Energy Conversion and Management 236 (2021) 114033

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Energy Conversion and Management

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

Heat and weight optimization methodology of thermal batteries by using

deep learning method with multi-physics simulation
Tae-Ryong Park *, Hyunseong Park , Kiyoul Kim , Chae-Nam Im , Jang-Hyeon Cho
Agency for Defense Development, P.O. Box 35, Yuseong, Daejeon 34186, Republic of Korea

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

Keywords: Thermal batteries are primary batteries, used in military applications, and must be designed to meet mission-
Thermal batteries specific requirements. This mission-specific nature makes the design of thermal batteries a pain-stacking task
Optimization as no specific guideline or concrete modeling technology is yet provided on optimizing heat, weight, energy
Deep learning
density, and other important criteria when the requirements are given. In this study, we present an optimization
Multi-physics simulation
methodology that can facilitate the weight-optimized design of a thermal battery by modeling the design pro­
cesses and optimizing accordingly. Using this methodology, a 25 cell Li-Fe thermal battery was optimized with
specific performance requirements as a case study. The performance of the thermal battery is highly dependent
on heat and thus it is important to accurately predict the temperature during the optimization process. The multi-
physics model can obtain accurate temperature prediction, but it takes a very long time to calculate and is
difficult to apply to the optimization problem. Therefore, a deep neural network (DNN) model trained from a
small number of multi-physics simulation data is adopted to overcome this issue. As a result, the DNN model
showed an accurate prediction result with a maximum error of 1.5 ◦ C, which is less than 1 % error. The DNN
model significantly improved the time-efficiency by reducing the calculation time per solution of the multi-
physics model, from 10 min to 0.01 s. The results indicate that our methodology can effectively guide the
optimal design of complex thermal battery systems.

1. Introduction temperature, current density, and pressure through an actual single-cell

A thermal battery is one of the most common primary reserve bat­
teries. It is generally used in military applications owing to its high
power and high reliability [1,2]. A thermal battery is activated when a
heat source is ignited and the solid electrolyte melts into a liquid with
ionic conductivity. In the inactive state, the electrolyte remains in a
solid-state so there is no self-discharge, even during long-term storage.
In addition, the lithium anode and metal sulfide cathode ensure a high
potential difference and exhibit high output characteristics. The per­
formance characteristics of the thermal battery include not only power
density and energy density, which are general battery performance
characteristics, but also heat-dependent performance. If the temperature
of the cathode exceeds 600 ◦ C, the FeS2 of the cathode is decomposed
and generates LiS2 with Li, reducing the performance and possibly
leading to thermal runaway. Conversely, if less heat is applied to the
electrolyte from the heat source, the ionic conductivity of the electrolyte
and performance of the battery decrease. Recently, Im et al. [3] opti­
mized the operating conditions of a thermal battery, such as
discharge test. It was found that the optimal temperature range for
thermal battery performance is 500–550 ◦ C. Therefore, the performance
of the thermal battery is greatly influenced by internal temperature.
Owing to the influence of internal temperature on performance,
several studies have been conducted regarding the development of a
thermal analysis model for predicting the temperature of a thermal
battery [4–7]. Thermal batteries require transient analysis and accurate
temperature prediction; thus, multi-physics models have been devel­
oped accordingly. Jang et al. [4] developed a multi-physics thermal
analysis model for a large-capacity thermal battery, considering heat by
heat source, joule heating, latent heat, and entropic cooling. The heat
balance of the battery was designed with the model and compared with
the actual battery performance. The model matched well with the actual
test results, proving its reliability. Lee et al. [7] also developed a multi-
physics thermal analysis model for a large-capacity thermal battery and
developed an effective thermal analysis model by applying effective
material properties to reduce the computation time. In previous studies,
precise multi-physics models have been developed that can predict the

* Corresponding author.
E-mail address: kaistryong@gmail.com (T.-R. Park).

https://doi.org/10.1016/j.enconman.2021.114033
Received 24 December 2020; Received in revised form 24 December 2020; Accepted 6 March 2021
Available online 27 March 2021
0196-8904/© 2021 Elsevier Ltd. All rights reserved.
T.-R. Park et al. Energy Conversion and Management 236 (2021) 114033

