Safety research on the power Li-ion battery cells for electric vehicles · 2020. 9. 25. · I ....
Transcript of Safety research on the power Li-ion battery cells for electric vehicles · 2020. 9. 25. · I ....
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Safety research on the power Li-ion battery cells for electric vehicles
Sheng Yang
June 2020
Submitted in fulfilment of the requirements of the degree of
Doctor of Philosophy
Faculty of Science, Engineering and Technology
Swinburne University of Technology
Melbourne, Australia
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Abstract
The introduction of electric vehicles (EVs) is an effective measure to significantly
reduce greenhouse gas emissions associated with the usage of fossil fuels.
Lithium-ion (Li-ion) batteries have been considered as dominant energy storage
systems for EVs due to their advantages over other energy storage systems. However,
the poor thermal stability of Li-ion batteries has attracted more and more attention on
their safety and reliability as the development and expansion of EVs market.
The derivative of force with respect to displacement can be used to characterize the
stiffness of Li-ion batteries. In chapter 2, the stiffness of Li-ion batteries in the
quasi-static compression tests is analysed. It is found that the stiffness curve distinctly
shows three stages corresponding to densification stage, microscopic damage stage
and macroscopic failure stage. The Li-ion battery’s stiffness increases in the
densification stage while decreasing in the microscopic damage stage and
macroscopic failure stage. Hence, the constitutive model of the jellyroll of Li-ion
batteries is improved with considering microscopic damage, which is then validated
by the established explicit finite element model (FEM) of the Li-ion batteries. The
voltages and temperatures of Li-ion batteries are also measured to further compare
their responses at different stages. It is found that the internal short circuit of Li-ion
batteries at the fully charged state occurs in the microscopic damage stage while that
of Li-ion batteries at low and medium SOCs occurs in the beginning of macroscopic
failure stage.
Understanding the mechanical responses of Li-ion batteries during the EVs
collision is the key to solve subsequent thermal runaway problems, which involves
complicated and coupled behaviors. In chapter 3, several dynamic compression tests
are performed on two types of 18650 Li-ion batteries, namely LiNiCoAlO2 (NCA)
and LiNiCoMnO2 (NCM). Experimental results indicate that their abilities to resist
deformation both have positive relationship with the loading rate, namely, the strain
rate hardening behaviors. The strain rate hardening behaviors of NCM Li-ion batteries
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can be observed at low loading rate while that of NCA Li-ion batteries can only be
observed when the loading rate rises to a certain value. The constitutive model of the
jellyroll of Li-ion batteries is proposed with considering the strain rate hardening
behaviors, which is then validated by the established explicit FEM of the Li-ion
batteries. The proposed model can be used to evaluate the safety performance of
Li-ion batteries under crash accidents and provide useful information for the structure
design of battery packs in EVs.
The thermal runaway induced by the internal short circuit (ISC) of Li-ion batteries
under mechanical abusive conditions is another focus of EV industries. In chapter 4,
the coupled electrochemical-electric-thermal model is improved with considering the
material properties and the damaged area of the short circuit object, which can predict
the occurrence of thermal runaway of Li-ion batteries under various ISC conditions.
Simulation results indicate that the safety performance of Li-ion batteries under
mechanical abusive conditions can be improved by appropriately increasing the
adhesion strength between the aluminum current collector and the positive electrode.
All above-mentioned outcomes can provide valuable guidance for the safety design
of battery packs in EVs.
Key words: Li-ion batteries, Safety performance, Mechanical abusive conditions,
Constitutive model, Finite element model, Electrochemical-electric-thermal coupled
model
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Acknowledgement
This research work is completed under the careful guidance and patient help of my
principal supervisor Professor Cheng Lin and second supervisor Associate Professor
Wenwei Wang at Beijing Institute of Technology, China. It includes the selection of
the topic, the formulation of research content and program, the performance of related
work and the writing of this thesis. These two supervisors both give me meticulous
guidance, care and help not only in the side of my study and research but also in the
side of my life and emotion. In the side of my study and research, their profound
knowledge and excelsior attitude make me effectively carry out the related research of
safety performance of Li-ion batteries. In the side of my life and emotion, their
elegant style of conversation and common touch benefit me a lot and they also teach
me how to deal with people and things. Besides, they also try to create various
opportunities to send me to foreign countries to have academic communications with
world famous scholars, learn the latest research trends in the international frontier and
expand my academic horizons and enrich my research theories.
On the occasion of completing this thesis, I also would like to specially express my
sincere gratitude to my principal supervisor Associate Professor Weixiang Shen and
second supervisor Professor Guoxing Lu at Swinburne University of Technology for
their meticulous care and careful help. Their rigorous and realistic scientific attitude,
excelsior scientific style, sharp and meticulous scientific thinking and innovative
research awareness are beneficial to my whole life. Moreover, A/Prof. Shen strictly
requires every cooperative paper with excelsior attitudes and paid a lot of efforts to
review each paper and improve their qualities. Prof. Lu provided me a strong support
on my experiments.
Finally, I would like to express my sincere gratitude to Professor Rui Xiong. He
gives me a strong help and patient guidance on my research work. Besides, he offers
me a help, points out the aims for me and promotes me to move on without hesitation
when I lost the direction of both my study and life. Besides, I want to thank for the
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financial assistance of China Scholarship Council and Swinburne University of
Technology. Thanks also go to all experts and professors who reviewed this thesis,
your valuable comments and suggestions significantly improve this thesis.
I am very appreciated for my parents for their care, help, support, understanding
and tolerance, who bring me up and teach me to use ethical rules to guide my
behaviors. I will use the rest of my life to repay them.
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Declaration
This is to certify that the thesis entitled "Safety research on the power Li-ion
battery cells for electric vehicles" submitted in fulfillment of the requirements for the
Degree of Doctor of Philosophy in the Faculty of Science, Engineering and
Technology of Swinburne University of Technology, is my own original work and
that it contains no material which has been accepted for the award of any other degree
or diploma, except where due reference is made in the text of the thesis. To the best of
my knowledge, it contains no material previously published or written by another
person except where due reference is made in the text of the thesis.
Sheng Yang
June 2020
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List of Publications
1. SCI journal papers
[1] WW Wang*, S Yang, C Lin. Clay-like mechanical properties for the jellyroll of
cylindrical Lithium-ion cells. Applied Energy, 2017, 196: 249-258.
[2] WW Wang, S Yang*, C Lin, WX Shen, GX Lu, YD Li, JJ Zhang. Investigation
of mechanical property of cylindrical lithium-ion batteries under dynamic
loadings. Journal of Power Sources, 2020, 451:227749.
[3] S Yang, WW Wang*, C Lin, WX Shen, YD Li. Improved constitutive model of
the jellyroll for cylindrical lithium ion batteries considering microscopic
damage. Energy, 2019, 185: 202-212.
[4] WW Wang, S Yang*, C Lin, YD Li. State of charge dependent constitutive
model of the jellyroll of cylindrical Lithium-ion cells. IEEE ACCESS, 2018, 6:
26358-26366.
[5] S Yang, WW Wang*, C Lin, WX Shen, YD Li. Investigation of internal short
circuits of lithium-ion batteries under mechanical abusive conditions. Energies,
2019, 12: 1885.
2. EI and conference papers
[1] WW Wang*, S Yang, C Lin, YD Li. Measuring the internal short circuit
resistance under mechanical abusive conditions. International Conference on
Electric and Intelligent Vehicles (ICEIV2018), Melbourne, Australia, Nov,
2018.
[2] WW Wang*, S Yang, C Lin, YD Li. Mechanical and electrical response of
cylindrical Lithium-ion cells at various State of Charge. Energy Procedia 2018;
145; 128–132.
[3] WW Wang*, S Yang, C Lin, FC Sun. Mechanical behaviors of cylindrical
Lithium-ion cells at various State of Charge. International Symposium on
Electric Vehicles (ISEV 2017), Stockholm, Sweden, July 2017.
[4] WW Wang*, S Yang, C Lin. Clay-like mechanical properties of components for
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the jellyroll of cylindrical Lithium-ion cells. Energy Procedia 2016; 104;
56–61.
[5] WW Wang*, S Yang, FC Sun, QQ Yu. The Clay-like mechanics model of
cylindrical Lithium-ion battery cells under radial compression. Energy Procedia
2016; 88; 652–655.
