Applied Thermal Engineering 236 (2024) 121752

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Applied Thermal Engineering

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Research Paper

An inverse methodology to estimate the thermal properties and heat

generation of a Li-ion battery
Suraj Kumar a,b ,1 ,∗, Rajesh Akula b , C. Balaji b
a Heat Transfer and RAC Laboratory, Department of Mechanical Engineering, Indian Institute of Technology Delhi, New Delhi 110016, India
b
Heat Transfer and Thermal Power Laboratory, Department of Mechanical Engineering, Indian Institute of Technology Madras, Chennai 600036, India

ARTICLE INFO ABSTRACT

Keywords: Accurate estimation of temperature-dependent orthotropic thermal properties and volumetric heat generation
Artificial neural network of a Li-ion battery is crucial for thermal modeling, thermal safety, and the design of thermal management
Bayesian method systems for electric vehicles. Though various studies are available on estimating thermophysical properties
Li-ion battery
and heat generation, simple and easily applicable methods are rare. Moreover, these studies failed to report
MH-MCMC
temperature sensitivity and standard deviation of the estimates. In this study, the temperature-dependent
Orthotropic thermal properties
Volumetric heat generation
orthotropic thermal conductivities (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 ), specific heat (𝑐𝑝 ), and volumetric heat generation (𝑞𝑣 ) of
Panasonic NCR18650BD cylindrical battery are estimated using an inverse approach (Metropolis Hastings-
Markov Chain Monte Carlo algorithm based Bayesian method) with the help of experimentally obtained surface
temperatures measured at convenient locations on the battery. From the estimation, the average values of
𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 and 𝑐𝑣 are observed to be 3.18 ± 0.19, 20.34 ± 1.26, 19.89 ± 1.29 (W/mK), and 3180 ± 202 (J/kgK),
respectively. The average heat generation rates from the same battery obtained using the same methodology are
0.1 ± 0.005, 0.34 ± 0.012, and 1.51 ± 0.026 W for 0.5, 1, and 2C discharge rates, respectively. The estimated
thermophysical properties and heat generation rates are in good agreement with the results obtained from
both in-house experiments and literature. In addition to the estimation of thermophysical properties and heat
generation, the proposed methodology opens vistas to predict the strength and location of hotspots in the
battery domain, which helps in designing appropriate and effective thermal management systems for battery
packs.

1. Introduction optimal temperature range of LIBs is between 20 and 40 ◦ C [6,7].

Lithium-Ion Batteries (LIBs) have been widely used as energy stor-
age and conversion systems in a wide range of applications, including
Electric Vehicles (EVs), Hybrid Electric Vehicles (HEVs), consumer
electronics such as cell phones and laptops, and aerospace systems [1].
LIBs enable high energy storage densities and faster conversion rates in
energy storage and conversion applications compared to its competing
technologies. In automobile applications, for example, EVs and HEVs,
LIBs enhance fuel efficiency, reduce emission of greenhouse gases,
and unfasten fossil fuels depletion rate [2–4]. At present, LIBs are
the leading power source technologies in EVs and HEVs owing to
their high energy density, high power, low rate of self-discharge, high
nominal voltage, and long cycle life compared to other secondary
battery technologies [5].
However, the advantages of LIBs and their safety are highly sen-
sitive to their operating temperatures. Several studies show that the
Despite starting the battery operations (discharging) at room temper-
ature, its operating temperature rises due to internal heat generation
throughout the volume caused by ionic resistance and exothermic
reactions. The temperatures beyond the mentioned limits adversely
affect their performance and stability. For example, operating LIBs
at higher temperatures enhance the risk of fire and explosion [8],
and at lower temperatures and high discharge rates deteriorates its
capacity due to lithium plating [9]. The limits on operating temper-
atures restrain bulk deployment of LIBs in EVs. In addition to the
absolute temperatures, large thermal gradients in a pack affect battery
performance. The maximum allowable thermal gradient in any battery
pack is 5 ◦ C [10]. With these notes on the thermal limitations of
LIBs, it is of great importance to design a Battery Thermal Man-
agement System (BTMS) either by using active, or passive, or both
cooling methodologies [11–13] to keep the operating temperatures
of LIBs within the safety limits during all events of their operation.

∗ Corresponding author.
E-mail address: suraj@iitd.ac.in (S. Kumar).
1
Post-Doctoral Fellow.

https://doi.org/10.1016/j.applthermaleng.2023.121752
Received 12 June 2023; Received in revised form 6 September 2023; Accepted 4 October 2023
Available online 7 October 2023
1359-4311/© 2023 Elsevier Ltd. All rights reserved.
S. Kumar et al. Applied Thermal Engineering 236 (2024) 121752

Nomenclature BTMS Battery thermal management system

EVs Electric vehicles
𝐴 Acceptance ratio
HGR Heat generation rate
𝐶 Discharge rate
LIB Lithium ion battery
𝑐𝑝 Specific heat capacity of the active material,
LFP Lithium Ferro Phosphate
J∕KgK
LTO Lithium Titanium Oxide
𝑐𝑝,𝑚 Specific heat capacity of the mandrel,
J∕KgK MH Metropolis Hastings
𝑐𝑝,𝑡𝑏 Specific heat capacity of the tabs, J∕KgK MCMC Markov Chain Monte Carlo
𝑐𝑝,𝑜𝑐 Specific heat capacity of the outer can, MAP Maximum a posteriori
J∕KgK MSMD Multi-Scale Multi-Domain
𝑐𝑝,𝑠𝑠 Specific heat capacity of the stainless steel, NMC Nickel Manganese Cobalt
J∕KgK PPDF Posterior probability density function
𝐸 Estimates vector SD Standard deviation
𝑓 Function TIS Thermal impedance spectroscopy
ℎ Heat transfer coefficient, W∕m2 K
𝑘𝑟 Radial thermal conductivity of the active
material, W∕mK
The traditional approach to design any BTMS is based on the surface
𝑘𝜃 Angular thermal conductivity of the active
temperature distribution of the battery for different discharge rates.
material, W∕mK
However, this method does not consider the thermal inertia of the
𝑘𝑧 Axial thermal conductivity of the active
battery, which decides the temperature distribution within its volume.
material, W∕mK
As a result, the BTMS design based on the surface temperature alone
𝑘𝑚 Thermal conductivity of the mandrel,
may not provide an acceptable quality of thermal protection [14].
W∕mK
Given this, the thermal modeling of LIBs, which elucidates the un-
𝑘𝑡𝑏 Thermal conductivity of the tabs, W∕mK derlying mechanism for heat generation and temperature evolution
𝑘𝑜𝑐 Thermal conductivity of the outer can, in the battery domain, is essential for designing an effective BTMS.
W∕mK Several numerical approaches have been developed in the literature
𝑘𝑠𝑠 Thermal conductivity of the stainless steel, for the thermal modeling of batteries. The electrochemical and lumped
W∕mK thermal models are two important and likely used thermal models [15].
𝑛 Number of locations of temperature mea- Electrochemical and thermal models can accurately estimate the heat
surements generation and temperature distribution of batteries; however, they are
𝑃 Probability complex and time-consuming. Lumped thermal models are simple and
𝑞𝑉 Volumetric heat generation, W∕m3 cost-effective in computation time but with relatively low accuracy
𝑅 Correlation coefficient compared to electrochemical thermal models. The accuracy of the
𝑅′ Radius of the active material, mm lumped capacity models can be improved by the correct estimation
of the thermophysical properties of the battery material and heat
𝑅0 Radius of the battery, mm
generation under different operating conditions [16].
𝑟 Radial direction
The LIBs are composed of three major components, namely, elec-
𝑡 Time, s trode layers, porous separator, and electrolyte, and they are rolled
𝑇 Temperature, ◦ C or folded into the required shape. As batteries are composed of het-
𝑣 Random number erogeneous materials, their overall thermal conductivity and specific
𝑌 Unsteady measured temperature data, ◦ C heat are often not well known in advance and not provided by LIB
𝑧 Axial direction manufacturers. The morphology and chemical composition of electrode
and separator layers and their packing within the battery shell influence
Greek letters
thermal conductivity and specific heat. As a result, these properties
𝜇𝑝 Mean of the prior change with changes in battery chemistries (e.g., LFP, NMC, LTO) and
𝜎𝑝 Standard deviation of the prior shapes (cylindrical, pouch, prismatic). In addition, these properties are
𝜃 Angular direction often strong functions of the electrochemical state of the battery and
temperature, and they vary significantly in space within the battery
𝜌 Density of the active material, kg∕m3
volume [15].
𝜌𝑚 Density of the mandrel, kg∕m3
With the necessity of knowing the values of anisotropic thermal
𝜌𝑡𝑏 Density of the tabs, kg∕m3
conductivity and specific heat, and their criticality in measuring or
𝜌𝑜𝑐 Density of the outer can, kg∕m3 estimating, researchers worldwide have developed several methods in
𝜌𝑠𝑠 Density of the stainless steel, kg∕m3 recent years. Shah et al. [17] provided an overview of techniques for
Subscripts measuring the thermal characteristics of a Li-ion cell. In Maleki et al.
[18], Nieto et al. [19], and Spinner et al. [20], the calorimeter method
sim Simulated was used to measure the heat capacity of a Li-ion battery. However,
meas Measured the complex methodology and requirement of an expensive calorimeter
𝑉 Volume make this method less preferable. A method of thermocouple insertion
in the battery volume to measure thermal conductivity and specific
Abbreviation heat capacity was used in the study by Forgez et al. [21]. Despite
ANN Artificial neural network getting accurate results with this method, thermocouple insertion in
the battery severely affects its functionality. The specific heat capacity
and thermal conductivity of a Li-ion battery were suggested to be