temperature of a thermal battery given its internal structure. However, prediction model is required in the process, a DNN model was used to
they still suffer from poor calculation time-efficiency, even if an effective reduce computation time. Using this methodology, a 25 cell Li-Fe
model is used. thermal battery was optimized as a case study and the results are pre­
Physics-based simulations using the finite element method are usu­ sented herein.
ally computationally expensive instead of providing accurate results. For
an optimization problem, such simulations must be run repeatedly and 2. Design and optimization methodology
performance predictions must be made for various combinations of
input values. Therefore, a full-scale simulation to search for an optimal 2.1. Internal structure of the thermal battery
design is computationally prohibitive. An effective way to reduce search
time is to use a surrogate model, i.e., a model of the relationship between Fig. 1 presents the general internal structure of a thermal battery
the input and output of the simulation, which can replace the expensive [3,4,7]. The thermal battery consists of a cell stack region, top and
physics-based simulation model. Recently, with the development of bottom stack regions, top and bottom insulator regions, and side insu­
machine learning technology, machine learning model — such as sup­ lation region. The unit cells are stacked in the cell stack region. In the top
port vector machine (SVM) or deep neural network (DNN) — has been and bottom stack regions, several heat pellets are added to maintain the
used as surrogate model [8–10]. In a related study in the field of elec­ heat of the thermal battery without cooling. To prevent decomposition
trochemical energy, Wang et al. [9] found an optimal catalyst layer of the 1st and nth unit cell due to the additional heat pellet in the top and
composition for maximizing the power density of polymer electrolyte bottom stack regions, few insulators are inserted. For the insulation of
fuel cell by using SVM as a surrogate model to replace the 3D CFD model. the battery, a mica insulator is applied to the top and bottom and a K-
Xu et al. [10] developed a DNN model with CFD simulation data to Shield BF ​ paper(BF, Morgan Thermal Ceramics) and BTU ​ Block(BTU,
obtain the thermal performance of a solid oxide fuel cell (SOFC), which Morgan Thermal Ceramics) insulators are used on the side. Finally, the
is difficult to obtain during online operation, enabling real-time opti­ case thickness is designed using stainless steel (SUS 304) to have
mization of SOFCs. In both studies, the SVM and DNN models showed adequate strength.
excellent prediction results, despite the small amount of training data. A unit cell of the thermal battery consists of a heat pellet
When applying an optimization problem to the thermal battery, the (Fe/KClO4 ), cathode (FeS2 with electrolyte salt), electrolyte
multi-physics model for temperature prediction can be replaced with the (LiCl-LiF-KBr with MgO), anode (Li-Fe or Li-Si), and current collector
surrogate model to significantly reduce calculation time. (stainless steel). The anode type has a marked effect on the discharge
Thermal batteries are not standardized in the same manner as other performance and stability [11]. It is known that two types of anodes are
batteries so a new design is required each time, according to the per­ widely used: Li-Si anodes and Li-Fe anodes. In this work, only the Li-Fe
formance requirements of the application system, e.g., operating time, anode is considered as it exhibits better discharge performance because
required current and voltage, and activation time [1]. However, many there is no voltage drop in the phase shift; it also exhibits better stability
parts of the design and optimization processes of the thermal battery at high temperatures than the Li-Si anode. The Li-Fe anode was prepared
remain in a trial-and-error method based on the experience of the by mixing lithium and Fe powder in a 13:87(w/w) ratio and then mol­
designer, consuming significant cost and time [3,5]. There are two major ded and pressed to form a disk-like shape. An FeS2 cathode is widely
challenges during the process: (1) the thermal battery is a specialized used because of its high reliability, capacity, and low cost. However,
primary battery, which is expensive and poses a risk of explosion if it is FeS2 has a disadvantage in that degradation occurs at high tempera­
incorrectly designed; hence, performing actual tests at the system level tures, which can cause performance degradation by forming LiS2 inside
consumes a lot of cost and time. Therefore, since many tests are the thermal battery. The cathode was prepared by mixing 75 wt% FeS2 ,
impossible, an accurate modeling technique for the design is essential 25 wt% LiCl-KCl eutectic salt(with MgO), and 1.5 wt% of LiO2 and then
and must be designed accordingly. (2) The performance of the thermal pressing. For the electrolyte, 55 wt% LiCl-LiF-KBr eutectic salt and 45
battery is strongly dependent on temperature so the thermal design must wt% MgO binder were mixed and pressed similarly. The electrochemical
proceed simultaneously with the battery design. However, temperature reaction of the unit cell is as follows:
prediction using a multi-physics model requires significant calculation
time and many design candidates cannot be considered. From this
perspective, research on the design and optimization methodology of a
thermal battery that can reduce cost and time is imperative.
Although optimizing the design of the thermal battery plays a very
important role in battery performance, to the best of our knowledge, no
research has been conducted on the design and optimization of thermal
batteries at the system level. However, application systems continue to
demand lighter and higher performance thermal battery systems, which
is a great challenge. Therefore, in this study, we introduce a method­
ology for optimizing the heat and weight of a thermal battery by
modeling the design process. In the methodology, the modeling for the
capacity, power, and heat of the thermal battery was developed using
theoretical and experimental approaches. In addition, as a temperature
prediction model is required in the process, a DNN model — trained
from the multi-physics simulation — is adopted to reduce computation
time. The methodology allows designers to obtain an optimized design
of a thermal battery with low cost and time so they can easily design
high-performance thermal batteries that meet the system requirements.
A summary of the methodology is provided. First, it is determined which
parts of the internal structure of the thermal battery must be set as
design parameters to be optimized. Second, the optimization problem is
formulated using thermal battery design modeling. Next, the optimiza­
tion problem is solved using an optimization algorithm for numerous
combinations of design parameters in design space. As a temperature Fig. 1. Schematic of thermal battery design (2-D axisymmetric).