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Contents
Chapter 1 Introduction ............................................................................. 1 1.1 Background and motivation .............................................................................. 1
1.2 Researches on mechanical properties of Li-ion batteries ................................. 1
1.2.1 Researches on mechanical properties of Li-ion batteries under
quasi-static loadings ......................................................................................... 2
1.2.2 Researches on mechanical properties of Li-ion batteries under dynamic
loadings ............................................................................................................ 4
1.3 Research contents of this thesis ........................................................................ 5
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings ...................................................... 6
2.1. Analysis of mechanical, electric and thermal responses of Li-ion batteries
under quasi-static loadings ...................................................................................... 6
2.2. Constitutive model for jellyroll of Li-ion batteries under quasi-static loadings
............................................................................................................................... 12
2.3. Validation and discussion ............................................................................... 16
2.4. Conclusions .................................................................................................... 19
Chapter 3 Investigation of safety performance of cylindrical Li-ion batteries under dynamic loadings ......................................................... 21
3.1. Analysis of mechanical, electric and thermal responses of Li-ion batteries
under dynamic loadings ........................................................................................ 21
3.2. Constitutive model for jellyroll under dynamic conditions ........................... 27
3.3. Validation and discussion ............................................................................... 28
3.4. Conclusions .................................................................................................... 31
Chapter 4 Investigation of Internal Short Circuits of Li-ion Batteries under Mechanical Abusive Conditions ................................................. 32
4.1 Investigating thermal responses of a Li-ion battery under various ISC
conditions .............................................................................................................. 32
4.1.1 Improved electrochemical-electric-thermal model ............................... 32
4.1.2 Effect of various ISC types on thermal responses ................................ 36
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4.1.3 Effect of the area of the ISC object on thermal responses .................... 39
4.1.4 Effect of the SOC of a Li-ion battery on thermal responses ................. 41
4.2 Validation and discussion ................................................................................ 44
4.3 Conclusions ..................................................................................................... 46
Chapter 5 Conclusions and Expectations ............................................. 47 5.1 Conclusions of this research ........................................................................... 47
5.2 Innovations of this research
............................................................................................................................... 47
5.3 Expectations in the future ............................................................................... 48
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List of Figures
2.1 (a) Measured force-time curve for cell 1 at the SOC of 100%; (b) Derivative of the
force with respect to time-stiffness; (c) Measured voltage and temperature
responses for cell 1 ............................................................................................... 7
2.2 (a) Measured force-time curve for cell 2 at the SOC of 20%; (b) Derivative of the
force with respect to time-stiffness; (c) Measured voltage response for cell 2 at
the SOC of 20% ..................................................................................................... 8
2.3 (a) Measured force-time curve for cell 3 at the SOC of 60%; (b) Derivative of the
force with respect to time-stiffness; (c) Measured voltage response for cell 3 at
the SOC of 60% ..................................................................................................... 9
2.4 (a) Measured force-time curve for cell 4 at the SOC of 100%; (b) Derivative of the
force with respect to time-stiffness; (c) Measured voltage and temperature
responses for cell 4 at the SOC of 100% ............................................................. 10
2.5 Measured force-displacement relations at various SOCs when the Li-ion battery is
compressed between two rigid flat plates and their analytical fittings: (a) SOC=0;
(b) SOC=0.2; (c) SOC=0.4; (d) SOC=0.5; (e) SOC=0.6; (f) SOC=0.8 ............... 13
2.6 Schematic description of Li-ion battery deformation compressed between two
plates .................................................................................................................. 14
2.7 Calculated and analytical stress-strain curves at various SOCs: (a) SOC=0; (b)
SOC=0.2; (c) SOC=0.4; (d) SOC=0.5; (e) SOC=0.6; (f) SOC=0.8 .................... 15
2.8 Simulated and measured force-displacement curves on Li-ion cells between two
rigid planes: (a) SOC=0; (b) SOC=0.2; (c) SOC=0.4; (d) SOC=0.5; (e) SOC=0.6;
(f) SOC=0.8 ......................................................................................................... 18
2.9 Simulated and measured force-displacement curves on Li-ion cells (a) under rigid
rod indentation, SOC=0.2; (b) under rigid rod, SOC=0.5; (c) under a
hemispherical punch, SOC=0.2; (d) under a hemispherical punch, SOC=0.5 .... 19
3.1 Compression tests at different loading rates: (a) INSTRON VHS 8800; (b) MTS
EXCEED E45; (c) Measured mechanical responses for NCM Li-ion batteries at
different loading rates; (d) Measured mechanical responses for NCA Li-ion
batteries at different loading rates ........................................................................ 22
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3.2 (a) INSTRON 5985; (b) FLUKE TI 400; (c) HIOKI 8880; (d) A NCA Li-ion
battery at the SOC of 100% ................................................................................. 23
3.3 (a) Measured load-time curve for NCM Li-ion battery at the SOC of 0.4; (b)
Measured voltage response; (c) Measured temperature response ...................... 24
3.4 (a) Measured Load-time curve for NCA Li-ion battery at the SOC of 0.4; (b)
Measured voltage response; (c) Measured temperature response ........................ 25
3.5 Calculated stress-strain curves for NCM Li-ion batteries at different loading rates
.............................................................................................................................. 28
3.6 Calculated stress-strain curves for NCA Li-ion batteries at different loading rates
.............................................................................................................................. 28
3.7 Simulated and measured force-displacement curves for NCM Li-ion batteries at
different loading rates: (a) v=0.5 mm/min; (b) v=5 mm/min; (c) v=25 mm/min;
(d) v=3 m/s ......................................................................................................... 29
3.8 Simulated and measured force-displacement curves for NCA Li-ion batteries at
different loading rates: (a) v=5 mm/min; (b) v=25 mm/min; (c) v=60 mm/min; (d)
v=3 m/s .............................................................................................................. 30
4.1 Thermal responses of various ISC conditions for a Li-ion battery at SOC = 0.2 and
0.5 mminr :(a) Positive–negative, (b) copper-positive, and (c)
aluminum-negative ............................................................................................ 38
4.2 Thermal response of various ISC areas, SOC = 0.4, positive–negative (a)
0.5 mminr , and (b) 1.5 mminr = .................................................................... 40
4.3 Thermal response of various ISC areas, SOC = 0.4, aluminum-negative (a)
=0.5 mminr , and (b) =1.5 mminr ........................................................................ 41
4.4 Thermal response of various capacities, =1.5 mminr , positive–negative (a) SOC =
0.2, and (b) SOC = 0.6 ....................................................................................... 42
4.5 Thermal response of various capacities, =1.5 mminr , aluminum-negative (a) SOC
= 0.2, and (b) SOC = 0.6 ...................................................................................... 43
4.6 Thermal responses under various loadings (unit: oC) at SOC = 0.2: (a) two rigid
plates, (b) a rigid rod, and (c) a hemispherical punch ........................................ 44
4.7 Thermal response of the battery compressed by a rigid rod (unit: oC) at SOC = 0.6
.............................................................................................................................. 45
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List of Tables
2.1 Specifications of 18650 Li-ion batteries ................................................................ 6
2.2 Fitting parameters ki, 0ia , 0ib and 0ic at various SOCs .................................. 12
2.3 Simulation parameters ......................................................................................... 17
3.1 Specifications of NCA 18650 Li-ion battery ......................................................... 21
3.2 Fitting parameters 1a , 1b and 1c for NCM and NCA L-ion batteries at various
loading rates ......................................................................................................... 27
4.1 Governing equations of the axisymmetric model ................................................ 33
4.2 Physiochemical parameters used in the axisymmetric model .............................. 34
4.3 The definition of those parameters used in improved coupled model ................. 35
4.4 Parameters of different internal short circuit (ISC) types .................................... 35
Chapter 1 Introduction
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Chapter 1
Introduction
1.1 Background and motivation
Electric vehicles (EVs) have been considered as an effective measure to alleviate
the emission of greenhouse gas associated with the usage of fossil fuels due to their
unique characteristics [1-7]. Li-ion batteries have been used as the dominant energy
storage for EVs due to their advantages over other types of energy storage in terms of
high energy/power density and long cycle life [8-15].
However, the poor thermal stability of Li-ion batteries has affected the safety and
reliability of EVs, especially when the energy/power density and physical size of
Li-ion batteries are increased to make EVs to meet the demand for long driving
mileage [16-18]. For an example, when Li-ion batteries operate above the normal
temperature range caused by mechanical abuse (e.g. EV crash) a series of exothermic
reactions may be triggered inside Li-ion batteries, leading to thermal runaway
[19-24].
Furthermore, highly energetic electrode materials, flammable electrolyte and the
oxygen produced by side reactions make thermal runaway of Li-ion batteries
extremely dangerous [25-30]. The catastrophic accidents associated with thermal
runaway are induced inside Li-ion batteries, which have been an obstacle for further
development and popularization of EVs. Therefore, there is an urgent need to
investigate the safety performance of Li-ion batteries and explore the mechanism of
thermal runaway under abusive conditions.
1.2 Researches on mechanical properties of Li-ion batteries
Li-ion batteries are mainly composed of two parts: a shell casing and the jellyroll.
The jellyroll consists of several identical single cells, which is composed of five
layers: positive/negative electrode (or cathode/anode), separator and copper/aluminum
foil. The electrolyte and separator are designed as a good ionic conductor but also act
as an electronic insulator, which allow Li-ions to pass while blocking electrons.
Chapter 1 Introduction
2
However, ISCs may be triggered inside a Li-ion battery under mechanical abusive
conditions (e.g. EV crashes) due to the failure of separator, or physical contact
between two electrodes or an electrode and a current collector (an aluminum or
copper foil) or two current collectors. This kind of ISC is the major cause for thermal
runaway. Hence, the understanding of mechanical properties of Li-ion batteries is the
key to reveal the complex mechanism of thermal runaway.
1.2.1 Researches on mechanical properties of Li-ion batteries under quasi-static
loadings
Some researchers focused on the mechanical property of separator and shell casing
of Li-ion batteries. Sheidaei et al. investigated the effect of electrolyte on the
mechanical property of a single layer of separator at both machine and transverse
direction [31]. They found that the mechanical properties of separators are anisotropic,
namely, the separators have different mechanical properties at different directions.
Zhang et al. investigated the mechanical properties of separators after several
charge/discharge cycles [32]. They found that the cycle number of separators had an
effect on their failure. Wierzbicki et al. calculated the compression resistance of the
metal casing and the positive end-cap of 18650 Li-ion batteries [33]. Although the
hardness of metal casing and the positive end-cap is high, their contributions to the
peak load of 18650 Li-ion batteries are small due to their small thickness.
Some researchers focused on the mechanical property of anode and cathode active
materials of Li-ion batteries. Zhang et al. utilized simulation to study the stress inside
electrode particles induced by the insertion of Li-ions [34]. They found that
decreasing the size while increasing the aspect ratios of electrode particles could
reduce the stress inside the electrode induced by the insertion/removal of Li-ions. Zhu
et al. studied the deformation mechanisms of electrodes of Li-ion batteries through
scanning electron microscope (SEM) [35]. They captured the derivation and
development of a number of cracks during the deformation process of electrodes.
Zhang et al. proposed the constitutive model of electrodes of Li-ion batteries, which
was used to predict their failure behaviors [36]. They also found that electrode failure
Chapter 1 Introduction
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was the combination of tensile and compression failure.
Some researchers focused on the mechanical property of electrolyte of Li-ion
batteries. Dixon et al. compared the deformation behaviors of Li-ion batteries with
and without electrolyte under mechanical tests [37]. It was found that the electrolyte
would decrease the force and displacement level of Li-ion batteries, namely, the
measured force and displacement of Li-ion batteries with electrolyte were smaller
than that of Li-ion batteries without electrolyte at the same loading scenarios.
Some researchers focused on the mechanical characteristics of whole Li-ion
batteries. Sahraei et al. utilized the experimental data measured from compression
tests to obtain the stress and strain relationship of pouch Li-ion batteries [38]. They
also found that the aluminum shell of pouch Li-ion batteries had obvious constraints
on its geometry structure, which affect its deformation and failure behaviors in some
cases. However, it was different from 18650 Li-ion batteries, whose steel shell had
little effect on its deformation and failure behaviors. Luo et al. investigated the
development of damage inside a pouch Li-ion battery under an indentation test. They
observed an important inflection point on the measured load-displacement curve of
pouch Li-ion batteries, which could be considered as the initiation of damage inside
Li-ion batteries [39].