2
S. Kumar et al.
Fig. 1. Schematic view of the complete experimental setup for estimating the temperature-dependent orthotropic thermal properties of the active material of the Li-ion battery
used in the present study.
measured using the thermal impedance spectroscopy (TIS) technique
in Fleckenstein et al. [22]. This method uses the thermal impedance
curves, which depict the cell temperature response to the excitation
signal, to estimate the thermophysical properties. The major drawback
of the TIS method is that the frequency of battery thermal response is
very low (typically in the scale of mHz), and as a result, it takes longer
times for estimation [23]. Using experimental temperature measure-
ments, Murashko et al. [14] analytically calculated the through-plane
thermal conductivity and average specific heat capacity of 18650 and
26650 cylindrical Li-ion batteries. In addition to the above methods, the
anisotropic thermal conductivity and specific heat of the battery were
also calculated by Zhang et al. [23] using optimization technique based
on least-square regression and by Ruan et al. [16] using the reduced
wide-temperature-range electro-thermal coupled model, and by other
researchers in their studies [15,24].
In addtion to the studies on identifying thermophysical properties,
researchers have also putforth different methodologies to estimate heat
generation from Li-ion batteries. The Bernardi technique [25] is the
most well-known theoretical approach for calculating the heat genera-
tion rate (HGR). The HGR in the Bernardi method is the result of adding
reversible and irreversible heat. The irreversible heat caused by ohmic
losses and the reversible heat due to entropy changes were directly
determined by heat flow measurements using a novel experimental
technique in Christen et al. [26]. The studies conducted in [27–30],
and [31], an electrochemical model named Multi-Scale Multi-Domain
(MSMD) approach is built to calculate the heat generation from battery
for various discharge rates. However, these theoretical and electro-
chemical methods are not appropriate for actual applications due to the
intricacies involved in calculating the parameters required to run the
model. In other studies, Wang et al. [32] introduced an empirical heat
source model, Cao et al. [33] and Sheng et al. [34] used calorimetric
approach, Esmaeili and Jannesari [35] implemented artificial neural
networks (ANNs), and Parhizi et al. [36] developed an analytical
heat transfer model to estimate or calculate heat generation from the
battery.
From the above literature, it is seen that many methods have been
implemented to measure the specific heat capacity, thermal conduc-
tivity, and volumetric heat generation of Li-ion batteries, which are
expensive and time-consuming. Moreover, the standard deviation of
estimation, sensitivity of thermophysical properties and heat generation
3
Applied Thermal Engineering 236 (2024) 121752
for various operating conditions, and strength and location of hotspots
in the battery have not been determined in the previous studies.
To fill the above-mentioned research gaps, the present study im-
plements an effective inverse technique called the Bayesian inference-
based Metropolis Hastings-Markov Chain Monte Carlo (MH-MCMC)
method [37–42]. This inverse methodology combines measurements,
modeling, probabilities, and sampling to estimate parameters in heat
transfer problems with an additional advantage of reporting uncer-
tainties in the parameters. In essence, the innovation in this study
lies in developing a methodology that uses experimental temperatures
measured at convenient locations to estimate temperature-dependent
orthotropic thermal properties, variation in volumetric heat generation,
and the occurrence of hot spots within a cylindrical Li-ion battery. An
added benefit of this approach is its efficiency in terms of computa-
tional time coupled with its independence from the need for detailed
electrochemical knowledge to predict heat generation. The identifi-
cation of these temperature hot spots holds significant implications
by providing valuable insights for the optimal design and effective
implementation of thermal management systems within battery packs.
2. Experimental methodology
In the present study, the experimental methodology is divided into
two parts: One is to estimate thermophysical properties and the other
is to estimate volumetric heat generation of Panasonic NCR18650BD
battery.
2.1. Experimental methodology for thermal characterization
Laminar natural conjugate convection experiments are conducted
on the active material of the Panasonic NCR18650BD Li-ion battery to
estimate the thermophysical properties. Fig. 1 shows a schematic view
of the complete experimental setup for estimating the temperature-
dependent orthotropic thermal properties of the active material of the
Li-ion battery. The setup consists of a cylindrical active material of the
battery, hot fluid circulator (Julabo), chamber, hot plate, copper plate,
stand, fixtures and fasteners, insulating material, T-type thermocouples,
data logger, and computer. An interior view of the chamber considered
in the experimental setup is explicitly shown in Fig. 2. The cylindrical
active material of the battery is placed on the top of the copper plate,
S. Kumar et al. Applied Thermal Engineering 236 (2024) 121752

Fig. 2. An image of the interior view of the chamber of the experimental setup used in the present study.

and both are clamped together on top of the hot aluminum plate using
fixtures and fasteners. The hot plate is placed inside the chamber and
fixed to a stand for support. This hot plate is integrated with cylindrical
copper tubes for the supply of hot fluid. Five T-type thermocouples
(uncertainty = ±0.25 ◦ C) are attached at different locations on the
surface of the active material, and one K-type thermocouple (uncer-
tainty = ±0.25 ◦ C) is used to measure the hot plate temperature (see
Fig. 3). The body of the active material is heated from its base by
supplying hot fluid in the hot plate. The data logger is connected to
thermocouples to read temperatures, and the temperature data is saved
in a computer. Low emittance tape is pasted over the active material to
eliminate the radiation heat transfer from its outer surface. As a result,
only conduction and natural convection are present inside and on the
outer surface of the active material of the battery, respectively.
The initial temperature of the system and the ambient temperature
are the same and equal to 26 ± 1 ◦ C. The temperature of the hot fluid
circulator is set at 38 ◦ C. The unsteady temperatures are measured on
the outer curved surface of the active material (Fig. 4(a)) and at the hot
plate (i.e., bottom surface of the active material) (Fig. 4(b)). The mea- Fig. 3. Locations of thermocouples for the temperature measurements.
sured temperatures (𝑇1 , 𝑇2 , 𝑇3 , 𝑇4 , 𝑇5 , 𝑇6 ) are used in the inverse model
to estimate the temperature-dependent orthotropic thermal properties
of the active material. From the in-house experiments, the temperatures battery is critical for effective thermal management. In view of this, an
measured using thermocouple 𝑇6 (hot plate temperature) are used as inverse heat transfer methodology is employed in the present study to
a boundary condition in the forward model. Full details of the use of estimate the volumetric heat generation in the Li-ion battery accurately.
forward model in the estimation of thermophysical properties of the For solving the inverse heat transfer problem, the experimental temper-
active material are reported in the ensuing sections. The heat transfer atures measured on the surface of the battery for various discharge rates
coefficient (h), to be also used as a boundary condition on the outer of 0.5, 1, and 2C are used. The thermocouple locations for measuring
curved surface of the active material in the forward model, is calculated temperatures on the surface of the battery are shown in Fig. 5(b).
using the average surface temperature measured from the temperature The unsteady temperatures measured at the given five locations are
data obtained by thermocouples (𝑇1 –𝑇5 ) and a correlation [43] for the shown in Figs. 6(a), (b), and (c) for discharge rates of 0.5, 1, and 2C,
Nusselt number. The calculated experimental heat transfer coefficient respectively. The ambient temperature of 22 ◦ C is maintained during
(h) is presented in Fig. 4(c), which is used as a boundary condition to these experiments.
solve the forward model of the active material. The heat transfer coefficient (ℎ𝐷 ) on the surface of the battery is
also calculated using the average temperatures obtained from thermo-
2.2. Experimental methodology for estimating volumetric heat generation couples 𝑇7 –𝑇11 and the Churchill-Chu correlation [43] of the Nusselt
number variation for natural convection. The variation of the calcu-
A cylindrical Li-ion battery of model, Panasonic NCR18650BD, is lated heat transfer coefficient with time is shown in Fig. 6(d). It is
considered and discharged at 0.5, 1, and 2C discharge rates using a used as a boundary condition in the forward model simulations to
battery charge–discharge cyclic tester (NEWARE, BTS-4000). Five T- obtain the simulated temperatures. It is to be noted that the forward
type thermocouples are attached on its outer surface to measure the model discussed in the previous section to estimate the thermophysical
temperature variation during these discharge rates (see Fig. 5). For properties of the active material is different from the present forward
more details on the experimental testing of the same Li-ion battery, model. In the previous forward model, only the base of the active
please refer to Ref. [44]. Heat generation is a byproduct of chemical material is heated with constant temperature boundary condition using
to electrical energy conversion. Estimation of heat generation in the a hot fluid circulator. Whereas, the forward model discussed in this

