reactions are mainly in operation. With the gradual increase in
time and battery temperature, a lithium-ion battery will undergo SEI 3.3. Validation model and sample data
film decomposition reaction, negative electrode and electrolyte reac
tion, positive electrode and electrolyte reaction and electrolyte decom Based on the theory discussed above, COMSOL Multi-physics soft
position reaction in sequence until the end of discharge or failure of the ware is used to calculate the battery terminal voltage, open circuit
lithium-ion battery. voltage and other battery performance parameters at every moment of
Bernardi et al. proposed a model of cell heat production with uniform lithium-ion battery operation. These parameters are set in the heat
internal heating [46]. The model has two assumptions: First, the battery generation model of the lithium-ion battery, while the temperature field
can be treated as a mass point with uniform heat generation; Second, the distribution of the battery is calculated by using the model.
heat generation of the battery mainly comes from the entropy change Due to the complex internal structure of an 18,650 battery, the mesh
heat generated by the chemical reaction of the battery itself and the quantity will be very large, therefore FEA is difficult to converge. In
ohmic heating generated by the polarization of the battery, ignoring order to reduce the computational complexity of the FEA, the finite
other heat generation factors inside the battery. This model reduces the element model is simplified while ensuring the accuracy of the model,
computational complexity of heat generation temperature prediction for and the battery is assumed to be the overall heat source. The selection of
Lithium-ion batteries, as described below mesh scale is very important for FEA. In order to select the optimal
[ ( )] convergent mesh, the lithium-ion battery surface temperature is used as
∂T dE the convergent parameter to conduct the mesh sensitivity analysis. Fig. 3
ρVCP = I (E − U) + T − hA (T − Tamb ) (10)
∂t dT shows that after the number of mesh elements exceeds 2 × 104, further
increase of mesh elements has little impact on the calculation results.
where ρ is the battery density, V is the battery volume, Cp is the specific Therefore, 2 × 104 elements are used as the baseline for the number of
heat capacity, E is the open circuit battery voltage, U is the terminal mesh elements in the subsequent calculation process.
voltage, I is the battery operating current, T is the battery temperature, Fig. 4 shows the comparison between the experiment and FEA tem
hA is the coefficient of heat convection, Tamb is the ambient temperature. perature distributions at the 3C discharge rates, where the highest
temperatures of the experiment and FEA are respectively: (a) 28.70 ◦ C
Table 3
and 28.51 ◦ C; (b) 29.35 ◦ C and 29.15 ◦ C; (c) 33.76 ◦ C and 33.52 ◦ C; (d)
P2D model parameters. 34.35 ◦ C and 34.09 ◦ C. In order to facilitate comparison with the
experimental data, the ambient temperature of FEA is set as the exper
Parameters Description Value Unit
imental temperature. According to the comparative analysis, the results
ce, n Negative electrode electrolyte concentration 2000 mol/m3 of the two methods are essentially the same, and the average relative
ce, Positive electrode electrolyte concentration 2000 mol/m3
p
errors between the two methods are 0.62 %, 0.68 %, 0.49 % and 0.43 %
ce, sep Separator electrolyte concentration 2000 mol/m3
Max concentration of negative electrode respectively, which are all within the acceptable range. Therefore, the
cmax 26,390 mol/m3
s, n
solid phase accuracy of the model is verified and the model can be used for subse
cmax
Max concentration of positive electrode solid
22,860 mol/m3
quent battery reliability analysis.
s, p
phase Currently, battery thermal runaway problem is a research hotspot in
cs, n Negative electrode solid phase concentration 14,870 mol/m3
cs, p Positive electrode solid phase concentration 3886 mol/m3
industry. Thermal runaway is a chain reaction caused by various factors,
3.9e- where a significant amount of heat and harmful gases emitted by the
Ds, Solid-phase Li diffusivity, negative electrode m2/s
n
14 reaction cause the battery to catch fire and explode. The solution to the
1.0e- thermal runaway problem is to improve the external protection (cooling
Ds, p Solid-phase Li diffusivity, positive electrode m2/s
13
mode) and internal improvement (material structure inside the cell), so
7.5e-
Deff
e, p Electrolyte Li diffusivity, positive electrode m2/s that the battery has better heat resistance and heat dissipation perfor
11
7.5e- mance. In order to show the influence of battery materials on thermal
Deff Electrolyte Li diffusivity, negative electrode m2/s
runaway more directly, the thermal analysis of batteries with different
e, n
11
7.5e- materials is carried out at 10C discharge rates (determined by experi
Deff
e, sep Electrolyte Li diffusivity, separator m2/s
11
ln Negative electrode thickness 79 μm
ment), and the FEA results are given in Fig. 5. For the convenience of
lp Positive electrode thickness 67 μm comparison, only the cell density was changed in the material parame
ls Separator thickness 25 μm ters, while the initial and boundary conditions of FEA are left
R Universal gas constant 8.314
J/ unchanged.