An individual Li-ion battery is composed of several components with each
component made of different material. The material properties of some components
exhibited anisotropic. Xu et al. took the material anisotropy into consideration and
then improved the constitutive model of jellyroll, which could better predict the
mechanical responses of 18650 Li-ion batteries under bending cases [40]. The
mechanical properties and failure mechanisms of 18650 Li-ion batteries under axial
direction were investigated in [41] which found three causes as follows: 1) the
physical contact between the steel casing and the jellyroll due to the fracture of
separator. 2) the physical contact among different components of the jellyroll. 3) the
physical contact between the safety value and the jellyroll. They may contribute to the
trigger of ISC of Li-ion batteries under axial direction.
Chapter 1 Introduction
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Xu et al. [42] investigated the deformation and failure behaviors of 18650 Li-ion
batteries at various SOCs under both compression and bending tests. They found that
the structure stiffness of Li-ion batteries increased as the increase of SOCs while the
failure strain of Li-ion batteries had an inverse linear relationship with their SOCs,
namely, the failure strain of Li-ion batteries decreased as the increase of SOCs.
However, the SOC-dependent behaviors were found insignificant for pouch Li-ion
batteries under spherical punch head indentation tests [43]. They also found that the
SOC-dependent mechanical behaviors of Li-ion batteries are due to the internal stress
triggered by the constraint of volume expansion.
The above-mentioned researches focused on the mechanical properties of Li-ion
batteries at the fully discharged state or the effect of the SOC of Li-ion batteries on
their mechanical behaviors using experimentation. In this study, the constitutive
model of the jellyroll of Li-ion batteries is established under quasi-static loadings,
considering the effect of SOC.
1.2.2 Researches on mechanical properties of Li-ion batteries under dynamic
loadings
For EV industry and customers, the safety performance of EVs especially at the
time of vehicle collision is one of their focuses, which are concerned with mechanical
responses of Li-ion battery under dynamic loadings.
Kisters et al. investigated the effect of electrolyte on the dynamic responses of
Li-ion batteries [44]. They found the peak force of the elliptic Li-ion battery with
electrolyte increased by 25% under dynamic loadings while that without electrolyte
increased by 65%. Chen et al. performed drop-weight tests on prismatic Li-ion
batteries [45]. They observed three failure modes of Li-ion batteries under dynamic
loadings, namely there was a total loss of battery capacity, partial loss of battery
capacity and no loss of battery capacity. The above studies focused on
experimentation and result analysis.
Xu et al. utilized simulation to study the dynamic responses of cylindrical Li-ion
batteries [46]. Kermani et al. utilized a Johnson-Cook model to predict the mechanical
Chapter 1 Introduction
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responses of Li-ion batteries under dynamic tests [47].
Currently, all corresponding researches under dynamic loadings are still in the
preliminary stage and there is no systematic research method, so it is necessary to
investigate mechanical properties of Li-ion batteries under dynamic loadings to reveal
complex mechanism of thermal runaway, which has recently become a hotspot of the
research on battery safety.
1.3 Research contents of this thesis
Thermal runaway process of a Li-ion battery induced under mechanical abusive
conditions can be simply divided into three stages. In stage 1, the ISC is triggered
inside a Li-ion battery and battery temperature starts to increase due to the large Joule
heat generated by large ISC current. It should be noted that Joule heat induced by ISC
current is much larger than the heat generated by decomposition of solid electrolyte
interphase (SEI). In stage 2, thermal contraction of separator inside the battery will be
induced once temperature exceeds critical value of o120 140 C , which will cause
more serious ISC and stimulate battery temperature rise again. In stage 3, a chain of
side reactions inside a Li-ion battery is induced and battery temperature will increase
rapidly, leading to thermal runaway. The process of thermal runaway can’t be stopped
once it is triggered inside a Li-ion battery.
This research is hence divided into two parts to investigate the safety performance
of Li-ion batteries under various mechanical abusive conditions. The first part is
aimed to predict the trigger of the ISC inside a Li-ion battery. It analyzes the
mechanical, electric and thermal responses of Li-ion batteries and investigates the
failure and out-of-control behaviors of Li-ion batteries after ISC. Then, the
constitutive model of Li-ion batteries based on experimental data is proposed to
predict mechanical responses at the trigger of ISC inside Li-ion batteries. The second
part is aimed to predict the thermal runaway triggered inside a Li-ion battery after ISC.
It investigates the development process of ISC of Li-ion batteries and proposes the
electrochemical-electric-thermal coupled model of Li-ion batteries to predict the
thermal responses and the trigger of thermal runaway after various ISCs.
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings
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Chapter 2
Investigation of safety performance of cylindrical Li-ion
batteries under quasi-static loadings In this chapter, quasi-static compression tests are performed on 18650 Li-ion
batteries at various SOCs. The stiffness, electric and thermal characteristics of 18650
Li-ion batteries under quasi-static loadings are analyzed to investigate its safety
performance. The constitutive model of the jellyroll of a 18650 Li-ion battery is
proposed by considering the microscopic damage, which is then validated by the
established explicit FEM of a Li-ion battery.
2.1. Analysis of mechanical, electric and thermal responses of Li-ion
batteries under quasi-static loadings
Quasi-static compression tests are performed on 18650 Li-ion batteries at the SOCs
of 20%, 60% and 100% and the loading rate is 0.5 mm/min. The specifications of
these 18650 Li-ion batteries are shown in Table 2.1. The measured load-displacement
relation is converted into the load-time relation to easily compare with the
corresponding relation of voltage and temperature versus time. Besides, the stiffness
of a Li-ion battery is obtained through the derivative of force with respect to
displacement to further investigate its mechanical responses under compression tests.
Table 2.1. Specifications of 18650 Li-ion batteries
Items Specifications
Normal capacity 2100 mAh
Normal voltage 3.6 V
Charge voltage 4.2 0.05 V
Cut off voltage 2.5 V
Cathode Material LiNiCoMnO2
Fig. 2.1 (a) describes the force-time relation and Fig. 2.1 (b) describes the
stiffness-time relation. It indicates that the deformation process of a Li-ion battery can
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings
7
be divided into three distinct stages corresponding to densification stage, microscopic
damage stage and macroscopic failure stage.
Figure 2.1. (a) Measured force-time curve for cell 1 at the SOC of 100%; (b) Derivative of the
force with respect to time-stiffness; (c) Measured voltage and temperature responses for cell 1.
In stage 1, the stiffness of a Li-ion battery keeps rising as the compression continues
until it reaches its maximum value, as shown in Fig. 2.1 (b). In stage 2, the decrease in
stiffness of a Li-ion battery indicates that microscopic damage appears inside the
battery, including micro cracks or micro holes. The number and size of those micro
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings
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cracks or holes increase as the compression continues until the measured force
reaches its maximum value, as depicted in Fig. 2.1 (a) and (b). Finally, the
deformation process enters stage 3 as the occurrence of macroscopic fracture
indicated by the decrease in the measured force.
Figure 2.2. (a) Measured force-time curve for cell 2 at the SOC of 20%; (b) Derivative of the
force with respect to time-stiffness; (c) Measured voltage response for cell 2 at the SOC of 20%.
Fig. 2.1 (c) shows the measured voltage and temperature with respect to time. It is
noteworthy that the maximum force occurs at 1068 s (see Fig. 2.1 (a)) while the
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings
9
voltage starts to decrease and temperature starts to increase at 972 s, which indicates
that the ISC has been triggered before the measured peak force, namely, at stage 2.
After the ISC is triggered, the battery voltage slowly decreases from 4.11 V at 972 s to
4.03 V at 1072 s and the battery temperature slowly increases from 29.2 °C at 972 s to
35.18 C at 1072 s.
Figure 2.3. (a) Measured force-time curve for cell 3 at the SOC of 60%; (b) Derivative of the
force with respect to time-stiffness; (c) Measured voltage response for cell 3 at the SOC of 60%.
Once the measured force reaches its maximum value, the voltage rapidly decreases
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings
10
from 4.03 V at 1072 s to 1 V at 1102 s and the temperature rapidly increases from
48.1 C to 745.52 C within 4 s, which is contributed from the internal
macroscopic fracture.
Figure 2.4. (a) Measured force-time curve for cell 4 at the SOC of 100%; (b) Derivative of the
force with respect to time-stiffness; (c) Measured voltage and temperature responses for cell 4.
The Li-ion batteries at the SOCs of 20% and 60% are chosen to perform
indentation tests to investigate the trigger of ISC at low and medium SOCs. Fig. 2.2 (c)
shows the voltage response of cell 2 at the SOC of 20% and Fig. 2.3 (c) describes the
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings
11
voltage response of cell 3 at the SOC of 60%. The stiffness of a Li-ion battery is also
analyzed during the indentation tests, as shown in Fig. 2.2 (b) and Fig. 2.3 (b),
respectively. Several conclusions can be obtained from the experimental results as
observed in Figs. 2.2 and 2.3. Firstly, the deformation process of Li-ion batteries at
low and medium SOCs also shows three distinct stages. Secondly, for Li-ion batteries
at low and medium SOCs, the battery voltage is stable before the maximum force and
it then rapidly decreases after the maximum force. Thirdly, the ISC of Li-ion batteries
at the SOCs of 20% and 60% is triggered at the stage 3 (i.e. macroscopic failure
stage).
The other kind of indentation test is performed on cell 4 at the fully charged state to
further investigate its electrical and thermal response after the trigger of ISC. The
difference of the indentation test for cell 4 from cell 1 is that the indenter will be
stopped but its position is remained when the decrease is observed in the battery
voltage. It should be mentioned that the mechanical testing platform will maintain the
load until the indenter is removed. Fig. 2.4 describes the measured mechanical,
electrical and thermal responses of cell 4. The battery voltage slowly decreases from
4.11 V at 882 s to 3.87 V at 1162 s and then rapidly decreases to 1.07 V at 1182 s, as
shown in Fig. 2.4 (c). Whereas the battery temperature slowly increases from the
initial value of 28.4 C at 852 s to 49.19 C at 1292 s. The indenter is removed
when the battery temperature continuously decreases. Fig. 2.4 (c) shows that the
battery temperature increases again after the indenter is removed.