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T.-R. Park et al. Energy Conversion and Management 236 (2021) 114033

Anode : Li→Li+ + e−
Cathode : 3Li+ + 3e− + 2FeS2 →Li3 Fe2 S4
Overall Reaction : 3Li + 2FeS2 →Li3 Fe2 S4
1 mol of FeS2 reacts with 1.5 mol of Li. The heat pellet plays a pivotal
role in the cell. By supplying heat to the cell through burning of the heat
pellet, the cell operates at a high temperature. The heat source pellet
contains Fe and KClO4 in a ratio of 84:16(w/w).
2.2. Design method of the thermal battery
The thermal battery is a primary battery so it is redesigned whenever
the performance requirements of the application system change. From
the application system, the current profile during the operating time,
cut-off voltage, weight limit, and volume limit are given. The terminal
voltage of the cell must not be lower than the cut-off voltage while
drawing the given current profile during the operating time. In this
study, to simplify the thermal battery design, the current profile is not
reflected but the average current in the equation below is used.
∫ toperating time
Irequired =
1
I(t)dt (4)
toperating time 0
When the performance requirements are provided, a Li-Fe thermal
battery is usually designed as follows. First, the number of unit cells
stack in the cell stack region is determined by choosing the cut-off
voltage of the unit cell according to cut-off voltage requirements. For
example, assuming a cut-off voltage requirement of 32 V, if the cut-off
voltage of the unit cell is selected as 1.6 V, 20 unit cells are selected.
When considering the discharge characteristics of the Li-Fe thermal
battery, the unit cell cut-off voltage is mainly selected as a value of 1.6 V
to 1.75 V [3]. Second, the current density, i.e., the diameter of the
electrode, should be designed according to the current requirements. If
the same current is drawn, the diameter becomes larger if a high current
density is selected and the diameter becomes smaller if a low current
density is selected. As the thermal battery is a battery with high output
characteristics, a high current density of 0.1–0.8 A/cm2 is used.
Next, once the electrode diameter is determined, the weight of the
anode and cathode can be designed to meet the capacity requirement
(Crequired ) as shown in Table 1. The unit theoretical capacity (cLi , cFeS2 ) of
the active material of the anode and cathode, which are Li and FeS2 ,
respectively, can be calculated from Faraday’s law. In Faraday’s law, n
represents the number of charge carriers, F is the Faraday constant, and
Mw denotes the molecular weight. Using the electrochemical Eqs. (1)–
(3), the n values of the anode and cathode are 1 and 1.5, respectively.
The Mw of Li and FeS2 are 6.9 g/mol and 120 g/mol, respectively. The
Faraday constant is 96,485 C/mol. Then, the unit theoretical capacity
(cAnode , cCathode ) of the anode and cathode can be obtained based on the
(1) weight ratio (αLi , αFeS2 ) of the active material. The weight ratio (αLi , αFeS2 )
can be obtained from the composition of the Li–Fe unit cell described in
(2) the previous section. According to the actual single-cell discharge tests,
the actual capacity is much lower than the theoretical capacity,
(3) depending upon the temperature and current density. Therefore, the
utilization coefficient (η) must be applied and obtained through an
actual test. Because it is widely known that the optimum temperature
range for thermal battery operation is 500–550 ◦ C, a single cell
discharge test was conducted at 500 ◦ C to obtain the capacity-current
density data. The discharge results are presented in Fig. 2. Based on
the results, Fig. 3 illustrates the relationship between the utilization
coefficient and current density according to different cut-off voltages.
The utilization coefficient is calculated as the actual unit anode capacity
(cAnode.actual ) divided by the theoretical unit anode capacity (cAnode ). A
linear interpolation method can be applied to obtain unmeasured utili­
zation coefficients. Finally, the weight is obtained by dividing the ca­
pacity requirement by the actual unit capacity. Since the weight,
diameter, and density of the anode and cathode are determined, the
thicknesses of the anode and cathode can be determined. In addition, if
the anode and cathode diameters are the same, the thickness ratio of the
anode and cathode is fixed as 1:2.35. In the case of the electrolyte, the
thinner the electrolyte, the better the performance of the battery.
However, if it is too thin, the battery becomes unstable [12]. It is pri­
marily determined in the thickness range of 0.4–0.6 mm and trial-and-
error testing is required after design. The thickness of the heat pellet is
an important design factor that determines the amount of heat generated
by the battery. It must be designed to maintain the temperature of each
cell in the range of 500–550 ◦ C during operation. However, this must be
verified through a multi-physics simulation and discharge test after the
design. The number of additional heat sources, number of top and bot­
tom mica insulation, and number of BTUs of the side insulation are
adjusted in an empirical manner depending on the operating time of the
application to achieve the optimal thermal insulation design. These in­
sulators play a crucial role in maintaining the proper temperature by
adjusting the heat loss to the surroundings during operation. The acti­
vation time refers to the time taken to measure the voltage of the battery
after the battery is ignited and the electrolyte is melted and activated. In
military applications, such as missiles, shortening of the activation time
is required for rapid launch. The activation time is related to the heat
conduction phenomenon between electrodes, which occurs in a very
short time and can only be confirmed via the actual discharge test. Here,
the activation time was defined as when the temperatures of all elec­
trolyte parts were 443 ◦ C, which is the melting point of the electrolyte;
this approach is thought to be meaningful for the simulation, despite the