(mol•K)
Fig. 5(f) shows that maximum temperature of the battery varies with
εe, n Negative electrode porosity 0.357
the density: When the density is 2500 kg/m3, the maximum temperature
–
εe, sep Separator porosity 1 –
εe, p Positive electrode porosity 0.444 – is 161.73 ◦ C; When the density is 3300 kg/m3, the maximum tempera
σeff
n Solid phase conductivity, negative electrode 100 S/m ture is 132.22 ◦ C; When the density changes from 2500 kg/m3 to 3300
σeff
p Solid phase conductivity, positive electrode 3.8 S/m kg/m3, the temperature curve shows nonlinear characteristics. The re
Symmetry factor 0.5
sults show that when the density is larger, the battery temperature is
βi –
4
Z. Yang et al. Journal of Energy Storage 59 (2023) 106504
Fig. 4. Comparison of experiment and FEA. (a) 20 ◦ C-Sensor 1; (b) 20 ◦ C-Sensor 2; (c) 25 ◦ C-Sensor 1; (d) 25 ◦ C-Sensor 2.
Fig. 5. Thermal analysis results of the battery with different densities. (a) ρ = 2500 kg/m3; (b) ρ = 2700 kg/m3; (c) ρ = 2900 kg/m3; (d) ρ = 3100 kg/m3; (e) ρ =
3300 kg/m3; (f)Maximum temperature curve with density.
5
Z. Yang et al. Journal of Energy Storage 59 (2023) 106504
methods, the adaptive Kriging surrogate model has been widely used
because of its characteristics of unbiased estimation with the smallest Step 7. The convergence of AK-MCS method is determined. If the
estimated variance. The Kriging surrogate model can be expressed as convergence condition is not satisfied, the size of the sample set
follows [49] should be increased and Steps 3–6 repeated until the convergence
criterion is satisfied.
GK (X) = FT (X)⋅β + Q(X) (12)
where F(X) = [f1(X), f2(X), ⋅⋅⋅, fn(X)]T is the basis function of a random 4.2. Battery reliability assessment and reliability sensitivity analysis
vector X, and provides a global approximate model within the design
space; β = [β1, β2, ⋅⋅⋅, βn]T is the vector of regression coefficients, and is According to the reliability theory, the thermal reliability perfor
obtained to estimate the known response value; Q(X) is the Gaussian mance function model is expressed as [50]
stochastic process, and the statistical characteristics are expressed as
[49] G(X) = T * − T(X) (16)
where X = [ρ, Cp, λx, λz]T is the material parameters of the lithium-ion
battery, T(X) is the maximum temperature of the battery, and T * is
the maximum temperature threshold of the battery.
Table 4
300 groups samples between material parameters and maximum temperature. The battery reliability is calculated based on Eq. (15) of subsection
4.1, and the result is compared with the result of MCS. The results ob
Number ρ(kg/ Cp(J/ λx(W/ λz(W/ Maximum temperature
tained from the two methods are RAK = 0.8704 and RMCS = 0.8685,
m3) kg⋅K) m3) m3) (◦ C)
respectively, with a relative error of 0.2188 %. In order to better reflect
1 2512 1400 54.19 0.92 145.93
the influence of battery design parameters on its reliability, the AK-MCS
2 2653 1320 53.38 1.06 146.29
3 3101 1088 55.93 1.08 150.56 method is used to conduct the gradual reliability analysis and the
⋮ ⋮ ⋮ ⋮ ⋮ ⋮ sensitivity analysis when the mean value of each design parameter
298 3068 1108 48.71 0.82 150.02 change within a given range. The gradual reliability and reliability
299 2967 1124 52.73 1.08 151.93 analysis results are shown in Figs. 6-8.
300 2886 1203 50.2 1.07 147.20
The conclusion from Fig. 6 is as follow: The reliability increases as
6
Z. Yang et al. Journal of Energy Storage 59 (2023) 106504
Fig. 6. The gradual reliability curve of lithium-ion battery. (a)density; (b) specific heat capacity; (c) thermal conductivity in x-direction; (d) thermal conductivity in
z-direction.
Fig. 7. The mean sensitivity curve as the parameter change. (a)density; (b) specific heat capacity; (c) thermal conductivity in x-direction; (d) thermal conductivity in
z-direction.
the density increases. When the density reaches 3150 kg/m3, the reli be seen from Fig. 7 that the sensitivity values of the density and the
ability is stable above 0.99; With the specific heat capacity increasing, specific heat capacity are larger, while the sensitivity values of the
the reliability increases. When the specific heat capacity reaches 1310 J/ thermal conductivity are smaller. The greater the density and the spe
kg⋅K, the reliability is stable above 0.98; The thermal conductivity has cific heat capacity, the smaller the sensitivity values of all material pa
little influence on the reliability, and the reliability is generally between rameters. When the density reaches 3150 kg/m3, the sensitivity value is
0.86 and 0.87. 0.039 and starts to stabilize. When the specific heat capacity reaches
Fig. 7 shows the results of the mean value sensitivity analysis. It can 1310 J/kg⋅K, the sensitivity value is 0.041 and starts to stabilize. The
7
Z. Yang et al. Journal of Energy Storage 59 (2023) 106504
Data availability
Fig. 8. The standard deviation sensitivity curve as the design parameter mean Acknowledgments
change. (a)density; (b) specific heat capacity; (c) thermal conductivity in x-
direction; (d) thermal conductivity in z-direction. The authors are grateful for the support from the National Natural
Science Foundation of China (52172401), and the Fundamental
mean value of the thermal conductivity has little influence on the reli Research Funds for the Central Universities (N2003022).
ability, and the sensitivity value is generally between 3.99e-5 and 2.5e-
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