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S. Kumar et al. Applied Thermal Engineering 236 (2024) 121752

Fig. 4. (a) and (b) variations of the unsteady temperatures measured on the side (𝑇1 , 𝑇2 , 𝑇3 , 𝑇4 , 𝑇5 ) and bottom (𝑇6 ) surface of active material, respectively (c) variation of the heat
transfer coefficient on the surface of the active material.

Fig. 5. (a) An image of the experimental setup and (b) locations of the thermocouples for temperature measurements to estimate the volumetric heat generation in the battery.

section has a full Li-ion battery, which is discharged using a battery neural network to develop the surrogate model, which is implemented
charge–discharge cyclic tester. More details about both the forward in the inverse methodology to estimate the unknown parameters.
models are presented in the ensuing sections. The measured unsteady
temperatures are used in the inverse model to estimate the volumetric 3.1. Forward model for thermal characterization
heat generation variation in the battery.
Experiments performed to estimate the thermophysical properties Fig. 8 shows the three-dimensional geometry of the active material
and heat generation are conducted twice to ensure repeatability. From of the battery for the unsteady-state conduction problem. The gov-
the repeatability test, the highest temperature deviation at any location erning equation for the above is presented in Eq. (1). The boundary
and at any time instant is less than 0.5 ◦ C. As mentioned earlier, this conditions, shown in Table 1, are used to solve the following governing
study combines experimentation, modeling, and inverse methodology equation in COMSOL [45].
principles to estimate the temperature-dependent orthotropic thermal ( ) ( ) ( )
properties of the active material of the Li-ion battery and the volumetric 1 𝜕 𝜕𝑇 1 𝜕 𝜕𝑇 𝜕 𝜕𝑇 𝜕𝑇
𝑘 (𝑇 )𝑟 + 𝑘𝜃 (𝑇 ) + 𝑘 (𝑇 ) = 𝜌𝑐𝑝 (1)
heat generation for 0.5, 1 and 2C discharge rates. A detailed flow chart 𝑟 𝜕𝑟 𝑟 𝜕𝑟 𝑟2 𝜕𝜃 𝜕𝜃 𝜕𝑧 𝑧 𝜕𝑧 𝜕𝑡
of the entire study is shown in Fig. 7. Grid independence study is conducted on the computation domain
by comparing the variation of simulated temperature–time histories at
3. Forward model location (8.7, 0, 40 (all in mm)) of the forward model for extra coarse,
fine, and extra fine mesh types. The number of mesh elements gener-
The forward model includes the governing equations of the problem ated for extra coarse, fine, and extra fine mesh types are 2197, 56408,
along with the respective boundary conditions. The solution of the and 256385, respectively. The thermophysical properties 𝑘𝑟 = 2.5
forward model gives the simulated temperatures for various values W/mK, 𝑘𝜃 = 16 W/mK, 𝑘𝑧 = 16 W/mK, and 𝑐𝑝 = 2600 J/kgK are taken
of the unknown parameters. The simulated data corresponding to the for simulations. The temperature–time history for the computational
multiple values of the unknown parameters are used in an artificial meshes with fine and extra-fine are very close, which can be clearly

5
S. Kumar et al. Applied Thermal Engineering 236 (2024) 121752

Fig. 6. Variations of unsteady temperatures measured at five locations (𝑇7 , 𝑇8 , 𝑇9 , 𝑇10 , 𝑇11 ) on the side surface of a Li-ion battery for the discharge rates of (a) 0.5C (b) 1C, and (c)
2C and (d) an experimental heat transfer coefficient variation for discharge rates of 0.5, 1, and 2C.

Table 1 Table 2
Boundary conditions for solving the governing equations of the active material of the Ranges of the unknown parameters (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 ) at each time interval to obtain the
battery. simulated temperatures.
Boundary Condition Description Time (t), s Ranges of unknown parameters
at each time interval
Outer side surface of the battery −𝑘𝑟 (𝑇 ) 𝜕𝑇
𝜕𝑟
= ℎ(𝑇𝑠 − 𝑇∞ ), Natural convection
(𝑟 = 8.7, 0 ≤ 𝜃 ≤ 360, 0 ≤ 𝑧 ≤ 60) −𝑘𝜃 (𝑇 ) 𝑅𝜕𝑇 = ℎ(𝑇𝑠 − 𝑇∞ ), 0.5 ≤ 𝑘𝑟 ≤ 5 (W/mK),
′ 𝜕𝜃
2 ≤ 𝑘𝜃 ≤ 32 (W/mK),
−𝑘𝑧 (𝑇 ) 𝜕𝑇
𝜕𝑧
= ℎ(𝑇𝑠 − 𝑇∞ ) 100 ≤ 𝑡 ≤ 1 200 Time step (𝛥t) = 100
2 ≤ 𝑘𝑧 ≤ 32 (W/mK),
Bottom surface 𝑇 (𝑟, 𝜃, 𝑧, 𝑡) = 𝑇𝑏 (𝑡) Constant base 600 ≤ 𝑐𝑝 ≤ 5 000 (J/kgK)
(𝑧 = 0, 0 ≤ 𝜃 ≤ 360, 0 ≤ 𝑟 ≤ 8.7) temperature (samples = 201)
𝜕𝑇
Top surface 𝜕𝑧
=0 Insulated
(𝑧 = 60, 0 ≤ 𝜃 ≤ 360, 0 ≤ 𝑟 ≤ 8.7)
𝜕𝑇 𝜕𝑇 𝜕𝑇
Inner surface of the mandrel = 0, = 0, =0 Insulated
(𝑟 = 1, 0 ≤ 𝜃 ≤ 360, 0 ≤ 𝑟 ≤ 8.7)
𝜕𝑟 𝜕𝜃 𝜕𝑧
3.2. Forward model for estimating the volumetric heat generation