Table 1
Anode and cathode weight design method that satisfies capacity requirements.
Anode Cathode Description Unit

Capacity Crequired Crequired Crequired = Irequired toperatingtime As

Requirement
Weight ratio of 0.13 0.75 αLi , αFeS2 const
active material
Theoretical 13983 1206 cLi , cFeS2 = nF/Mw As/g
capacity of
active material
Theoretical 1817 784 cAnode = αLi cLi As/g
capacity cCathode = αFeS2 cFeS2
Utilization η η η = cAnode.actual /cAnode const
coefficient
Weight Wanode Wcathode Wanode = Crequired /(cAnode.actual ) g
Wcathode = Crequired /(cCathode.actual )
Fig. 2. Single-cell discharge result according to current density at 500 ◦ C.

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T.-R. Park et al.
Fig. 3. Utilization coefficient according to current density and cut-off voltage.
voltage being measured before the electrolyte is completely dissolved.
As explained above, the performance of the thermal battery, especially
the thermal-dependent performance, varies greatly depending on the
internal structure, and now relies on the multi-physics model. The
problem is that calculations in multi-physics simulations are time-
consuming, making it difficult to verify various designs.
2.3. Framework of optimization methodology
Fig. 4 shows the workflow of the optimization methodology used in
this study. This methodology aims to obtain a thermal- and weight-
optimized thermal battery structure based on certain performance re­
quirements. First, once the performance requirements are determined,
the parameters to be optimized are determined. Second, the optimiza­
tion problem was formulated by modeling the design method of the
thermal battery. Third, the optimization algorithm verifies whether the
Fig. 4. Work flow of the optimization methodology.
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Energy Conversion and Management 236 (2021) 114033
constraints in the optimization problem are satisfied for the parameters
in the design space and determines the lightest weight among the pa­
rameters that satisfy all the constraints. However, because the con­
straints include a function of temperature, a temperature prediction
model is required. The DNN model was used as the temperature pre­
diction model instead of the multi-physics model because the use of the
latter requires a tremendous computation time instead of making ac­
curate temperature predictions. However, if we simulate a multi-physics
model with a small number of parameters in the design space and sub­
sequently train a DNN model using this data, the DNN model can pro­
vide accurate and computationally fast temperature prediction.
Therefore, the DNN model plays the role of a surrogate model that
predicts the temperature of the thermal battery while solving the opti­
mization problem with the optimization algorithm. The accuracy of the
DNN model was verified by comparing it with the temperature predic­
tion results from the multi-physics simulation. For the final validation,
after the optimization algorithm is completed, the optimized structure is
checked to determine whether it satisfies the constraints through a
multi-physics simulation
3. Case study
3.1. Performance requirements and optimization problem formulation
The Li-Fe battery was optimized by applying introduced optimiza­
tion methodology. The following cases were randomly assumed to be the
performance requirements, and the optimization process was performed
to obtain the lightest and thermally optimized design for each case.
Case 1: Cut-off voltage = 40 V, Current requirement = 30 A, Oper­
ating time = 500 s, Activation time = 0.8 s
Case 2: Cut-off voltage = 43.8 V, Current requirement = 10 A,
Operating time = 1000 s, Activation time = 1.0 s
In this study, the number of unit cells for both cases was assumed to
be 25. Therefore, in case 1, the cut-off voltage of the unit cell is 1.6 V,
and in case 2, it is 1.75 V. As shown in Fig. 5, a total of 7 design pa­
rameters, including electrode diameter (D), electrolyte thickness (ET),
T.-R. Park et al.
Fig. 5. Seven optimization parameters for designing thermal battery.
anode thickness (AT), heat pellet thickness (HT), additional heat pellet
thickness (AHT), mica thickness (MT), and BTU thickness (BT) were