Again, several conclusions can be obtained from the above-mentioned experimental
results. Firstly, the ISC isn’t triggered when a Li-ion battery is compressed to the
initiation point of stage 2, no matter at the low, medium SOCs and even at the SOC of
100%. Secondly, the thermal runaway won’t be induced by the ISC triggered at stage
2 but can be induced at stage 3, especially for those Li-ion batteries at the SOC of
100%, where the battery voltage and temperature responses are rapid and dramatic.
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings
12
2.2. Constitutive model for jellyroll of Li-ion batteries under
quasi-static loadings
In this section, several 18650 Li-ion batteries at various SOCs are compressed
between two rigid plates and Fig. 2.5 describes the measured results. In all the
measured curves, it can be seen that there is one part from 0 mm to 3 mm representing
linear relationship and there is the other part from 3 mm onwards representing
exponential relationship. The Gaussian function is chosen to fit the exponential part
and a linear function simply passes the point (0, 0) and the inflection point in 3 mm.
Table 2.2 Fitting parameters ki, 0ia , 0ib and 0ic at various SOCs
SOC 0 0.2 0.4 0.5 0.6 0.8
Coefficient k 360.1 459.6 562 514 693.9 715.48
Coefficient 0a 73630 76360 78250 72030 74340 80190
Coefficient 0b 9.793 9.772 9.729 9.119 8.909 8.813
Coefficient 0c 3.307 3.38 3.435 3.121 3.125 3.055
Thus, the fitting function is described as follows
20 0 0
( 3)( ) exp( (( ) / ) ) ( 3)i
i i i
k w wH w a w b c w
(2.1)
where ki, 0ia , 0ib and 0ic are the fitting parameters. Table 2.2 lists the values of
those fitting parameters corresponding to each SOC and w is the displacement of top
plate in x direction.
The deformation process of a 18650 Li-ion battery compressed between two rigid
plates can be described in Fig. 2.6. H is the applied load corresponding to the
measured load and w is the displacement of top rigid plate in the x direction
corresponding to the measured displacement. Moreover, some following
simplifications are made based on the experimental observation:
(1) Length of a battery in the z direction remains unchanged during the whole
deformation process.
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings
13
Figure 2.5. Measured force-displacement relations at various SOCs when the Li-ion battery is
compressed between two rigid flat plates and their analytical fittings: (a) SOC=0; (b) SOC=0.2; (c)
SOC=0.4; (d) SOC=0.5; (e) SOC=0.6; (f) SOC=0.8.
(2) The perimeter of outside metal casing of the battery remains unchanged during
the whole deformation process.
(3) Shape of a battery in the x-y plane is comprised of three parts corresponding to
one rectangular part and two semicircular parts.
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings
14
Figure 2.6. Schematic description of Li-ion battery deformation compressed between two plates.
The strain in x direction at time t (i.e. x ) is calculated as follows.
( ) 2 ( ) 2x t r t R w (2.2)
( ) 2 ( ) 2x t t r t t R w dw (2.3)
( ) ( )( ) 2x
x t t x t dwdx t R w
(2.4)
0
2ln( )2 2
w
xdw RR w R w
(2.5)
The total volume of the 18650 Li-ion battery at time t is calculated as:
( ) (2 ( ) ( ) ( ) ( )) ( )( )2 2w wV t b t r t r t r t L L R R (2.6)
The volumetric strain of the 18650 Li-ion battery at time t (i.e. v ) is calculated as
follows:
( ) ( )( )2 2 2 2w dw w dwV t t L R R (2.7)
2( ) ( ) ( )( ) ( ) 2 2 2 2 2( ) ( )( )
2 2
V
dw w dw w dwR RV t t V td w wV t R R
(2.8)
Solving Eqs. (2.4) and (2.8) yields:
2ydwdR w
(2.9)
0
2ln( )2 2
w
ydw R wR w R
(2.10)
The equivalent stress and strain can be expressed as:
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings
15
Figure 2.7. Calculated and analytical stress-strain curves at various SOCs: (a) SOC=0; (b)
SOC=0.2; (c) SOC=0.4; (d) SOC=0.5; (e) SOC=0.6; (f) SOC=0.8.
2 2 2 2 2 22 ( ) ( ) ( ) 6( ) 2i x y x z y z xy yz zx (2.11)
2 2 2 2 2 22 3( ) ( ) ( ) ( ) 3 2i x y x y x y xy yz zx (2.12)
The shear forces inside the Li-ion battery and its strain in z direction are ignored,
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings
16
namely, 0 xy , 0 yz , 0 zx , and 0 z . The internal stress in x direction (i.e.
x ) is compressive stress while that in y direction is tensile stress (i.e. y ). The
following equations can be obtained based on the plastic flow rule:
2 2 2
222 2( )
x yix
x x y x y
dwd d dR w
(2.13)
2 2 2
222 2( )
y xiy
y x y x y
dwd d dR w
(2.14)
where is plastic ratio. Solving Eqs. (2.13-2.14) yields
2 22 2
x y
y x
R wR w
(2.15)
x can be calculated as:
xHbL
(2.16)
y can be obtained after solving Eqs. (2.15) and (2.16):
66y x
R wR w
(2.17)
Solving Eqs. (2.5), (2.10-2.12) and (2.16-2.17) can calculate the equivalent
stress-strain relation of a 18650 Li-ion battery. Fig. 2.7 describes the calculated
stress-strain results of Li-ion batteries corresponding to various SOCs.
2.3. Validation and discussion
The mechanical structure of an individual 18650 Li-ion battery mainly consists of
four parts corresponding to a steel casing, a positive end-cap, a jellyroll and a metal
core. In this study, only the jellyroll is considered in establishing the FEM of a Li-ion
battery since the effect of the other three parts on the battery's failure stress and strain
are small, ignoring their effect is beneficial to the mesh generation and the
improvement of computational efficiency and convergence. Moreover, the five layers
of jellyroll are integrated into a homogenized representative volume element (RVE)
during the establishment of its FEM. Hyperworks/Ls-dyna software is utilized to carry
out the simulation analysis. The mechanical property of the jellyroll is modeled by
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings
17
crushable foam (Material type 63) and its mechanical behaviors are considered as
isotropic. The material property of two plates is set as rigid, which is consistent with
the experimental setup. Fig. 2.7 are used as the input to crushable foam to model the
mechanical responses of 18650 Li-ion batteries at various SOCs. Table 2.3 lists other
simulation parameters. The displacement of the top plate is considered as the
simulated displacement and the contact force between the top plate and jellyroll is
considered as the simulated load.
Table 2.3. Simulation parameters.
Component Young’s modulus Poisson ratio Density Tensile cut-off value
Jellyroll jellyroll 1.5 GpaE jellyroll 0.15 -32.8 g cm 10 Mpaf
Three loading cases are chosen to validate the constitutive model, including the
compression test between two rigid plates, the indentation test with a rigid rod of 12
mm in radius and the compression test with a hemispherical punch of 7 mm in radius.
Fig. 2.8 shows the simulated force-displacement curves for the compression between
two rigid plates. In all curves, the simulation results in the part from 0 mm to 5 mm
have a good agreement with those corresponding experimental results. In the part
after 5 mm, the simulation results for Li-ion battery at the SOC below 0.6 (i.e.
SOC<0.6) also have a good agreement with those corresponding experimental results
(see Fig. 2.8 (a)-(d)) while those simulation results for Li-ion battery at the SOC over
0.6 (i.e. SOC>=0.6) do not agree well with those corresponding experimental results
(see Fig. 2.8 (e)-(f)). However, the simulated forces at 8 mm are 74146 N for a Li-ion
battery at the SOC of 0.6 and that for a Li-ion battery at the SOC of 0.8 is 80498 N.
The measured force at 8 mm is 69421 N and 75673 N, respectively.
Fig. 2.9 (a)-(b) show the simulated force-displacement curves for the indentation
test with a rigid rod of 12 mm in radius and Fig. 2.9 (c)-(d) show the simulated
force-displacement curves for the compression test with a hemispherical punch of 7
mm in radius. In all curves, the simulation results also have a good agreement with
those corresponding experimental results, especially for the peak force.
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings
18
Figure 2.8. Simulated and measured force-displacement curves on Li-ion cells between two rigid
planes: (a) SOC=0; (b) SOC=0.2; (c) SOC=0.4; (d) SOC=0.5; (e) SOC=0.6; (f) SOC=0.8.
The reasons for the errors between experimental and simulation results are as
follows.
(1) Ignoring the steel casing, the metal core and the positive-end cap in the
establishment of the FEM is responsible for the errors in the simulations especially in
the part from 0 mm to 4 mm.
(2) There are some gaps inside a real 18650 Li-ion battery. However, solid elements
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings
19
are utilized to establish the FEM of the jellyroll. This simplification is contributed to
the errors in simulation results especially in the part from 0 mm to 4 mm.
(3) The electrolyte isn’t taken into consideration in the establishment of the FEM of
the jellyroll and its material property is set as isotropic. This simplification may also
lead to the errors in simulation results for the part after 4 mm.
Even though many factors contribute to the errors, overall simulation results for
three loading cases agree well with those corresponding experimental results.
Figure 2.9. Simulated and measured force-displacement curves on Li-ion cells (a) under rigid rod
indentation, SOC=0.2; (b) under rigid rod, SOC=0.5; (c) under a hemispherical punch, SOC=0.2;
(d) under a hemispherical punch, SOC=0.5.
2.4. Conclusions
In this chapter, the stiffness, electric and thermal characteristics of a 18650 Li-ion
battery under quasi-static loadings are analyzed and it is proposed that the
Chapter 2 Investigation of safety performance of cylindrical Li-ion batteries under quasi-static loadings
20
deformation process of a 18650 Li-ion battery can be divided into three stages,
corresponding to densification stage, microscopic damage stage and macroscopic
failure stage. The effect of the SOC of a Li-ion battery on its failure and
out-of-control behaviors after ISC under quasi-static loadings are investigated. The
constitutive model of the jellyroll of a 18650 Li-ion battery is proposed by
considering the microscopic damage. The proposed model can be used to predict the
mechanical responses on the trigger of ISC under various quasi-static loadings, which
can benefit to the safety of Li-ion batteries in EVs.