Fig. 10 shows the three-dimensional geometry of the cylindrical Li-

seen in Fig. 9. Based on the grid independence tests, 56408 fine-size ion battery considered in the forward model to estimate the volumetric
elements are employed for simulations. heat generation (𝑞𝑉 ). The governing equations of the active material,
Simulations are conducted on the active material of the battery mandrel, positive and negative tabs, and outer can of the Li-ion battery
using forward model for the ranges of unknown orthotropic thermal are presented in Eqs. (2), (3), (4), and (5), respectively. In the governing
properties (radial thermal conductivity (𝑘𝑟 ), angular thermal conductiv- equation (shown in Eq. (2)) of the active material, the orthotropic ther-
ity (𝑘𝜃 ), axial thermal conductivity (𝑘𝑧 ), specific heat capacity (𝑐𝑝 )). The mal properties (𝑘𝑟 (𝑇 ), 𝑘𝜃 (𝑇 ), 𝑘𝑧 (𝑇 ), 𝑐𝑝 (𝑇 )) are temperature dependent.
ranges of the unknown orthotropic thermal properties are found from The values of these properties are estimated first, hence, the volumetric
literature [30,46–50], and the same are shown in Table 2. For these heat generation (𝑞𝑉 ) is the only unknown term in Eq. (2). Table 3 shows
ranges, the simulated temperatures are obtained at each time interval of the boundary conditions used to solve the above governing equations
100 s. The total time intervals and samples of the unknown parameters in COMSOL [45].
(𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 ) are 12 and 201, respectively. The simulated temperatures Active material of the Li-ion battery:
obtained for the given ranges of the unknown parameters at each time ( ) ( ) ( )
1 𝜕 𝜕𝑇 1 𝜕 𝜕𝑇 𝜕 𝜕𝑇 𝜕𝑇
interval are used to develop the surrogate model. 𝑘𝑟 (𝑇 )𝑟 + 𝑘𝜃 (𝑇 ) + 𝑘𝑧 (𝑇 ) +𝑞𝑉 = 𝜌𝑐𝑝 (2)
𝑟 𝜕𝑟 𝜕𝑟 2
𝑟 𝜕𝜃 𝜕𝜃 𝜕𝑧 𝜕𝑧 𝜕𝑡

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S. Kumar et al. Applied Thermal Engineering 236 (2024) 121752

Fig. 7. A flow chart of the entire study.

Mandrel of the battery: fine, and extra fine mesh types when subject to a volumetric heat of
( ) 5000 W∕m3 . From the figure, it is clear that 259880 number of elements
1 𝜕 𝜕𝑇 𝜕𝑇
𝑘𝑚 𝑟 = 𝜌𝑚 𝑐𝑝,𝑚 (3) are sufficient for all the simulations conducted on this geometry.
𝑟 𝜕𝑟 𝜕𝑟 𝜕𝑡
Positive and negative tabs of the battery: The range of the unknown ‘𝑞𝑉 ’ at the given discharge rates of 0.5,
( ) 1, and 2C are taken from literature [53] and are shown in Table 4. The
1 𝜕 𝜕𝑇 𝜕𝑇 simulated temperatures are obtained at each time interval for this range
𝑘𝑡𝑏 𝑟 = 𝜌𝑡𝑏 𝑐𝑝,𝑡𝑏 (4)
𝑟 𝜕𝑟 𝜕𝑟 𝜕𝑡
of the unknown parameter 𝑞𝑉 at the given discharge rates. The total
Outer can of the battery: time intervals for 0.5, 1, and 2C are 16, 15, and 16, respectively (see
( ) Table 4). The total number of samples of ‘𝑞𝑉 ’ for each time interval and
1 𝜕 𝜕𝑇 𝜕𝑇
𝑘𝑜𝑐 𝑟 = 𝜌𝑜𝑐 𝑐𝑝,𝑜𝑐 (5)
𝑟 𝜕𝑟 𝜕𝑟 𝜕𝑡 each discharge rate is equal to 201. The simulated temperatures thus
Where 𝑘𝑚 = 𝑘𝑡𝑏 = 𝑘𝑜𝑐 = 𝑘𝑠𝑠 = 14.5 W∕mK [51], 𝑐𝑝,𝑚 = 𝑐𝑝,𝑡𝑏 = 𝑐𝑝,𝑜𝑐 = obtained for the given range of the unknown parameter (𝑞𝑉 ) at each
𝑐𝑝,𝑠𝑠 = 560 J∕kgK [52], and 𝜌𝑚 = 𝜌𝑡𝑏 = 𝜌𝑜𝑐 = 𝜌𝑠𝑠 = 8000 kg∕m3 . time interval are used to develop the surrogate model.
As this geometry is composed of active material, positive and neg-
ative tabs, and outer casing, the grid independence study is again con- 4. Surrogate model
ducted to identify the optimum number of mesh elements required for
simulation. Fig. 11 depicts the variation of the simulated temperature– Artificial Neural Networks (ANNs) are created to act as a surrogate
time histories of the battery at location (9, 0, 13 (all in mm)) for coarse, model to reduce computational time for solving the present inverse

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S. Kumar et al. Applied Thermal Engineering 236 (2024) 121752

Table 3
Boundary and domain conditions of the Li-ion battery for solving the governing equations.
Boundary Condition Description
Outer surface of the battery −𝑘𝑟 (𝑇 ) 𝜕𝑇
𝜕𝑟
= ℎ𝐷 (𝑇𝑠 − 𝑇∞ ), Natural convection
−𝑘𝜃 (𝑇 ) 𝑅𝜕𝑇𝜕𝜃 = ℎ𝐷 (𝑇𝑠 − 𝑇∞ ),
0

−𝑘𝑧 (𝑇 ) 𝜕𝑇
𝜕𝑧
= ℎ𝐷 (𝑇𝑠 − 𝑇∞ )
𝜕𝑇 𝜕𝑇 𝜕𝑇
Inner surface of the mandrel 𝜕𝑟
= 0, 𝜕𝜃
= 0, 𝜕𝑧
=0 Insulated
(𝑟 = 1, 0 ≤ 𝜃 ≤ 360, 0 ≤ 𝑟 ≤ 8.7)
Domain Condition Description
Active material of the battery 𝑞𝑉 = 𝑓 (𝑡) Volumetric heat generation

Fig. 8. Three-dimensional geometry of the active material of the battery for the Fig. 10. Three-dimensional geometry of the cylindrical Li-ion battery with volumetric
unsteady-state conduction problem. heat generation.

Fig. 9. Simulated temperature–time history at location (8.7, 0, 40 (all in mm)) of Fig. 11. Variation of simulated temperature–time history at location (9, 0, 13 (all
the forward model with assumed values parameters (𝑘𝑟 = 2.5 W/mK, 𝑘𝜃 = 16 W/mK, in mm)) of the forward model with assumed value parameter (𝑞𝑉 = 5000 W∕m3 ) for
𝑘𝑧 = 16 W/mK, and 𝑐𝑝 = 2600 J/kgK) for different mesh size elements. different mesh size elements.

connects the simulated temperatures (𝑇𝑠𝑖𝑚,1 , 𝑇𝑠𝑖𝑚,2 , 𝑇𝑠𝑖𝑚,3 , 𝑇𝑠𝑖𝑚,4 , 𝑇𝑠𝑖𝑚,5 ) as

problems. To estimate the temperature-dependent orthotropic thermal
properties (𝑘𝑟 (𝑇 ), 𝑘𝜃 (𝑇 ), 𝑘𝑧 (𝑇 ), 𝑐𝑝 (𝑇 )), 12 ANNs corresponding to 12
time intervals, are generated (shown in Table 2). At each time instant,
each neural network is trained with input data of 201 samples of
𝑘𝑟 (𝑇 ), 𝑘𝜃 (𝑇 ), 𝑘𝑧 (𝑇 ), 𝑐𝑝 (𝑇 ) and an output data of corresponding simulated
temperatures obtained from forward model. The trained neural network
a function of 𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 .
The surrogate model developed in the case of estimating volu-
metric heat generation, a total of 16, 15, and 16 ANNs are created
corresponding to total time intervals (shown in Table 4) for 0.5, 1,
and 2C discharge rates, respectively. Again, each ANN is used to
train the simulated temperatures (𝑇𝑠𝑖𝑚,7 , 𝑇𝑠𝑖𝑚,8 , 𝑇𝑠𝑖𝑚,9 , 𝑇𝑠𝑖𝑚,10 , 𝑇𝑠𝑖𝑚,11 ) as

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S. Kumar et al. Applied Thermal Engineering 236 (2024) 121752

Fig. 12. ANN architectures for estimating (a) the temperature-dependent orthotropic thermal properties (𝑘𝑟 (𝑇 ), 𝑘𝜃 (𝑇 ), 𝑘𝑧 (𝑇 ), 𝑐𝑝 (𝑇 )) of the active material and (b) the volumetric
heat generation (𝑞𝑉 ) with time in the battery.