selected as optimization parameters. The bottom stack region and bot­
tom insulator region were designed to be symmetrical to the top. The
thickness of the cathode was designed to be 2.35 times the thickness of
the anode, as explained in the previous section. The insulator thickness
(2 mm) of the top stack region, BF thickness, current collector thickness
(0.08 mm), and the case thickness (2 mm) of the battery were assumed
to be constant. Although these parameters are also subject to optimi­
zation considerations, for the simplification of the optimization process,
they were applied as constants. Because the same dimensions are used
for all thermal battery, or the effect is considered to be insufficient to
affect performance.
The optimization problem is presented in Table 2. The cost function
was set as the total weight of the thermal battery. The weight is calcu­
lated by multiplying the volume of each element by the density. As an
optimization constraint, first, the current density which is a function of
the required current and diameter, was set as a constraint to be 0.1–0.8
A/cm2 . Next, the anode capacity calculated from the amount of active
material with volume of the anode is determined to be greater than the
required capacity. Here, the utilization coefficient was obtained by
linear interpolation of the data in Fig. 3. Finally, the temperature of the
electrolyte was set between 500 and 550 ◦ C, and the temperature of the
cathode was set to not exceed 600 ◦ C during the operating time.
Table 2
Optimization problem formulation.
Function/Parameter
Given Vcutoff , Irequired , toperatingtime ,tactivationtime
Parameter μ = (D, ET, AT, HT, AHT, MT, BT)
Minimize Wtotal (μ)
Subject to 0.1 ≤ J(Irequired , D) ≤ 0.8
η(J, Vcutoff )
Canode (D, AT, η) ≥ Irequired toperatingtime
tTelectrolyte =443 (μ) ≤ tactivationtime
500 ≤ Telectrolyte (μ, t) ≤ 550
Max{Tcathode (μ, t)} ≤ 600
Energy Conversion and Management 236 (2021) 114033
3.2. Development of multi-physics model
A two-dimensional (2-D) thermal analysis model is built for thermal
batteries using COMSOL Multiphysics software for the optimization. In
the model, the heat generated from the heat pellet, joule heating during
discharge, latent heat due to the electrolyte and lithium melting, heat
loss to the surroundings, and entropic cooling were considered. The
overall equation of the heat analysis is expressed as follows.
∂T
ρC p = qheat source + ∇∙(k∇T) − qfusion + qjouleheating − qentropiccooling (5)
∂t
To demonstrate the activation process of the thermal battery, the
heat pellet was designed to burn at a speed of 10 cm/s from the inner
diameter to the outer diameter after the ignition [13]. The heat amount
of the heat pellet is set to 1243 × 103 J/kg.
The ignition signal between the heat pellets proceeds by burning the
thin heat paper wrapped in the middle hole, and the burning speed is
known to be very fast. Therefore, it is assumed that all heat pellets are
ignited at the same time. The heat of phase change is also applied in the
electrolyte, cathode, and anode by applying the melting point and latent
heat of the electrolyte and lithium. The latent heat properties were
estimated to be 266 × 103 J/kg for LiF-LiCl-LiBr and 422 × 103 J/kg for
lithium [5,6]. Melting points of 443 ◦ C and 180 ◦ C were adopted for the
electrolyte and lithium, respectively. After the activation process, joule
heating and entropic cooling should be described. The following equa­
tions were used:
qjoule heating = i2 Rtot (6)
Unit
∂V
qentropic cooling = i[− T∙ ] (7)
∂T
m
kg where i is the current per area, T is the temperature, and ∂V/∂T is the
A/cm2 variation of the open circuit cell potential with respect to temperature.
constant Both equations are functions of the current density. In this study, the
A∙s current density value was assumed to be 0.45 A/cm2 for joule heating in
s order to reduce the optimization parameter because we consider only
◦
C 0.1–0.8 A/cm2 for the design, as we discussed in the previous section. In
◦
C a thermal battery, the heat generated by the heat source is much more
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T.-R. Park et al. Energy Conversion and Management 236 (2021) 114033