Chapter 3 Investigation of safety performance of cylindrical lithium-ion batteries under dynamic loadings
21
Chapter 3
Investigation of safety performance of cylindrical Li-ion
batteries under dynamic loadings In this chapter, compression tests at various loading rates are performed on two
types of 18650 Li-ion batteries. The effect of the loading rate on the mechanical
property of a 18650 Li-ion battery is investigated. The mechanical, electric and
thermal responses of a 18650 Li-ion battery under dynamic loadings are analyzed.
The failure and out-of-control behaviors of a 18650 Li-ion battery after ISC under
dynamic loadings are investigated. The constitutive model of the jellyroll of a Li-ion
battery is proposed to describe its dynamic behavior, which is then validated by the
explicit FEM of a Li-ion battery.
3.1. Analysis of mechanical, electric and thermal responses of Li-ion
batteries under dynamic loadings
Compression tests at various loading rates are carried out on NCM and NCA 18650
Li-ion batteries. The specifications of the NCM Li-ion battery are the same as those in
the chapter 2.1 and those of the NCA Li-ion battery are listed in Table 3.1.
Table 3.1. Specifications of NCA 18650 Li-ion battery
Items Specifications
Normal capacity 2500 mAh
Normal voltage 3.7 V
Charge voltage 4.2 0.05 V
Cut off voltage 2.5 V
Cathode Material LiNiCoAlO2
Firstly, two types of Li-ion batteries are compressed at various loading rates to
investigate their dynamic responses and all batteries are discharged to their cut-off
voltage to avoid the occurrence of fire or even explosion during tests. Compression
tests at high speed are performed by INSTRON VHS 8800 as shown in Fig. 3.1(a)
Chapter 3 Investigation of safety performance of cylindrical lithium-ion batteries under dynamic loadings
22
and those at low speed are performed by MTS EXCEED E45 100 KN as shown in Fig.
3.1(b). Moreover, the compression tests at high speed are recorded by a high-speed
camera (i.e. Phantom V2512), as shown in Fig. 3.1(a). The measured load-time
relations are all converted into load-displacement relations to easily compare the
mechanical responses at different loading rates.
Figure 3.1. Compression tests at different loading rates: (a) INSTRON VHS 8800; (b) MTS
EXCEED E45; (c) Measured mechanical responses for NCM Li-ion batteries at different loading
rates; (d) Measured mechanical responses for NCA Li-ion batteries at different loading rates.
Chapter 3 Investigation of safety performance of cylindrical lithium-ion batteries under dynamic loadings
23
The loading rate for NCM Li-ion battery includes 0.5 mm/min, 5 mm/min, 25
mm/min and 3 m/s, respectively, while that for NCA Li-ion battery includes 0.5
mm/min, 5 mm/min, 25 mm/min, 60 mm/min and 3 m/s, respectively. The reliability
of experimental data of compression tests between two plates is ensured by repeating
each test at least three times. The measured load-displacement curves for NCM Li-ion
battery compressed at different loading rates are shown in Fig. 3.1(c) and those for
NCA Li-ion battery are described in Fig. 3.1(d). There are several similarities between
the mechanical response of NCM and NCA Li-ion battery. Firstly, the general trend of
mechanical response of NCM Li-ion battery compressed at different loading rate is
almost the same as that of the NCA Li-ion battery. Secondly, the measured load for
NCM and NCA Li-ion battery both increases as the increase in the loading rate,
namely, the strain rate hardening behaviors. There are also some differences between
the mechanical response of NCM and NCA Li-ion battery. Firstly, the strain rate
hardening behavior of a NCM Li-ion battery can be obviously observed from
measured load-displacement curves at low loading rates corresponding to 0.5 mm/min,
5 mm/min and 25 mm/min. However, the measured load-displacement curve for NCA
Li-ion battery is almost the same at the loading rate of 0.5 mm/min, 5 mm/min and 25
mm/min. Their strain rate hardening behaviors can also be obviously observed when
the loading rate reaches 60 mm/min.
Figure 3.2. (a) INSTRON 5985; (b) FLUKE TI 400; (c) HIOKI 8880; (d) A NCA Li-ion battery at
the SOC of 100%.
Chapter 3 Investigation of safety performance of cylindrical lithium-ion batteries under dynamic loadings
24
Figure 3.3. (a) Measured load-time curve for NCM Li-ion battery at the SOC of 0.4; (b) Measured
voltage response; (c) Measured temperature response.
NCM and NCA Li-ion batteries at the SOC of 0.4 are compressed between two
plates to further investigate the effect of the differences in the cathode materials on
their safety performance. It should be noted that these compression tests are
performed by INSTRON 5985 and the loading rate is set as 60 mm/min, as shown in
Fig. 3.2 (a). During the compression tests, the battery temperature is recorded in situ
by FLUKE TI 400 as shown in Fig. 3.2 (b) while the battery voltage is measured in
Chapter 3 Investigation of safety performance of cylindrical lithium-ion batteries under dynamic loadings
25
situ by HIOKI MR 8880 as shown in Fig. 3.2 (c). The measured relations of load,
voltage and temperature versus time of NCM Li-ion batteries are shown in Fig. 3.3
and those measured relations of NCA Li-ion batteries are shown in Fig. 3.4.
Figure 3.4. (a) Measured Load-time curve for NCA Li-ion battery at the SOC of 0.4; (b)
Measured voltage response; (c) Measured temperature response.
For the NCM Li-ion battery compressed between two plates, the maximum force
occurs at 7.83 s and its measured value is 92.47 kN, as depicted in Fig. 3.3 (a). The
battery voltage firstly remains stable before the measured force reaching its maximum
Chapter 3 Investigation of safety performance of cylindrical lithium-ion batteries under dynamic loadings
26
value and rapidly decreases from the initial voltage of 3.64 V at 8 s to 2.12 V at 8.5 s
and then continues to decrease to 0.01 V at 10.5 s, as depicted in Fig. 3.3 (b). The
battery temperature also firstly maintains stable before the maximum force and slowly
increases from the initial temperature of 17.03 C at 8.88 s to its maximum
temperature of 102.78 C at 86.58 s and then starts to slowly decrease, as depicted
in Fig. 3.3 (c).
For the NCA Li-ion battery compressed between two plates, the maximum force
also occurs at 7.83 s while its measured value is 90.817 kN, as depicted in Fig. 3.4 (a).
The battery voltage also firstly maintains unchanged before the maximum force and
rapidly decreases from the initial voltage of 3.64 V at 8.3 s to 1.65 V at 8.85 s and
then continues to decrease to 0.07 V at 8.9 s, as depicted in Fig. 3.4 (b). The battery
temperature also firstly maintains unchanged before the maximum force and slowly
increases from the initial temperature of 20.38 C at 9.99 s to its maximum
temperature of 112.51 C at 74.37 s and then starts to slowly decrease, as depicted
in Fig. 3.4 (c).
Several conclusions can be obtained from the experimental results. Firstly, the ISC
is triggered at the peak force for NCM and NCA Li-ion battery at the SOC of 0.4
under dynamic loadings, but the thermal runaway isn’t triggered inside both batteries.
Secondly, for NCM and NCA Li-ion battery at the SOC of 0.4, the battery voltage
both rapidly decreases to almost zero while the battery temperature both slowly
increases to the maximum temperature. Thirdly, the general trends of electrical and
thermal responses of the NCM Li-ion battery are almost the same as those of the NCA
Li-ion battery during the compression tests at the loading rate of 60 mm/min except
that the maximum temperature for the NCA Li-ion battery after the occurrence of ISC
is slightly higher than that of the NCM Li-ion battery. This is due to that the normal
capacity of NCA Li-ion battery is 2500 mAh while that of NCM Li-ion battery is
2100 mAh.
The compression tests are also performed on NCM and NCA Li-ion batteries at the
fully charged state (i.e. the 100% SOC), which causes strong fire during the
Chapter 3 Investigation of safety performance of cylindrical lithium-ion batteries under dynamic loadings
27
compression tests as shown in Fig. 3.2 (d). Thus, the battery voltage and temperature
can’t be measured due to the strong fire. This indicates that catastrophic accidents
may be caused at the collision of EVs especially when the ISC is triggered at the fully
charged state. Hence, more researches should be carried out to investigate the safety
performance of Li-ion batteries at the fully charged state under dynamic loading.
3.2. Constitutive model for jellyroll under dynamic conditions
For NCM and NCA Li-ion batteries, their deformation processes under
compression test at high loading rate is similar to those at low loading rate, which can
be seen in Fig. 2.6. Moreover, Fig. 3.1 shows that the general trend of mechanical
behaviors of NCM and NCA Li-ion battery at the high and low loading rate is similar.
Hence, those measured load-displacement curves at different loading rates are fitted
by Gaussian functions.
21 1 1( ) exp( (( ) / ) )H w a w b c (3.1)
where 1a , 1b and 1c are the fitting parameters. Table 3.2 lists the value of those
fitting parameters corresponding to each loading rate and w is the compression
displacement in x direction.
Table 3.2. Fitting parameters 1a , 1b and 1c for NCM and NCA Li-ion batteries at various
loading rates.
NCM Li-ion batteries NCA Li-ion batteries
Loading rete mm/min m/s mm/min m/s
0.5 5 25 3 5 25 60 3
Coefficient 1a 74.99 75.96 87.11 61.67 102.8 95.43 90.95 72.18
Coefficient 1b 10.26 9.927 10.19 6.835 9.981 9.766 9.566 7.014
Coefficient 1c 3.771 3.56 3.836 2.377 3.028 3.019 3.105 2.087
The calculation process from the measured load-displacement relationship to the
stress-strain relationship is the same as those explained in chapter 2.2. The calculated
equivalent stress and strain for NCM and NCA Li-ion battery compressed at different
Chapter 3 Investigation of safety performance of cylindrical lithium-ion batteries under dynamic loadings
28
loading rates is shown in Figs. 3.5 and 3.6, respectively.
Figure 3.5. Calculated stress-strain curves for NCM Li-ion batteries at different loading rates.