Table 4 model) for the given parameters as

Range of the unknown parameter (𝑞𝑉 ) at each time interval to obtain the simulated
1 𝜒2
temperatures. −( 2 )
𝑃 (𝑌 ∕𝐸) = (√ )𝑛 𝑒 (7)
Discharge rate Time (t), s Ranges of unknown parameters 2𝜋𝜎 2
at each time interval
∑𝑛
0.5C 437 ≤ 𝑡 ≤ 6992 4000 ≤ 𝑞𝑉 ≤ 12000 (W/m3 ) (𝑌 −𝑌 )2
Time step (𝛥t) = 437 (samples = 201)
where 𝜒 2 = 𝑖=1 𝑚𝑒𝑎𝑠,𝑖𝜎2
𝑠𝑖𝑚,𝑖
, 𝜎 is the uncertainty between the mea-
surement and forward model, 𝑛 is a dimension of the temperature
1C 231 ≤ 𝑡 ≤ 3465 15000 ≤ 𝑞𝑉 ≤ 60000 (W/m3 )
Time step (𝛥t) = 231 (samples = 201) measurement (𝑌𝑚𝑒𝑎𝑠 ), and 𝑌𝑠𝑖𝑚 is the simulated temperatures obtained
from the surrogate model with given the parameter vector (𝐸). In the
2C 200 ≤ 𝑡 ≤ 1700 15000 ≤ 𝑞𝑉 ≤ 180000 (W/m3 )
Time step (𝛥t) = 100 (samples = 201) study, n (the number of locations where temperatures were measured)
is 5. The prior density function (P(𝐸)) is written as follows in the case of
a normal prior, where the mean and standard deviation of the estimates
are 𝜇𝑝 and 𝜎𝑝 , respectively.
a function of 𝑞𝑉 . Figs. 12(a) and (b) show the ANN architectures for
(𝐸−𝜇𝑝 )2
estimating the temperature-dependent orthotropic thermal properties 1 −
2𝜎𝑝2
(𝑘𝑟 (𝑇 ), 𝑘𝜃 (𝑇 ), 𝑘𝑧 (𝑇 ), 𝑐𝑝 (𝑇 )) of the active material and the volumetric 𝑃 (𝐸) = √ 𝑒 (8)
heat generation (𝑞𝑉 ) with time in the battery, respectively. Based on 2𝜋𝜎𝑝2
the neuron independence study, a total of 10 neurons in each hidden Using Eqs. (7) and (8) in Eq. (6), the PPDF was calculated as
layer are used to develop ANNs for both estimations. The Levenberg– [ ]
𝜒2 (𝐸−𝜇𝑝 )2
Marquardt optimization method is used to minimize the weights of each − +
2 2𝜎𝑝2
network. The output layer of the activation function uses the sigmoid 𝑒
𝑃 (𝐸∕𝑌 ) = [ ] (9)
logistic function while training the ANNs. For developing each ANN 𝜒2 (𝐸−𝜇𝑝 )2
− +
2 2𝜎𝑝2
in this study, 70%, 15%, and 15% of samples are used for training, ∫ 𝑒 d𝐸
validating, and testing, respectively. Here, 𝐸 denotes (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 ) or 𝑞𝑉 , as the case may be.
The Mean, Maximum a posteriori (MAP), and Standard deviation
5. Inverse model (SD) employed in the study are described in Kumar et al. [54].

Metropolis Hastings-Markov Chain Monte Carlo (MH-MCMC) algo-

The study employs the Bayesian inference method to retrieve the
rithm
temperature-dependent orthotropic thermal properties (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , and
𝑐𝑝 ) and volumetric heat generation (𝑞𝑉 ) separately from unsteady ex-
To dynamically produce the samples of the parameters (𝐸), the
periments carried out on (i) the active material of the Li-ion battery
MH-MCMC algorithm is used in Bayesian inference. In the MH-MCMC
arrangement connected to a hot fluid circulator and (ii) the Li-ion
algorithm, the new sample is produced using a normal density function
battery for various discharge rates (0.5, 1, and 2C), respectively. The
N(𝐸) around the mean of the old sample, a standard deviation of 5%
Bayesian inference method depends on the Bayes theorem, which states
of the mean, and a random number between 0 and 1. More details on
that the posterior probability density function of an estimate is directly
the MH-MCMC sampling algorithm have been presented in Kumar and
proportional to its likelihood function.
Balaji [52]. In this study, 10% samples are used for burn-in.
Given the unsteady measured data (Y), the posterior probability For both single-parameter estimation and multi-parameter estima-
density function (PPDF) of the estimates vector 𝐸 is defined by tion, the sampling procedure of the MH-MCMC algorithm is as follows:
𝑃 (𝑌 ∕𝐸) × 𝑃 (𝐸) 𝑃 (𝑌 ∕𝐸) × 𝑃 (𝐸)
𝑃 (𝐸∕𝑌 ) = = (6) 1. Initialize 𝐸 1 = (𝐸11 , 𝐸21 , . . . .., 𝐸𝑛1′ )
𝑃 (𝑌 ) ∫ 𝑃 (𝑌 ∕𝐸) × 𝑃 (𝐸) d𝐸
2. For i = 1, 2, . . . ., M or j = 1, 2, . . . ., 𝑛′
where P(𝐸/Y), P(Y/𝐸), and P(𝐸) are the PPDF, likelihood, and prior
density functions, respectively. The P(Y/𝐸) acquired by comparing the (a) Generate a random number, v∼R(0,1)
𝑖+1
experimental and simulated temperatures (obtained from the surrogate (b) Evaluate the next sample 𝐸𝑗∗ ∼ 𝑁(𝐸−𝑗 , 𝐸𝑗𝑖 , 𝜎 2 𝑖 )
𝐸𝑗