dominant than that generated by joule heating or entropic cooling, so Table 4

the heat due to the difference in current density 0.35 A/cm2 is negli­ Input ranges and output of multi-physics model for data generation.
gible. According to Lee et al. [7] the difference in current density of Parameter Value Unit
0.5 A/cm2 only caused a difference of approximately 1 ◦ C in the internal Input
temperature during the operating time of 600 s. On the other hand, Rtot Diameter (D) 50, 70, 90, 110 mm
was determined to be 56 mΩ and ∂V/∂T to be 4.5 × 10− 4 V/K. Heat pellet thickness (HT) 0.5, 0.75, 1, 1.25, 1.5 mm
In the simulation, the initial temperature of the battery and tem­ Anode thickness (AT) 0.3, 0.6, 0.9, 1.2 mm
Electrolyte thickness (ET) 0.4, 0.5, 0.6 mm
perature of the outside atmosphere were assumed to be 20 ◦ C. Heat loss BTU thickness (BT) 0, 3.175, 6.35 mm
due to free convection was applied to the boundary with a heat transfer Mica thickness (MT) 2, 5, 10 mm
coefficient of 10 W/m2 K. The time step size was set densely at the Additional heat pellet (AHT) HT, 2HT, 3HT mm
beginning of the simulation because a drastic temperature change Output
occurred when the battery was activated and was set sparsely after the Max temperature of 1st cell cathode (T1 ) Max(Tpoint1 , Tpoint2 , ◦
C
activation. In addition, the time duration of the simulation was set as Tpoint3 )
1000 s. The detailed thermo-physical properties for the simulation are Max temperature of 13th cell cathode (T2 ) Max(Tpoint4 , Tpoint5 , ◦
C
listed in Table 3. Tpoint6 )
Max temperature of 13th cell electrolyte (T3 ) Max(Tpoint7 , Tpoint8 , ◦
C
Tpoint9 )
3.3. Data generation
Temperature of electrolyte at 100 s, 500 s, 1000 s Avg(Tpoint7 , Tpoint8 , ◦
C
(T4 , T5 , T6 ) Tpoint9 )
To construct the simulation database for DNN model training, all
Activation time tTpoint7 =443 s
combinations of the seven input parameters in Table 4, a total of
4*5*4*3*3*3*3 = 6480 inputs, were simulated through the model. On
average, it took 10 min to calculate each simulation. During the simu­ simulation presented in Table 4 were adopted for the input and output
lation, nine points, as shown in Fig. 6, were measured as probe points to data to train the DNN models. In Model i (i = 1,2,3…6), a total of 6480
obtain temperature data over time. To obtain the output data, data parameter combinations in Table 4 were given as input data and Ti in
processing was performed with measured data, as shown in Table 4. The Table 4 obtained by the simulation were given as output data. For
highest temperatures of the 1st cell cathode and the 13th cell cathode example, Model 1 trains T1 as output data and Model 2 trains T2 as
were obtained as the output data by calculating the maximum values of output data. For Model 7, because the activation time — the output for
point 1,2, and 3 and point 4,5, and 6. Since the 1st cell has an insulator Model 7 — can only be calculated when T3 is higher than 443 ◦ C, only
directly above it and an additional heat pellet above it, heat concen­ data with T3 is higher than 443 ◦ C were adopted as input. A total of 6480
tration may occur; therefore, the cathode of the 1st cell was also data entries for Models 1–6 and 2700 for Model 7 were split into two
considered. Next, the electrolyte temperature at 100 s, 500 s, and 1000 s sets, with a ratio of 0.8:0.2 (training set:test set). A description of the
was determined as the output value and was measured by calculating the training protocol for DNN training is given below. The batch size was set
average value of point 7,8, and 9. Finally, the activation time was to 10. Models 1–3 were set to 1500, and Models 4–7 were set to an epoch
calculated when the temperature at point 7 attained 443 ◦ C, the melting size of 1000. The mean square error function was used as the loss
point of the electrolyte. To obtain a more accurate activation time, a function and ADAM was used as the optimizer. Relu was used as the
linear interpolation method was adopted between the time steps of the activation function and the learning rate was set to 0.01. The min–max
simulation due to the drastic temperature changes in the activation data processing method was adopted because the magnitude of each
process. input is not within the same range. The DNN framework was imple­
mented through Tensorflow1.5x in Python programming languages.
3.4. Development of DNN model After the DNN model was trained, the root mean squared error and
maximum percentage error for the output data were measured for
A DNN is an artificial neural network comprising multiple hidden validation. The root mean squared error and maximum error are defined
layers between the input and output layers. A DNN can statistically as follows:
model a complex non-linear system. In this work, a conventional back­ √̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
propagation DNN method was used. 1∑ n
(8)
2
Root mean square error = (Ti − T ’i )
Fig. 7 presents a schematic of the DNN models used in our training. A n i=1
total of seven models are used; each model comprises seven inputs, three
{⃒ ⃒}
hidden layers, and one output. Each hidden layer consists of 10,14, and Maximum error = max ⃒Ti − Ti’ ⃒ (9)
10 neurons, respectively. Data generated through the multi-physics
where n is the number of data, Ti is the output data using the DNN
Table 3 model, and Ti’ is the output using the multi-physics model. The predic­
Thermo-physical properties of the Li-Fe battery used in COMSOL modeling tion errors in the training and test sets are listed in Table 5. From the
[4,7]. error values of the training and test sets, the training result is considered
Density Specific heat Thermal conductivity sufficient. The maximum error for temperature prediction is approxi­
(kgm− 3 ) (Jkg− 1 K− 1 ) (Wm− 1 K− 1 ) mately 1.5 ◦ C. A temperature difference error of less than 1.5 ◦ C is
considered to be sufficiently acceptable when designing the thermal
Heat pellet 3299.28 745.38 21.86
Cathode 2783 992.3 1.02 battery. Considering that the temperature of the thermal battery is
Electrolyte 2210.47 870 1.02 approximately 500 ◦ C, 1.5 ◦ C is less than 1% error. Similarly, the acti­
Anode 2827.16 849.1 64.355 vation time error is also considered to be within the allowable range of
Current collector 7874 450 43.3 0.1 s. Through validation, it was confirmed that a sufficient number of
Mica 2263.54 850 0.4
BF 205.776 979.7 0.0475
multi-physics simulation data were trained to build an accurate DNN
BTU 256 979.7 0.04 model. Therefore, the DNN model can not only reduce the expensive cost
Stainless steel 8030 690.8 21.646 and time but also provide accurate solutions for predicting the tem­
perature of the thermal battery.

6
T.-R. Park et al. Energy Conversion and Management 236 (2021) 114033

Fig. 6. Probe points of simulation to obtain output data.

design space, was adopted as the optimization algorithm [14]. If the

challenge of a lengthy calculation time is solved, this algorithm can
obtain the accurate global optimum value for a non-linear optimization
problem. The specific ranges and the number of optimization parame­
ters used in the algorithm are summarized in Table 6. A total of 100
million optimization parameters in the design space are searched for
optimization. In the optimization process, as exhibited in Fig. 4, the
temperature prediction results of the optimization parameters were
obtained from the DNN model. Next, if each constraint in the optimi­
zation problem illustrated in Table 2 is satisfied, the weight calculation
proceeds. The optimal value is subsequently updated by comparing the
calculated weight with the previously calculated weight. This process is
repeated for all parameters in the design space. Optimization was con­
ducted according to the performance requirements of Case 1 and Case 2.