Figure 3.6. Calculated stress-strain curves for NCA Li-ion batteries at different loading rates.
3.3. Validation and discussion
The established FEM in chapter 2.3 is also utilized to validate the constitutive
model of a Li-ion battery under dynamic loadings, which is proposed in chapter 3.2.
All settings used in this section are consistent with those described in chapter 2.3
except for the following aspects. Firstly, the dynamic loading rate in the experiment is
used in the simulation. Secondly, the calculated stress-strain relations shown in Fig.
3.5 and 3.6 are used as the input to crushable foam to model the mechanical responses
of NCM and NCA Li-ion batteries at different loading rates, respectively.
The comparisons between the simulation and experimental results for NCM and
NCA Li-ion batteries compressed at different loading rates are shown in Fig. 3.7 and
Chapter 3 Investigation of safety performance of cylindrical lithium-ion batteries under dynamic loadings
29
Fig. 3.8, respectively.
Figure 3.7. Simulated and measured force-displacement curves for NCM Li-ion batteries at
different loading rates: (a) v=0.5 mm/min; (b) v=5 mm/min; (c) v=25 mm/min; (d) v=3 m/s.
Overall, the simulation results agree well with the corresponding experimental results
for both NCM and NCA Li-ion batteries. For the NCM Li-ion battery compressed at
the loading rate of 0.5 mm/min, the measured and simulation force at 8 mm is 52.08
kN and 55.05 kN respectively, as depicted in Fig. 3.7 (a). For that at the loading rate
of 5 mm/min, the measured force at 8 mm is 56.928 kN and the corresponding
simulation force is 59.57 kN, as shown in Fig. 3.7 (b). For that at the loading rate of
25 mm/min, the measured force at 8 mm is 63.557 kN whereas the corresponding
simulation force is 67.69 kN, see Fig. 3.7 (c). For that at the loading rate of 3 m/s, the
measured force at 6.08 mm is 57.919 kN and that at 6.318 mm is 58.2 kN while the
simulation force at 6.0866 mm and 6.286 mm is 59.893 kN and 67.193 kN
Chapter 3 Investigation of safety performance of cylindrical lithium-ion batteries under dynamic loadings
30
respectively, as shown in Fig. 3.7 (d).
Figure 3.8. Simulated and measured force-displacement curves for NCA Li-ion batteries at
different loading rates: (a) v=5 mm/min; (b) v=25 mm/min; (c) v=60 mm/min; (d) v=3 m/s.
For the NCA Li-ion battery compressed at the loading rate of 5 mm/min, the
measured force at 8 mm is 66.489 kN while the simulation force is 8.324 kN, as
depicted in Fig. 3.8 (a). For that at the loading rate of 25 mm/min, the measured and
simulation force at 8 mm is 67.105 kN and 69.944 kN respectively, as shown in Fig.
3.8 (b). For that at the loading rate of 60 mm/min, the measured force at 8 mm is
70.819 kN and the corresponding simulation force is 74.541 kN, see Fig. 3.8 (c). For
that at the loading rate of 3 m/s, the measured force at 6.7 mm is 71.398 kN while the
simulation force at 6.714 mm is 74.904 kN, as shown in Fig. 3.8 (d).
The reasons listed in chapter 2.3 are also responsible for the errors between the
experimental and simulation results in this section, which are induced by the
Chapter 3 Investigation of safety performance of cylindrical lithium-ion batteries under dynamic loadings
31
simplification involved in the establishment of FEM. Moreover, the prediction
accuracy of simulation force at 6.3 mm for the NCM Li-ion battery compressed at the
loading rate of 3 m/s is only approximately 84%. For the NCA Li-ion battery
compressed at the loading rate of 3 m/s, the relative error between the measured force
from 4.5 mm to 6.5 mm and the corresponding simulation force is also large. The
reasons are as follows. Firstly, under compression tests at the loading rate of 3 m/s,
aluminum foil is covered on the top and the bottom plate respectively to prevent the
corrosion of electrolyte. It may cause a slight slip during the compression process.
Secondly, according to the recorded videos for the compression tests at the loading
rate of 3 m/s, the movement process of the Li-ion battery can be divided into three
stages. The Li-ion battery firstly moves with the bottom plate (i.e. the indenter) and it
then shoots from the bottom plate to the top plate due to its inertia. Finally, the bottom
plate starts to compress the Li-ion battery. Hence, some measurement errors may be
caused during the compression test. Nevertheless, the established FEM has
sufficiently good accuracy to simulate the mechanical responses of 18650 Li-ion
batteries under dynamic loadings.
3.4. Conclusions
In this chapter, the mechanical, electric and thermal responses of a 18650 Li-ion
battery under dynamic loadings are analyzed. The effect of the loading rate on the
mechanical property of a 18650 Li-ion battery is investigated. The effect of the
cathode materials on the mechanical, electric and thermal responses of a 18650 Li-ion
battery is also investigated. These investigations have helped to understand the
mechanism of the failure and out-of-control behaviors of a 18650 Li-ion battery after
ISC under dynamic loadings. The constitutive model of the jellyroll of a Li-ion
battery is proposed to describe its dynamic behavior and can be used to predict the
mechanical responses at the trigger of ISC under dynamic loadings, which can
provide valuable guidance for the structure design of battery pack for EVs.
Chapter 4 Investigation of Internal Short Circuits of Lithium-Ion Batteries under Mechanical Abusive Conditions
32
Chapter 4
Investigation of Internal Short Circuits of Li-ion Batteries
under Mechanical Abusive Conditions In this chapter, the material property and the damaged area of the short-circuit
object is taken into consideration to improve the electrochemical-electric-thermal
coupled model, which is then used to investigate the thermal responses of a Li-ion
battery under various ISC conditions and predict the triggering of thermal runway.
4.1 Investigating thermal responses of a Li-ion battery under various
ISC conditions
4.1.1 Improved electrochemical-electric-thermal model
COMSOL Multiphysics (version 5.2a) is utilized to establish an axisymmetric
electrochemical-electric-thermal coupled model to investigate the thermal response of
Li-ion battery under various ISC conditions. In this model, the electrolyte is 3:7 EC:
EMC LiPF6 and the material of positive and negative electrode is
LiyCo1/3Ni1/3Mn1/3O2 and LixC6, respectively. Table 4.1 and 4.2 list the governing
equations and parameters used in the model. In Table 4.1, qr is defined as reaction
heat produced by the reaction overpotential, qj represents ohmic heat generated by
charge transport in the electrodes and electrolyte and qe is defined as reversible heat
(i.e. entropy heat). Some parameters listed in Table 4.2 are taken from [48-50] and the
others are estimated by a trial-and-error approach through simulation.
The small ISC resistance will induce large short-circuit current when the ISC is
triggered inside a Li-ion battery. Hence, the ohmic heat generated by large
short-circuit current should be taken into consideration when establishing the coupled
model, which is calculated by the following equations.
2S S
SISC
I RqV
(4.12)
Chapter 4 Investigation of Internal Short Circuits of Lithium-Ion Batteries under Mechanical Abusive Conditions
33
Table 4.1. Governing equations of the axisymmetric model.
Physical and chemical mechanisms Equations
Solid phase: Charge conservation ( )eff Lis j (4.1)
Electrolyte phase: Charge conservation ( ) ( ln )eff eff Lie D ek k c j (4.2)
Electrolyte phase: Conservation of Li+ species 0( ) 1( )eff Lie e
ec tD c jt F
(4.3)
Solid phase: Conservation of Li+ species 22 ( )s s sc D cr
t r r r
(4.4)
Energy conservation ( )
( )pe r j
c Tk T q q q
t
(4.5)
Electrochemical kinetics 0 exp[ ] exp[ ]Li a cs
F Fj a iRT RT
(4.6)
Overpotential s e U (4.7)
Exchange current density 0 ,max , ,( ) ( ) ( )a a ce s s e s ei k c c c c
(4.8)
Ohmic heat lneff eff effj s s e e e eq k k c (4.9)
Reaction heat ( )Lir s e jq j U (4.10)
Entropy heat ( )jLie
Uq j T
T
(4.11)
,s SS
s
IR
(4.13)
where ,s S represents the solid potential drop along the ISC object in the axial
direction, SR is defined as ISC resistance, and ISCV represents the volume of the ISC
object.
For a Li-ion battery under mechanical abusive conditions, the ISC resistance has a
strong correlation with the internal damaged area, which determines the short-circuit
current. The material property of the ISC object has some effects on the heat
dissipation. Hence, the above electrochemical-electric-thermal coupled model is
improved by considering the damaged area and the material property of the
short-circuit object. As discussed above, four types of ISC may be triggered inside the
Chapter 4 Investigation of Internal Short Circuits of Lithium-Ion Batteries under Mechanical Abusive Conditions
34
Li-ion battery under mechanical abusive conditions corresponding to
negative–positive ISC, aluminum-negative ISC, copper-positive ISC, and
aluminum–copper ISC.
Table 4.2. Physiochemical parameters used in the axisymmetric model.
Parameter Unit Cu Foil Negative
Electrode
Separator Positive
Electrode
Al Foil
Density 3kg/cm 38.9 10
31.2 10 45.3 10 32.9 10 32.7 10
Specific heat J/(Kg K) 385 1150 2050 1150 900
Thermal conductivity W/(cm K) 4.0 0.004 0.005 0.004 2.38
Electron conductivity S/cm 55.8 10 1.0 0.1 53.54 10
Thickness cm 410 10 498 10 417 10 492 10 415 10
Particle radius cm 410 10 48 10
Initial electrolyte
concentration
3mol/cm 0.001
Porosity 0.4
These parameters used in the improved coupled model at the negative–positive ISC
are calculated as follows.
2inS r (4.14)
1 1pos negS
pos neg
L LR
S S (4.15)
( )pos pos neg neg
Spos neg
L S L SL L S
(4.16)
pos pos neg negS
pos neg
C m C mC
m m
(4.17)
pos nega
pos neg
pos neg
L Lk L L
k k
(4.18)
Chapter 4 Investigation of Internal Short Circuits of Lithium-Ion Batteries under Mechanical Abusive Conditions
35
pos pos neg negr
pos neg
L k L kk
L L
(4.19)
The definitions of these parameters are listed in Table 4.3. It should be mentioned that
the ISC resistance mainly consists of two parts corresponding to the intrinsic and
contact resistance. It is difficult to determine the precise value of the contact
resistance especially for that involves in the ISC of Li-ion battery triggered under
mechanical abusive conditions due to the limitation of measuring techniques [48].