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S. Kumar et al.
Fig. 13. (a) Estimated orthotropic thermal conductivities (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 ) and (b) specific heat capacity (𝑐𝑝 ) variations with time (t) using ‘‘offline’’ Bayesian approach.
(c) If v < A(𝐸𝑗∗ , 𝐸𝑗𝑖 ), accept 𝐸𝑗𝑖+1 = 𝐸𝑗∗
(d) Else go to step 2 with 𝐸𝑗𝑖+1 = 𝐸𝑗𝑖
In the aforementioned procedure, 𝐸 stands for the parameter or group
of parameters that need to be retrieved, depending on the situation.
M and 𝑛′ are the number of samples and parameters, respectively, and
𝑖+1
𝐸−𝑗 = (𝐸1𝑖+1 , … , 𝐸𝑛𝑖 )𝑇 . ‘A’ denotes the acceptance ratio and has been
discussed in Kumar and Balaji [52].
6. Results and discussion
6.1. Estimation of the temperature-dependent orthotropic thermal properties
(𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 )
As mentioned earlier, accurate estimations of the temperature-
dependent orthotropic thermal properties (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 ) of the active
material and the volumetric heat generation in the active material of Li-
ion battery are important for the thermal management. In this section,
the estimation of temperature-dependent orthotropic thermal proper-
ties are presented first. Following this, the estimation of volumetric heat
generation with time in a Li-ion battery is reported for 0.5, 1, and 2C
discharge rates of Panasonic NCR18650BD battery.
The orthotropic thermal properties (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 ) of the active
material are estimated in terms of the mean and standard deviation
(SD) at each time interval using unsteady surface temperatures ob-
tained from the in-house experiments. These estimations are performed
using two inverse methods, namely (i) ‘‘offline’’ and (ii) ‘‘online’’
Bayesian approaches. In the ‘‘offline’’ inverse method, the samples of
the estimates (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 ) are generated by dividing the ranges of
estimates into a set of equal intervals. The ‘‘online’’ method means sam-
ples of the estimates are generated dynamically using the Metropolis
Hasting-Markov Chain Monte Carlo (MH-MCMC) sampling algorithm.
The samples of 2000 and 4000 are considered in ‘‘offline’’ and ‘‘online’’
Bayesian approaches, respectively, for the estimations. The variation of
the estimated orthotropic thermal conductivities 𝑘𝑟 , 𝑘𝜃 , and 𝑘𝑧 with
time are shown in Fig. 13(a) by employing the inverse method of
‘‘offline’’ Bayesian approach. Fig. 13(b) shows the estimated specific
heat capacity (𝑐𝑝 ) variation with time of the active material using the
same inverse method. The estimated parameters (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 ) using
‘‘offline’’ inverse approach are given in the ‘‘online’’ Bayesian approach
as priors knowledge for better estimations. The results of the estimated
𝑘𝑟 , 𝑘𝜃 , and 𝑘𝑧 variation with time using ‘‘online’’ Bayesian approach
with priors are presented in Fig. 14(a). From Fig. 14(a), it can be
observed that the predicted values for axial thermal conductivity (𝑘𝑧 )
and angular thermal conductivity (𝑘𝜃 ) are nearly the same. Fig. 14(b)
shows the results of the estimated 𝑐𝑝 variation with time using the same
10
Applied Thermal Engineering 236 (2024) 121752
Table 5
Validation of the estimated average values of the thermal properties (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 )
with literature.
Average values of thermal properties Present study Literature [30,46,55]
𝑘𝑟 (W/mK) 3.18 ± 0.19 3
𝑘𝜃 (W/mK) 20.34 ± 1.26 28.05
𝑘𝑧 (W/mK) 19.89 ± 1.29 28.05
𝑐𝑝 (J/kgK) 3180 ± 202 2400
‘‘online’’ inverse approach. The estimated variation of the standard
deviation with time for the orthotropic thermal conductivities (𝑘𝑟 , 𝑘𝜃 ,
and 𝑘𝑧 ) and the specific heat capacity (𝑐𝑝 ) of the active material using
‘‘offline’’ and ‘‘online’’ Bayesian methods are shown in Figs. 15(a) and
(b), respectively. From these figures, it is observed that the standard
deviation (SD) of the orthotropic thermal properties (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 )
estimated using ‘‘online’’ Bayesian method with priors is much lower
compared to ‘‘offline’’ Bayesian method. A higher reduction in the SD
of the estimates (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 ) using priors denotes the superiority of
the Bayesian method and the significance of the priors in the estima-
tion process. The average values of the estimated orthotropic thermal
properties (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 ) of a cylindrical Li-ion battery obtained from
the present study and literature [30,46,55] are shown in Table 5 for
comparison. In view of the close agreement of the estimated thermo-
physical properties against literature, the properties estimated in the
present study can be deemed to be accurate.
To obtain the temperature-dependent orthotropic thermal proper-
ties, the average measured temperature on the surface of the active
material is considered corresponding to each time interval. The Gaus-
sian curve fits of the estimated 𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , and 𝑐𝑝 with respect to the
average measured temperatures are shown in Figs. 16(a), (b), (c), and
(d), respectively. The temperature-dependent functions of the estimated
𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , and 𝑐𝑝 are obtained using Gaussian curve fit and are shown
in Table 6. The temperature-dependent functions of the estimated 𝑘𝑟 ,
𝑘𝜃 , 𝑘𝑧 , and 𝑐𝑝 are then given to the forward model of the active material
to obtain the simulated temperatures at locations shown in Fig. 3.
These simulated temperatures are compared against experimental tem-
peratures for validation, and are presented in a parity plot shown in
Fig. 17. From this figure, it is observed that the discrepancy between
the experimental and the simulated temperatures (obtained by giving
the estimated temperature-dependent orthotropic thermal properties
(𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 ) in the forward model) is observed to be less than
±1.5 ◦ C. The small deviation (±1.5 ◦ C) demonstrates that the procedure
employed in the present study is quite effective in accurate estimation
of the thermal properties of the active material.
S. Kumar et al. Applied Thermal Engineering 236 (2024) 121752

Fig. 14. (a) Estimated orthotropic thermal conductivities (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 ) and (b) specific heat capacity (𝑐𝑝 ) variations with time (t) using ‘‘online’’ Bayesian approach.

Fig. 15. Estimated standard deviation variation with time of (a) the orthotropic thermal conductivities (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 ) (b) specific heat capacity (𝑐𝑝 ) using offline and online Bayesian
approaches.

Fig. 16. Gaussian fits of the estimated (a) radial thermal conductivity (𝑘𝑟 ) (b) angular thermal conductivity (𝑘𝜃 ) (c) axial thermal conductivity (𝑘𝑧 ) and (d) specific heat capacity
(𝑐𝑝 ).

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S. Kumar et al. Applied Thermal Engineering 236 (2024) 121752

Table 6 Table 7
Estimated temperature-dependent orthotropic thermal properties (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 ) using Estimation of the volumetric heat generation (𝑞𝑉 ) in the Li-ion battery at each time
Gaussian curve fit. interval for a discharge rate of 0.5C using the ‘‘offline’’ Bayesian method.
Temperature-dependent orthotropic Gaussian curve fit Time (t), s Mean (W∕m3 ) MAP (W∕m3 ) SD (W∕m3 ) SD/Mean
thermal properties
437 6 557.0 4 104.0 1 833.0 0.279
( )2 ( )2
𝑇 −𝑏 𝑇 −𝑏
− 𝑐 1 − 𝑐 2 874 5 832.0 5 044.5 1 234.5 0.211
Radial thermal conductivity (𝑘𝑟 ) 𝑘𝑟 = 𝑎1 𝑒 1 + 𝑎2 𝑒 2
1 311 5 500.6 5 096.5 944.0 0.171
𝑎1 = 1.267, 𝑏1 = 306.7, 𝑐1 = 1.175, 𝑎2 = 3.465,
2 1 748 5 226.4 4 932.5 756.3 0.145
𝑏2 = 303.9, 𝑐2 = 5.41, 𝑅 = 0.8606
( ) ( )
2 185 7 285.0 7 285.6 800.2 0.109
𝑇 −𝑏3 2 𝑇 −𝑏4 2

Angular thermal conductivity (𝑘𝜃 )

−
𝑘𝜃 = 𝑎3 𝑒 𝑐3
−
+ 𝑎4 𝑒 𝑐4 2 622 7 240.3 7 237.6 699.4 0.096
𝑎3 = 17.62, 𝑏3 = 306.3, 𝑐3 = 2.077, 𝑎4 = 17.67, 3 059 6 297.3 6 297.1 623.5 0.099
𝑏4 = 302.4, 𝑐4 = 4.907, 𝑅2 = 0.9007 3 496 5 445.2 5 440.7 556.2 0.102
( ) ( )2 3 933 4 903.2 4 836.4 467.2 0.095
𝑇 −𝑏5 2 𝑇 −𝑏6
− − 4 370 4 673.5 4 556.3 398.0 0.085
Axial thermal conductivity (𝑘𝑧 ) 𝑘𝑧 = 𝑎5 𝑒 𝑐5 + 𝑎6 𝑒 𝑐6
𝑎5 = 15.95, 𝑏5 = 306.4, 𝑐5 = 2.167, 𝑎6 = 17.56, 4 807 4 463.7 4 228.1 317.5 0.071
𝑏6 = 302.3, 𝑐6 = 5.098, 𝑅2 = 0.8861 5 244 4 346.3 4 008.0 258.2 0.059
( ) ( )
𝑇 −𝑏8 2
5 681 4 384.3 4 132.1 271.7 0.061
𝑇 −𝑏7 2
− −
Specific heat capacity (𝑐𝑝 ) 𝑐𝑝 = 𝑎7 𝑒 𝑐7 + 𝑎8 𝑒 𝑐8 6 118 4 534.4 4 432.2 320.1 0.071
𝑎7 = 2760, 𝑏7 = 301.7, 𝑐7 = 5.272, 𝑎8 = 2678, 6 555 5 302.6 5 300.6 375.1 0.071
𝑏8 = 306.4, 𝑐8 = 2.379, 𝑅2 = 0.8991 6 992 7 271.4 7 269.6 376.3 0.052