3.6. Optimization results and analysis of time-efficiency

Table 7 lists the optimized parameters, weight, and temperature

prediction results as the optimization results for Case 1 and Case 2. A
corresponding multi-physics simulation is conducted to verify the result
and its temperature prediction results are also compared. It is found that
Fig. 7. Schematic of DNN models used in the training. the predicted values from the DNN model and COMSOL model are very
similar. Verification results shows maximum error of 4 ◦ C for tempera­
ture distributions and 0.05 s for activation time, respectively.
Table 5 Using this methodology, the time required to optimize the design of
Prediction error in the training set and test set. the thermal battery was significantly reduced. Using the COMSOL model
Training set Test set takes approximately 10 min to calculate one solution but using the DNN
model takes approximately 0.01 s on an Intel i7 2.4 GHz computer with
Root mean Root mean Maximum
square square Error 8.0 RAM. Since various factors affect the time-efficiency of this meth­
odology, an in-depth analysis is required to determine the time-
Model 1 (T1 ) 0.13 0.9 1.24
efficiency of this methodology. Time-efficiency should be considered
Model 2 (T2 ) 0.91 1.10 1.54
from the following four points of view:
Model 3 (T3 ) 0.42 0.98 1.32
Models 4–6 (T4 ,T5 ,T6 ) 0.21,0.12,0.19 0.09,0.11,0.2 0.95,0.67,1.02
(1) Number of multi-physics simulations required to train DNN
Model 7 (Activation 0.01 0.04 0.08
time)
model (N1 )

In our study, 6480 data obtained through a multi-physics simulation

3.5. Optimization procedure were used to train the DNN model. It took a single computer approxi­
mately 42 days (6480 × 10) to simulate 6480 data (considered a long
The optimization problem defined in Table 2 is solved in this section. time). If the number of data points can be reduced, the time-efficiency of
The brute force algorithm, which investigates all parameters in the this methodology will be better. However, because reducing the number

7
T.-R. Park et al. Energy Conversion and Management 236 (2021) 114033

Table 6
Optimization parameters in design space.
D[mm] HT[mm] AT[mm] ET[mm] MT[mm] BT[mm] AHT[mm]

Range 30–130 0.5–1.8 0.2–1.5 0.4–0.65 0–10 0–6.35 0.5–5.5

Number of parameters 50 20 20 5 10 10 10

Table 7
Optimal value and corresponding results COMSOL for each case.
Optimized parameter (D,HT,AT,ET,MT,BT,AHT)[mm] Temperature(T1 , T2 , ...T6 )[◦ C] Activation time[s] Weight[g]

DNN COMSOL DNN COMSOL

Case1 (70, 1.43, 0.66, 0.4, 2, 4.23, 2.9) (615,509,540, (614,509,538, 0.787 0.792 1247.5
519,501,466) 520,499,466
Case2 (80, 1.4, 0.57, 0.4, 2, 4.23, 1.3) (650,547,557, (649,546,553 0.876 0.873 1636.9
540,528,501) 541,528,499]

of data can reduce the accuracy of the DNN model, determining this
number is a trade-off problem.

(2) The number of parameters in the optimization problem design

space (N2 )

The number of parameters in the design space has a significant

impact on the time-efficiency. The range and number of parameters in
Table 6 need to be carefully designed. This number is decided by the
designer according to the application needs. The larger the design space
required, the more efficient it is to use the DNN model. However, if the
size of the design space is smaller than the number of data required to
create a DNN model of 6480, it will be more beneficial to use multi-
physics simulation.

(3) Multi-physics simulation time (t)

In our study, an average of 10 min was required to obtain a solution

of one 25 cell class battery from Comsol. However, this time may vary
depending on the simulation conditions (e.g., analysis area, solver,
mesh, time step, etc.). It takes more than 50 min to simulate the 80 cell
Fig. 8. Time-efficiency analysis according to 3 factors (N1 ,N2 , and t).
class battery instead of the 25 cell class battery in our study. A multi-
physics model should be created with a good balance between accu­
racy and computation time. 4. Conclusion