Hence, the ISC resistance only considers the intrinsic resistance in this chapter. Those
parameters under the other three ISC types are also calculated based on Equations
(4.14-4.19) and the values of those parameters are listed in Table 4.4.
Table 4.3. The definition of those parameters used in improved coupled model.
Parameter Definition Parameter Definition
L Thickness ak Thermal conductivity in the axial direction
m Mass of the ISC object rk Thermal conductivity in the radial direction
Density S Area of the ISC object
C Specific heat inr Radius of the area of the ISC object
k Thermal conductivity
Table 4.4. Parameters of different internal short circuit (ISC) types.
Parameter Unit Negative-Positive Al-Negative Cu-Positive Cu-Al
SR 0.1S
-39.8 10
S
-29.2 10S
-95.96 10S
S 3kg/cm 62003.8 10 61399 10 63458 10 -
SC J/(Kg K) 1150 1086 955.7 -
ak W/(cm K) 0.004 0.0046 0.0044 -
rk W/(cm K) 0.004 0.32 0.396 -
,s S V , ,s pos s neg , ,s al s neg , ,s pos s cu -
When ISC is triggered inside a battery, the un-shorted electrode layers and the
shorted electrode layers formed a closed loop current path, where the un-shorted
electrode layers were responsible to provide the energy to the shorted electrode layers
Chapter 4 Investigation of Internal Short Circuits of Lithium-Ion Batteries under Mechanical Abusive Conditions
36
[48]. Hence, the temperature in shorted electrode layers is higher than that in the
un-shorted electrode layers inside the Li-ion battery after ISC and the established
axisymmetric electrochemical-electric-thermal coupled model only takes the shorted
electrode layers into consideration.
Only one shorted electrode layer is taken into consideration in the establishment of
the axisymmetric electrochemical-electric-thermal coupled model and its radius is 3
cm. This simplification is explained as follows. Firstly, it is considerably difficult to
solve a detailed electrochemical-electric-thermal model and even a single layer has a
high computation burden. Secondly, all electrode layers inside the Li-ion battery are
fairly equivalent in the aspects of heat and electricity [51]. Thirdly, one established
shorted electrode layer has a similar working principle a whole Li-ion battery since it
consists of one layer of aluminum and copper current collector, one layer of separator
and one layer of positive and negative electrode. The effect of the electron transport
may be underestimated by this simplification to a certain extent, but it is still within a
reasonable range. The surface heat transfer coefficient is set to 5 W/(m2k) since this
chapter also investigates the effect of the material property of the ISC object on the
thermal response. This boundary condition may have some slight differences with the
real condition since the heat dissipation is also affected by those neglected layers, but
the effect brought by this setting should not be exaggerated and it is still within a
reasonable range. Besides, it is considered that thermal runaway is triggered inside a
Li-ion battery when its internal temperature exceeds o120 C .
4.1.2 Effect of various ISC types on thermal responses
The established axisymmetric electrochemical-electric-thermal coupled model is
utilized to investigate thermal responses of a Li-ion battery under various ISC types,
where the damaged area of the ISC object (i.e. the ISC resistance) and the SOC of the
battery is the same. Table 4.4 shows that the resistance of the copper-aluminum ISC
corresponding to 95.96 10 S is much less than that value of the
Chapter 4 Investigation of Internal Short Circuits of Lithium-Ion Batteries under Mechanical Abusive Conditions
37
aluminum-negative ISC corresponding to 39.8 10 S , which indicates that the
temperature rise of battery under copper-aluminum ISC is much more serious than
that under aluminum-negative ISC. Besides, recent research found that the ISC
process may be interrupted inside a Li-ion battery under copper-aluminum ISC due to
the melting of ISC current path induced by large Joule heat [50], which isn’t hence
investigated in this study.
Figure 4.1 shows the simulation thermal responses of a Li-ion battery under
different ISC types, where the SOC is 0.2 and the radius of the area of the ISC object
is 0.5 mm (i.e. rin=0.5 mm). The simulation thermal response under positive-negative
ISC is shown in Fig. 4.1 (a). It indicates that the temperature rise in the positive
electrode is similar to that in the negative electrode, which is higher than that in the
separator. For the simulation response under copper-positive ISC, the temperature rise
in the negative electrode is similar to that in the separator, which is slightly less than
that in the positive electrode, as shown in Fig. 4.1 (b). The simulation thermal
response under aluminum-negative ISC is described in Fig. 4.1 (c). The temperature
rise in the positive electrode is similar to that in the separator, which is less than that
in the negative electrode. The comparison between Fig. 4.1 (a) and (b) shows that the
temperature rise in the positive and negative electrode of a Li-ion battery under
positive–negative ISC is slightly higher than that under copper–positive ISC this is
due to the fact that the higher thermal conductivity of copper and higher resistance
under the positive-negative ISC than that under copper–positive ISC. Hence, the
influence of material property of the ISC object on the thermal response of a Li-ion
battery is important, which should be considered in the
electrochemical-electric-thermal coupled model.
Chapter 4 Investigation of Internal Short Circuits of Lithium-Ion Batteries under Mechanical Abusive Conditions
38
Figure 4.1. Thermal responses of various ISC conditions for a Li-ion battery at SOC = 0.2 and
0 5 mm .inr . (a) Positive–negative, (b) copper-positive, and (c) aluminum-negative.
Several conclusions can be obtained from the simulation results of a Li-ion battery at
the SOC of 0.2 and the radius of the area of the ISC object is 0.5 mm, as shown in Fig.
4.1. Firstly, the thermal response of a Li-ion battery under the aluminum-negative ISC
is stronger and quicker than that under other two types of ISC. Secondly, the
maximum temperature occurs inside the negative electrode for a Li-ion battery under
aluminum-negative ISC while that occurs inside the positive electrode under other
Chapter 4 Investigation of Internal Short Circuits of Lithium-Ion Batteries under Mechanical Abusive Conditions
39
two types of ISC. Hence, the hazard level of the aluminum-negative ISC is higher
than that of other two types of ISC since the initial temperature of these side reactions
occurring inside the negative electrode is lower than these inside the positive
electrode. The adhesion strength between the positive active materials and the
aluminum foil can be appropriately increased to improve the safety performance of
Li-ion batteries under mechanical abusive conditions. However, it should be noted
that plenty of glue for strengthening adhesion will degrade electrochemical
performance of Li-ion batteries.
4.1.3 Effect of the area of the ISC object on thermal responses
In this study, the established axisymmetric electrochemical-electric-thermal
coupled model is utilized to investigate thermal responses of the Li-ion battery
induced by different damaged areas of ISC object, where the SOC of the battery and
the type of ISC is the same as before. In general, the common ISC of a Li-ion battery
triggered under mechanical abusive conditions is the positive–negative ISC due to the
failure of separator. Moreover, the simulation results shown in Fig. 4.1 indicate that
the temperature rise in a Li-ion battery under the copper-positive ISC is slightly lower
than that under the positive–negative ISC. Hence, this section only investigates the
effects of different damaged areas of ISC object on the temperature rise in a Li-ion
battery under the positive–negative and aluminum-negative ISC.
Fig. 4.2 describes the simulation thermal response of a Li-ion battery at different
radii of the ISC object, where the SOC is 0.4 and the ISC type is the positive–negative
ISC. Fig. 4.2 (a) shows the simulation result for a Li-ion battery with the ISC object at
the radius of 0.5 mm, the temperature in the negative and positive electrode increases
from the initial value of o20 C to the maximum value of approximately o75 C
within 0.96 s. For a Li-ion battery with the ISC object at the radius of 1.5 mm, the
temperature in the negative and positive electrode increases from the initial value of o20 C to the maximum value of approximately o93 C within 0.17 s, as shown in
Fig. 4.2 (b).
Chapter 4 Investigation of Internal Short Circuits of Lithium-Ion Batteries under Mechanical Abusive Conditions
40
Figure 4.2 Thermal response of various ISC areas, SOC = 0.4, positive–negative (a)
0.5 mminr , and (b) 1.5 mminr = .
The simulation results of a Li-ion battery at different radii of the ISC object is
depicted in Fig. 4.3, where the SOC is 0.4 and the ISC type is aluminum-negative ISC.
For a Li-ion battery with the ISC object at the radius of 0.5 mm, the temperature in
the negative and positive electrode increases from the initial value of o20 C to the
maximum value of approximately o153 C and o138 C within 0.47 s, respectively,
as shown in Fig. 4.3 (a). For a Li-ion battery with the ISC object at the radius of 1.5
mm, the temperature in the negative and positive electrode increases from the initial
value of o20 C to the maximum value of approximately o196 C within 0.1 s and o140 C within 0.13 s, respectively, as shown in Fig. 4.3 (b).
Several conclusions can be obtained from the simulation results shown in Fig. 4.2
and 4.3. Firstly, for a Li-ion battery under both two types of ISC, the temperature rise
inside a Li-ion battery with a large damaged area is higher and quicker than that with
a small damaged area. Secondly, for a Li-ion battery under the positive–negative ISC,
Chapter 4 Investigation of Internal Short Circuits of Lithium-Ion Batteries under Mechanical Abusive Conditions
41
the thermal runaway may not be triggered inside the battery even with a large
damaged area, as shown in Fig. 4.2 (b), while the thermal runaway may be triggered
inside a Li-ion battery under the aluminum–negative ISC even with a small damaged
area, as shown in Fig. 4.3 (a). It accounts for the phenomenon observed during the
compression tests of 18650 Li-ion batteries that the thermal runaway may be triggered
inside a Li-ion battery compressed at a small displacement, while it may be not
triggered inside a Li-ion battery compressed at a large displacement.
Figure 4.3. Thermal response of various ISC areas, SOC = 0.4, aluminum-negative (a)
=0.5 mminr , and (b) =1.5 mminr .
4.1.4 Effect of the SOC of a Li-ion battery on thermal responses
The SOC of a Li-ion battery has positive correlation with its voltage and capacity.