Table 8
Estimation of the volumetric heat generation (𝑞𝑉 ) in the Li-ion battery at each time
interval for a discharge rate of 0.5C using ‘‘online’’ Bayesian method with priors.
Time (t), s Mean (W∕m3 ) MAP (W∕m3 ) SD (W∕m3 ) SD/Mean
437 6 330.7 6 462.6 474.6 0.074
874 5 632.0 5 750.5 409.2 0.072
1 311 5 363.6 5 435.6 349.4 0.065
1 748 5 081.2 5 162.6 334.6 0.065
2 185 7 225.8 7 285.4 388.0 0.053
2 622 7 201.2 7 238.8 363.6 0.050
3 059 6 269.9 6 298.6 309.8 0.049
3 496 5 400.4 5 443.3 276.3 0.051
3 933 4 833.1 4 872.9 256.1 0.053
4 370 4 583.0 4 616.4 246.6 0.054
4 807 4 303.5 4 349.6 232.9 0.054
5 244 4 140.4 4 171.0 221.7 0.053
5 681 4 205.4 4 250.4 224.1 0.053
6 118 4 453.4 4 474.9 213.7 0.047
6 555 5 287.8 5 302.7 217.2 0.041
6 992 7 248.1 7 269.7 235.5 0.032

from the surrogate model and the unsteady measured temperatures on

Fig. 17. Parity plot between the experimental and simulated temperatures (obtained
by giving the estimated temperature-dependent orthotropic thermal properties (𝑘𝑟 , 𝑘𝜃 ,
𝑘𝑧 , 𝑐𝑝 ) in the forward model).
6.2. Estimation of the volumetric heat generation (𝑞𝑉 ) and hot spot varia-
tion
There are several routes to obtain volumetric heat generation (𝑞𝑉 )
variation with time in a Lithium-ion battery. The usual way is to solve
the electrochemistry of the Li-ion battery. This can often be tedious.
Another alternative is to devise heat transfer experiments and measure
temperatures at convenient locations. Following this, one can apply
the inverse methodology to estimate 𝑞𝑉 . In the inverse methodology,
the electrochemistry of the battery is not required for estimating the
volumetric heat generation, 𝑞𝑉 . The simulated temperature distribu-
tions and hot spots are then obtained by running the forward model
of the battery with the estimated 𝑞𝑉 . These temperatures can be finally
used to assess the efficacy of the thermal management of the Li-ion
battery. Hence, in the present study, three-dimensional unsteady lami-
nar conjugate natural convection experiments are conducted on a Li-ion
battery using a battery charge–discharge cyclic tester (NEWARE, BTS-
4000) for 0.5, 1, and 2C discharge rates. The temperature-dependent
orthotropic thermal properties (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 ) estimated from the pre-
vious section are used in the unsteady forward model to obtain the
simulated temperatures for the given range of the unknown parameter
𝑞𝑉 . The trained simulated temperatures as a function of 𝑞𝑉 obtained
the surface of the battery for 0.5, 1, and 2C are then used in the inverse
methodology to estimate the volumetric heat generation. In the inverse
methodology, the ‘‘offline’’ and ‘‘online’’ Bayesian methods are used.
Using the ‘‘offline’’ Bayesian approach, the volumetric heat generation
(𝑞𝑉 ) estimated in terms of the mean, maximum a posteriori (MAP),
and SD at each time interval for 0.5, 1, and 2C as shown in Tables 7,
9, and 11, respectively. These estimations using the ‘‘offline’’ Bayesian
method are used as priors in the ‘‘online’’ Bayesian method. A total of
2000 and 5000 samples are used in the ‘‘offline’’ and ‘‘online’’ Bayesian
methods, respectively, to estimate the parameter. Tables 8, 10, and 12
show the results of the estimated 𝑞𝑉 in terms of the mean, MAP, and SD
at each interval for the discharge rates of 0.5, 1, and 2C, respectively
using ‘‘online’’ Bayesian method with priors. The estimated standard
deviations of the 𝑞𝑣 using the ‘‘online’’ Bayesian method with priors
are observed to be low compared to the ‘‘offline’’ Bayesian method. The
SD/Mean of the 𝑞𝑉 is also calculated at each time interval for 0.5, 1,
and 2C discharge rates and the same is presented in these tables. The
calculated SD/Mean of the 𝑞𝑉 using the ‘‘online’’ Bayesian method with
priors are observed to be lower than the SD/Mean of the 𝑞𝑉 obtained
using the ‘‘offline’’ method. This indicates a good effectiveness of the
retrieval methodology. Posterior probability density functions (PPDFs)
of the volumetric heat generation for 0.5C (time interval = 6992 s), 1C
(time interval = 3465 s), and 2C (time interval = 1700 s) are shown
in Figs. 18(a), (b), and (c), respectively. The MAP of the 𝑞𝑉 is obtained
corresponding to the maximum PPDF, which is shown in Figs. 18(a),
(b), and (c).

12
S. Kumar et al. Applied Thermal Engineering 236 (2024) 121752

Fig. 18. Posterior probability density function of the volumetric heat generation for (a) 0.5C (b) 1C, and (c) 2C for time intervals of 6992, 3465, and 1700 s, respectively.

Table 9
Estimation of the volumetric heat generation (𝑞𝑉 ) in the Li-ion battery at each time
interval for a discharge rate of 1C using ‘‘offline’’ Bayesian method.
Time (t), s Mean (W∕m3 ) MAP (W∕m3 ) SD (W∕m3 ) SD/Mean
231 22 163.5 19 884.9 4 621.0 0.208
462 25 971.7 25 962.9 3 157.4 0.121
693 25 725.4 25 715.3 2 176.5 0.084
924 23 680.2 23 689.3 1 660.9 0.070
1 155 21 919.9 21 955.9 1 356.2 0.062
1 386 20 422.8 20 425.2 1 161.1 0.056
1 617 19 529.5 19 524.7 1 028.7 0.052
1 848 18 618.6 18 646.8 916.8 0.049
2 079 18 250.8 18 259.5 831.3 0.045
2 310 18 048.1 18 060.9 774.1 0.043
2 541 17 750.9 17 746.6 717.9 0.040
2 772 17 415.6 17 399.1 686.5 0.039
3 003 17 477.7 17 432.2 665.3 0.038
3 234 18 911.3 18 888.2 678.3 0.036
3 465 23 817.4 23 785.8 728.1 0.031

Table 10
Estimation of the volumetric heat generation (𝑞𝑉 ) in the Li-ion battery at each time
Fig. 19. Variation of the estimated volumetric heat generation (𝑞𝑉 ) with time in a real interval for a discharge rate of 1C using ‘‘online’’ Bayesian method with priors.
cylindrical Li-ion battery for various discharge rates (0.5, 1, and 2C). Time (t), s Mean (W∕m3 ) MAP (W∕m3 ) SD (W∕m3 ) SD/Mean
231 21 587.8 21 900.8 1 568.4 0.072
462 25 638.6 25 963.9 1 447.8 0.056
693 25 635.2 25 726.3 1 196.2 0.046
The variation of the estimated volumetric heat generation (𝑞𝑉 )
924 23 548.8 23 693.2 972.2 0.041
with time using the ‘‘online’’ Bayesian method is shown in Fig. 19 for 1 155 21 854.1 21 940.8 834.6 0.038
various discharge rates of 0.5, 1, and 2C. The estimated volumetric 1 386 20 388.2 20 417.7 712.8 0.034
heat generation for 0.5, 1, and 2C discharge rates are compared against 1 617 19 516.5 19 531.5 627.8 0.032
literature and the same comparison is presented in Table 13. Cao et al. 1 848 18 599.1 18 641.7 578.2 0.031
2 079 18 232.8 18 264.1 540.5 0.029
[33] and He et al. [56] used the same cylindrical Li-ion battery of type
2 310 18 040.5 18 054.4 503.9 0.027
18650 and obtained volumetric heat generation in the Battery using 2 541 17 739.5 17 752.7 473.4 0.026
the Lumped capacitance and electrochemical models, respectively. Ta- 2 772 17 391.2 17 401.5 449.9 0.025
ble 13 shows the validation of the average values of the volumetric 3 003 17 440.2 17 441.1 455.0 0.026
heat generation rates estimated from present study with the literature 3 234 18 890.7 18 889.5 455.5 0.024
(Cao et al. [33], He et al. [56]). From this table, it can be observed 3 465 23 800.5 23 789.7 481.3 0.020
that the average values of the estimated volumetric heat generation
rates for 0.5, 1, and 2C discharge rates are close to the literature
(Cao et al. [33], He et al. [56]). Parity plots are also presented for variation with time in the forward model for various discharge rates of
validation of the estimated volumetric heat generation against in-house
0.5, 1, and 2C is shown in Fig. 21.
experiments for 0.5, 1, and 2C discharge rates. For this, the simulated
temperatures are calculated on the surface of the battery by giving
6.3. Application and advantages of the estimated temperature-dependent
the estimated volumetric heat generation variation with time in the
forward model of the battery for 0.5, 1, and 2C discharge rates and thermal properties and volumetric heat generation
compared them against in-house experimental temperatures measured
at the same locations (see Figs. 20(a), (b), and (c)). From these figures, In the present study, the hot spot temperatures (shown in Fig. 21)
it is clear that the experimental and estimated simulated temperatures in the absence of BTMS are identified to be 25.4, 30.2, and 42.1 ◦ C at
are within the uncertainty of ±1.5 ◦ C. The smaller deviation indicates 6992, 3465, and 1700 s time instants for 0.5, 1, and 2C discharge rates,
the accurate estimation of the volumetric heat generation variation respectively. The hot spots obtained for the discharge rates of 0.5 and
with time in the battery using inverse methodology solution. 1C are below the maximum operating temperature (40 ◦ C) of a cylin-
The hot spot (maximum temperature) variation with time in the Li- drical Li-ion battery, which are acceptable. However, for a discharge
ion battery obtained by giving the predicted volumetric heat generation rate of 2C, the obtained hot spot is above the maximum operating

13
S. Kumar et al. Applied Thermal Engineering 236 (2024) 121752

Fig. 20. Parity plot between the experimental temperatures and the simulated temperatures (obtained by giving the estimated volumetric heat generation variation in the forward
model) for (a) 0.5 (b) 1, and (c) 2C discharge rates.