(4) Hardware calculation speed
In our study, both COMSOL and DNN model calculations were per­
formed on relatively low-end hardware. Hardware performance also
affects the time-efficiency.
If the calculation time of the DNN model is fixed to 0.01 s and the
time-efficiency is defined as follows, the effect of N1 , N2 , and t on the
time-efficiency can be analyzed.
tDNN N1 t + 0.01N2
Time efficiency = = (10)
tMP N2 t
tMP is the total time when using a multi-physics model and tDNN is the
total time when using the DNN model. From Fig. 8, it can be seen that
using the DNN model can significantly improve the time compared to
MP simulation if N2 exceeds 100,000. In addition, it appears that N1 and
N2 have a very large effect on time-efficiency and t has little effect. If the
number of parameters in the design space is exceeded to some extent, it
is virtually impossible calculation time if MP is used. However, because
thermal batteries have complex systems and require more sophisticated
optimization, the number of design spaces is inevitably large, indicating
that our methodology is essential in designing thermal batteries.
In this study, a novel methodology is presented for optimizing the
heat and weight of a thermal battery. A case study based on detailed
performance requirements is presented to demonstrate the methodol­
ogy. In the methodology, the design method for the capacity, power, and
heat of the thermal battery is modeled by theoretical and experimental
methods, through which the optimization problem is formulated. The
brute force algorithm is used as an optimization algorithm to solve the
optimization problem. By modeling the design method, the battery can
be systematically designed according to the performance requirements,
and the optimal design problem can be converted into a mathematical
optimization problem. A DNN model trained with multi-physics simu­
lation data was used as the temperature prediction model. Using the
DNN model reduced the computational time required for optimization
by more than 10,000 times compared to that required using the multi-
physics simulation, and the prediction performance of temperature
distributions and activation time show that the maximum error in the
test set is less than 1.54 ◦ C and 0.08 s, respectively. Moreover, the
verification results for the optimized structure show a maximum error of
4 ◦ C for temperature distributions and 0.05 s for the activation time. It
can be concluded that the DNN model shows sufficient accuracy
compared to the multi-physics model, and its use drastically reduced the
optimization time, which was difficult to achieve by other means.

8
T.-R. Park et al.
Therefore, this methodology is expected to contribute to the develop­
ment of lightweight and high-performance thermal batteries by allowing
their systematic and optimal design, as opposed to the conventional
trial-and-error design method.
CRediT authorship contribution statement
Tae-Ryong Park: Conceptualization, Methodology, Software,
Investigation, Writing - original draft, Writing - review & editing.
Hyunseong Park: Software. Kiyoul Kim: Methodology. Chae-Nam Im:
Investigation. Jang-Hyeon Cho: Supervision.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgment
This work was supported by the Agency for Defense Development in
South Korea (ADD).
References
[1] Guidotti RA, Masset P. Thermally activated (“thermal”) battery technology: Part I:
an overview. J Power Sources 2006;161(2):1443–9.
[2] Kuper WE. A brief history of thermal batteries. In Proceedings of the 36th Power
Sources Conference, Cherry Hill, NJ, USA; 1994.
Energy Conversion and Management 236 (2021) 114033
[3] Im C-N, Hun Choi C, Yu H-R, Ahn T-Y, Yoon H-K, Seong Yeo J, et al. Investigation
of Li anode/FeS2 cathode electrochemical properties for optimizing high-power
thermal batteries. Batteries Supercaps 2021;4(2):304–15.
[4] Cho J-H, et al. Thermal stability characteristics of high-power, large-capacity,
reserve thermal batteries with pure Li and Li(Si) anodes. Electrochim Acta 2020;
353:136612.
[5] Haimovich N, Dekel DR, Brandon S. A simulator for system-level analysis of heat
transfer and phase change in thermal batteries. J Electrochem Soc 2009;156(6):
A442. https://doi.org/10.1149/1.3106103.
[6] Haimovich N, Dekel DR, Brandon S. A simulator for system-level analysis of heat
transfer and phase-change in thermal batteries. J Electrochem Soc 2015;162(3):
A350–62.
[7] Jeong MG, Cho J-H, Lee BJ. Heat transfer analysis of a high-power and large-
capacity thermal battery and investigation of effective thermal model. J Power
Sources 2019;424:35–41.
[8] Li H-W, et al. Performance prediction and power density maximization of a proton
exchange membrane fuel cell based on deep belief network. J Power Sources 2020;
461:228154.
[9] Wang B, et al. AI-based optimization of PEM fuel cell catalyst layers for maximum
power density via data-driven surrogate modeling. Energy Convers Manage 2020;
205:112460.
[10] Xu H, et al. Towards online optimisation of solid oxide fuel cell performance:
combining deep learning with multi-physics simulation. Energy and AI 2020;1:
100003.
[11] Choi Y-S, Yu H-R, Cheong H-W. Electrochemical properties of a lithium-
impregnated metal foam anode for thermal batteries. J Power Sources 2015;276:
102–4.
[12] Kang S-H, Chae SH, Cheong H-W, Kim K-H, Han YS, Lee S-M, et al. Thermal
batteries with ceramic felt separators – Part 2: Ionic conductivity, electrochemical
and mechanical properties. Ceram Int 2017;43(5):4023–8.
[13] Masset PJ. Thermal stability of FeS2 cathode material in “thermal” batteries: effect
of dissolved oxides in molten salt electrolytes. Zeitschrift für Naturforschung A
2008;63(9):596–602.
[14] Jackson D, et al. Machine learning enabled fast multi-objective optimization for
electrified aviation power system design. 2020 IEEE Energy Conversion Congress
and Exposition (ECCE). 2020.