Li-ion batteries in EVs may be at various SOCs at the time of vehicle collision. In this
study, the established axisymmetric electrochemical-electric-thermal coupled model is
utilized to investigate the thermal response of a Li-ion battery at various SOCs, where
the damaged area of the ISC object and the type of ISC is the same.
Chapter 4 Investigation of Internal Short Circuits of Lithium-Ion Batteries under Mechanical Abusive Conditions
42
Fig. 4.4 describes the thermal response of Li-ion battery at different SOCs, where the
ISC type is positive–negative ISC and the radius of the area of the ISC object is 1.5 mm
(i.e. 1 5 mm .inr ). For a Li-ion battery at the SOC of 0.2, the temperature in the
negative and positive electrode increases from the initial value of o20 C to the
maximum value of approximately o71 C within 0.12 s, as shown in Fig. 4.4 (a). For a
Li-ion battery at the SOC of 0.6, the temperature in the negative and positive electrode
increases from the initial value of o20 C to the maximum value of approximately o181 C within 0.63 s, as shown in Fig. 4.4 (b).
Figure 4.4. Thermal responses of various capacities, =1.5 mminr , positive–negative (a) SOC = 0.2,
and (b) SOC = 0.6.
The comparison between the simulation results shown in Fig. 4.4, Fig. 4.2 and Fig.
4.1 (a) shows that the effect of the increase in the SOC of a Li-ion battery on its
thermal response is more important than the effect of the decrease in the ISC
resistance when the ISC resistance decreases to a pretty low value. It explains for the
phenomenon observed under the indentation tests that the thermal runaway isn’t
Chapter 4 Investigation of Internal Short Circuits of Lithium-Ion Batteries under Mechanical Abusive Conditions
43
triggered inside the 18650 Li-ion battery at the SOC less than 0.4. The serious damage
inside the Li-ion battery is corresponding to a low ISC resistance when the internal
macroscopic fracture occurs under indentation tests.
Figure 4.5. Thermal response of various capacities, =1.5 mminr , aluminum-negative (a) SOC = 0.2,
and (b) SOC = 0.6.
Fig. 4.5 describes the thermal response of a Li-ion battery at different SOCs, where
the ISC type is aluminum–negative ISC and the radius of the area of the ISC object is
1.5 mm. For the Li-ion battery at the SOC of 0.2, the temperature in the aluminum
current collector and negative electrode increases from the initial value of o20 C to
the maximum value of approximately o153 C and o144 C within 0.07 s, as shown
in Fig. 4.5 (a). For the Li-ion battery at the SOC of 0.6, the temperature in the
aluminum current collector and negative electrode increases from the initial value of o20 C to the maximum value of approximately o424 C and o408 C within 0.36 s,
as shown in Fig. 4.5 (b).
Chapter 4 Investigation of Internal Short Circuits of Lithium-Ion Batteries under Mechanical Abusive Conditions
44
4.2 Validation and discussion As discussed in chapter 4.1.1, some simplifications are made in the establishment of
the axisymmetric electrochemical-electric-thermal coupled model in the COMSOL
Multiphysics, which only considers one shorted layer of electrode. For the validation,
obviously the predicted temperature from this established model cannot compare with
the measured temperature from a whole Li-ion battery, however it can be used to
predict the thermal runaway and then compare with the measured temperature
triggering thermal runaway of a whole Li-ion battery. The prediction of triggering
thermal runaway inside the Li-ion battery under mechanical abusive conditions is the
focus for the safety of EV industries. In this study, three loading cases corresponding
to the compression test between two plates, the compression test under a rigid rod,
and compression test under a hemispherical punch are performed on 18650 Li-ion
batteries at the SOC of 0.2 and 0.6. The specifications of the Li-ion batteries and the
mechanical testing platform are the same as those in the chapter 2.1. An infrared
camera (FLUKE TI 400) is used to record the surface temperature of a 18650 Li-ion
battery to determine if the thermal runaway is triggered.
(a)
(b)
(c) Figure 4.6. Thermal responses under various loadings (unit: oC) at SOC = 0.2: (a) two rigid plates,
(b) a rigid rod, and (c) a hemispherical punch.
All three loading cases are performed on 18650 Li-ion batteries at the SOC of 0.2,
where the radius of the rigid rod is 12 mm and that of the hemispherical punch is 7
mm. Fig. 4.6 shows that the recorded thermal responses of the 18650 Li-ion batteries.
Chapter 4 Investigation of Internal Short Circuits of Lithium-Ion Batteries under Mechanical Abusive Conditions
45
It should be mentioned that the left infrared image in Fig. 4.6 shows the maximum,
minimum, and average temperature of the Li-ion battery at the initial time of
macroscopic failure (i.e. peak force) under compression test while the right infrared
image in Fig. 4.6 shows the maximum, minimum, and average temperature of the
Li-ion battery at the time of reaching its maximum temperature. Moreover, the
moment of the trigger of a macroscopic failure inside the Li-ion battery is
corresponding to the initial time of recording temperature.
For a 18650 Li-ion battery compressed between two plates, its surface temperature
increases to the maximum value of o58.6 C after 300 s, as depicted in the right
infrared image in Fig. 4.6 (a). For a 18650 Li-ion battery compressed by a rigid rod,
its surface temperature increases to the maximum value of o92.5 C after 100 s, as
depicted in the right infrared image in Fig. 4.6 (b). For a 18650 Li-ion battery
compressed by a hemispherical punch, its surface temperature increases to the
maximum value of o81.5 C after 200 s, as depicted in the right infrared image in
Fig. 4.6 (c). These experimental results indicate that the thermal runaway isn’t
triggered inside the 18650 Li-ion battery at the SOC of 0.2 under all three loading
cases, they have a good agreement with the simulation results, where the thermal
runaway isn’t triggered inside the Li-ion battery no matter the sizes of the damaged
area and ISC types, as shown in Fig. 4.1, 4.4 (a) and 4.5 (a).
Figure 4.7. Thermal response of the battery compressed by a rigid rod (unit: oC) at SOC = 0.6.
For 18650 Li-ion batteries at the SOC of 0.6, the compression test under a rigid rod
is only carried out since the thermal responses of 18650 Li-ion batteries under three
loading cases are similar. Fig. 4.7 shows that the recorded thermal response of a
18650 Li-ion battery at the SOC of 0.6. The thermal runaway is triggered inside the
Li-ion battery only after 10 s, which simultaneously produces plenty of smoke, as
shown in the right infrared image of Fig. 4.7. It should be noted that the surface
temperature of 18650 Li-ion battery is obviously far higher than o90 C when the
thermal runaway is triggered. Moreover, the temperature measurement is also
Chapter 4 Investigation of Internal Short Circuits of Lithium-Ion Batteries under Mechanical Abusive Conditions
46
influenced by the generated smoke. Hence, the recorded temperature (i.e. o90 C ) in
the right infrared image of Fig. 4.7 is the temperature of the generated hot smoke
instead of the surface temperature of 18650 Li-ion battery. This experimental result
indicates that the thermal runaway is triggered inside the 18650 Li-ion battery at the
SOC of 0.6 under compression tests. For simulation results, the thermal runaway is
also triggered inside the Li-ion battery at the SOC of 0.6, no matter the types of ISC,
as shown in Fig. 4.4 (b) and 4.5 (b). The good agreement between the simulation and
experimental results validates the established model.
4.3 Conclusions
In this chapter, an improved axisymmetric electrochemical-electric-thermal coupled
model is established by considering the material property and the damaged area of the
short-circuit object, which can be utilized to predict the thermal responses of a Li-ion
battery under various ISC conditions and then determine if the thermal runaway is
triggered.
Chapter 5 Conclusions and Expectations
47
Chapter 5
Conclusions and Expectations
5.1 Conclusions of this research
This research investigates the mechanical, electric and thermal responses of Li-ion
batteries under both quasi-static and dynamic loadings in chapters 2-3 and establishes
the corresponding constitutive model of jellyroll of Li-ion batteries. It also establishes
an improved electrochemical-electric-thermal coupled model to investigate the
thermal responses of Li-ion batteries under various ISC conditions in chapter 4.
In summary, this research work provides the prediction of the mechanical responses
and the mechanical safety tolerance corresponding to the trigger of ISC of a Li-ion
battery under various mechanical abusive conditions and the determination of the
trigger of thermal runaway induced inside a Li-ion battery after various ISCs. This
research forms a primary theoretical system for the analysis of mechanical property of
Li-ion batteries and provides the theoretical foundation for the safety design of Li-ion
battery systems in EVs. This will benefit to the promotion of the healthy and rapid
development of EV industries.
5.2 Innovations of this research
(1) It is found that the deformation process of a 18650 Li-ion battery can be divided
into three stages corresponding to densification stage, microscopic damage stage and
macroscopic failure stage. The constitutive model of the jellyroll is proposed by
considering microscopic damage, which can be utilized to evaluate the safety
performance of 18650 Li-ion batteries under quasi-static loadings.
(2) The constitutive model of the jellyroll suitable for dynamic loadings is proposed
based on the experimental results, which can be utilized to evaluate the safety
performance of 18650 Li-ion batteries under dynamic loadings
(3) The electrochemical-electric-thermal coupled model is improved by considering
the material property and the damaged area of the short-circuit object, which can be
utilized to determine if the thermal runaway is triggered inside a Li-ion battery under
Chapter 5 Conclusions and Expectations
48
various ISC conditions.
The innovations of this thesis provide valuable guidance for the structure design of
battery packs for EVs and significantly improve safety of Li-ion batteries in EVs.
5.3 Expectations in the future
This research has made some achievements on the investigation of the safety
performance of Li-ion batteries under mechanical abusive conditions. However, there
is still a lot of work to do in solving the safety problems of Li-ion batteries. The
followings are the list of some problems for future research:
(1) The constitutive model of the jellyroll suitable for dynamic loadings needs to be
improved based on the investigation of the mechanical behaviors of the
components of the jellyroll under dynamic loadings.
(2) The evolution and development of microscopic damage inside the Li-ion batteries
under various mechanical abusive conditions need to be further investigated.
(3) The failure criterion of Li-ion batteries needs to be proposed, which can be
utilized to determine the type and position of ISC inside the Li-ion batteries under
various mechanical abusive conditions.
(4) The electrochemical-electric-thermal coupled model of Li-ion batteries needs to
be improved with adding a mechanical model.
49
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