Table 11 Table 13
Estimation of the volumetric heat generation (𝑞𝑉 ) in the Li-ion battery at each time Validation of average value of the estimated heat generation rate with
interval for a discharge rate of 2C using ‘‘offline’’ Bayesian method. literature.
Time (t), s Mean (W∕m3 ) MAP (W∕m3 ) SD (W∕m3 ) SD/Mean Average value of volumetric heat generation rate (W)
200 72 646.1 72 613.8 7 073.1 0.097 C-rate Present study Cao et al. He et al. [56]
300 91 595.8 91 268.1 5 258.6 0.057 [33]
400 97 315.1 97 053.5 4 576.2 0.047
0.5 0.10 ± 0.005 0.17 0.16
500 101 706.4 101 645.8 4 124.4 0.040
1 0.34 ± 0.012 0.55 0.28
600 102 266.4 102 861.4 3 708.2 0.036
2 1.51 ± 0.026 1.90 0.96
700 103 707.4 103 334.2 3 171.1 0.030
800 100 540.8 100 092.5 2 035.1 0.020
900 97 419.8 97 661.3 875.1 0.008
1 000 94 565.4 95 520.7 1 477.7 0.015
1 100 90 705.6 90 842.2 1 685.5 0.018
1 200 87 199.8 88 138.2 1 741.8 0.019
1 300 85 385.2 84 489.8 1 271.1 0.014
1 400 84 222.7 83 888.9 995.6 0.011
1 500 83 750.5 83 717.3 621.2 0.007
1 600 83 186.8 83 202.2 575.6 0.006
1 700 83 656.8 83 631.4 648.9 0.007

Table 12
Estimation of the volumetric heat generation (𝑞𝑉 ) in the Li-ion battery at each time
interval for a discharge rate of 2C using ‘‘online’’ Bayesian method with priors.
Time (t), s Mean (W∕m3 ) MAP (W∕m3 ) SD (W∕m3 ) SD/Mean
200 72 026.9 72 623.3 3 654.3 0.050
300 91 289.1 91 320.5 3 291.3 0.036
400 97 045.7 97 130.4 3 092.3 0.031
500 101 533.2 101 651.4 2 773.3 0.027
600 102 456.0 102 767.3 2 600.3 0.025
700 103 609.4 103 370.6 2 097.8 0.020
800 100 299.6 100 134.5 1 308.5 0.013
900 97 556.5 97 635.6 458.0 0.004
1 000 94 883.1 95 517.2 1 134.5 0.011
1 100 90 818.7 90 821.2 1 157.6 0.012 Fig. 21. Variation of the hot spot temperature with time in a real cylindrical Li-ion
1 200 87 390.7 88 108.4 1 370.3 0.015 battery for various discharge rates (0.5, 1, and 2C).
1 300 85 053.6 84 486.5 915.5 0.010
1 400 84 073.8 83 892.5 641.4 0.007
1 500 83 745.7 83 732.5 280.9 0.003
1 600 83 199.3 83 187.8 369.8 0.004 management system (BTMS). The simulated temperature distribution
1 700 83 644.5 83 615.1 433.5 0.005
in the Li-ion battery and the fluid domain of the BTMS obtained
from simulation in COMSOL are shown in Fig. 22(a). The inlet water
velocity, inlet water temperature, and battery discharge rate are taken
temperature of a cylindrical Li-ion battery, which is not acceptable. as 0.3 m/s, 28 ◦ C, and 2C, respectively. The hot spot strength and its
In view of this, thermal management of the battery is required. In location obtained from the simulation of BTMS are 28.9 ◦ C and (𝑟 =
1 mm, 𝜃 = 0, 𝑧 = 5 mm), respectively. Fig. 22(b) shows the hot spot
this section, one example of the battery thermal management system
variation over time for a discharge rate of 2C using BTMS simulation.
(shown in Fig. 22(a)) is demonstrated in which laminar forced liquid
The hot spot obtained using BTMS is 28.9 ◦ C, which is below the
(water) convection cooling is applied on the same Li-ion battery. The maximum operating temperature of the battery. Hence, with BTMS, the
estimated temperature-dependent orthotropic thermal properties (𝑘𝑟 , operating temperature of the battery is confined below 40 ◦ C, which
𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 ) and volumetric heat generation variation (𝑞𝑉 ) with time of enables more reliability and possibly longer durability of Li-ion battery
the present battery are used in the simulation of this battery thermal even for higher discharge rates.

14
S. Kumar et al.
Fig. 22. (a) The simulated temperature distribution in the Li-ion battery and the fluid domain of the BTMS for inlet water velocity, inlet water temperature, and discharge rate
of 0.3 m/s, 28 ◦ C, and discharge rate of 2C, respectively and (b) the obtained hot spot variation over time using BTMS for discharge of 2C.
7. Conclusions
A simple yet powerful inverse methodology named Metropolis
Hastings-Markov Chain Monte Carlo (MH-MCMC) based Bayesian
method was implemented in the present study to estimate orthotropic
thermal conductivities (𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 ), specific heat (𝑐𝑝 ), and volumetric
heat generation (𝑞𝑣 ) of Panasonic NCR18650BD battery. The unsteady
temperature distribution on the battery surface was initially mea-
sured experimentally when its base was maintained at a constant
temperature using a hot fluid circulator. The same experimental setup
was simulated using a forward model with the help of COMSOL for
different combinations of 𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , and 𝑐𝑝 . The unsteady simulated
temperatures obtained from simulations were trained as a function
of 𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , and 𝑐𝑝 using ANN as a surrogate model. The optimum
values of 𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧 , 𝑐𝑝 are estimated using Metropolis Hastings-Markov
Chain Monte Carlo (MH-MCMC) based Bayesian method by minimizing
error between experimental and predicted temperatures from ANN. The
same procedure was adopted to estimate the heat generation. However,
the experimental temperatures for driving the inverse approach and
final validation are obtained from discharge tests conducted for 0.5,
1, and 2C discharge rates. The estimated average values of 𝑘𝑟 , 𝑘𝜃 , 𝑘𝑧
and 𝑐𝑣 are observed to be 3.18 ± 0.19, 20.34 ± 1.26, 19.89 ± 1.29
(W/mK), and 3180 ± 202 (J/kgK), respectively, and the average heat
generation rates are calculated to be 0.1 ± 0.005, 0.34 ± 0.012, and
1.51 ± 0.026 W for 0.5, 1, and 2C discharge rates, respectively. The
thermophysical properties and heat generation which are estimated
from the procedure were plugged into the forward model and the
surface temperatures thus obtained were validated against in-house
experiments with the maximum uncertainty of ±1.5 ◦ C. The estimated
thermophysical properties and volumetric heat generation help to
identify the hotspot temperature in the battery domain which turned
out to be 42.1 ◦ C at a time instant of 700 s. This is beyond the
maximum operating temperature limits. The present study also re-
ported a thermal management system design that confines the hotspot
temperatures below 30 ◦ C, which was made possible by accurately
estimating thermophysical properties and heat generation with the
proposed inverse approach, coupled with the forced convection cooling.
The proposed inverse method is handy and can easily be implemented
for other battery chemistries and even for battery packs to estimate
hotspots and to design efficient cooling systems with limited knowledge
of electrochemistry.
15
Applied Thermal Engineering 236 (2024) 121752
Declaration of competing interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared to
influence the work reported in this paper.
Data availability
Data will be made available on request.
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