1. Introduction
Energy storage systems, such as fuel cells, batteries, flywheels, and ultracapacitors, play important roles in pure electric vehicles and the hybrid electric vehicle industry. There are currently three leading types of batteries in the market: Li-ion, nickel–metal hydride, and lead–acid. The Li-ion battery is a promising candidate with outstanding features, including a low self-discharge rate, high specific energy, and fast charging capacity without a memory effect [
1]. However, the internal electrochemical reactions and resistances in its cells produce a considerable amount of heat. This results in fairly high and non-uniform cell temperatures when it is charged and discharged. The optimal operating temperature of a Li-ion battery ranges from 25 °C to 40 °C [
2]. In addition, the maximum temperature difference within a cell should be less than 5 °C to maintain a balance between its life cycle and efficiency [
3]. When the maximum temperature is higher than 80 °C, thermal runaway could happen and exothermic reactions will occur, eventually leading to catastrophic results [
4].
Various thermal management strategies have been proposed, which can be classified into the active (air and liquid cooling), passive (phase change material (PCM) cooling and heat pipes), and hybrid methods. Chen et al. [
5] optimized the distance between cells to improve the air cooling performance, whereby the maximum temperature of the battery pack was decreased by 4 K and the maximum temperature difference was decreased by 69%. Under uphill conditions (high heat generation and/or a high discharge rate), liquid cooling may be required to sufficiently dissipate the thermal energy. Shang et al. [
6] achieved the best performance of liquid cooling when the width of the cooling plate was 70 mm, the inlet had a temperature of 18 °C, and the mass flow rate was 0.21 kg/s. In that setup, the maximum temperature was decreased by 12.61% and the temperature uniformity was increased by 20.83%.
PCMs have been shown to greatly improve the temperature uniformity of Li-ion batteries. Wang et al. [
7] showed that the melting process can be sped up by using a paraffin/aluminum foam composite. Compared with pure paraffin, the heat storage time of that composite PCM was 74.4% when the heat flux was 12,000 W/m
2. Jilte et al. [
8] proposed the best design with seven cells, seven primary containers, and one secondary container. At the environment temperature of 40 °C, the use of a nanoparticle-enhanced PCM (nePCM) can reduce the temperature of a cell to under 46 °C with the effect of natural convection.
Heat pipes are employed as effective systems to maintain homogeneity on the evaporator surface at a constant temperature while having high thermal conductivity. Putra et al. [
9] investigated the cooling capacity of alcohol, acetone, and distilled water at a heat flux load of 1.61 W/cm
2. They demonstrated that acetone is a potential candidate with a thermal resistance of 0.22 W/°C and an evaporation temperature of 50 °C. For the hybrid method, Yang et al. [
10] studied the thermal performance of a battery thermal management system (BTMS) integrated with mini-channel liquid cooling and air cooling. At 80% depth of discharge (
DOD), the maximum temperature and the temperature difference were decreased by 11.12 K and 9.52 K, respectively, when the water flow rate increased by 2.2 × 10
−4 kg/s. If the air velocity increased from 0 to 4 m/s, the battery temperature was reduced by 2.22 K, and the temperature uniformity was decreased by 2.04 K.
Kiani et al. [
11] designed a hybrid thermal management system with a nanofluid integrating metal foam and a PCM. Compared with water cooling, the nanofluid with volume fraction of 2% increased the operating time of the battery by 29% at a Reynolds number of 420. Jilte et al. [
12] investigated heat dissipation in cylindrical batteries with liquid channels and a PCM. At an environment temperature of 40 °C, the surface temperature of the battery was kept under 43 °C if the PCM was applied, and under 41.2 °C if the PCM and liquid channels were used simultaneously. Depending on the desired effectiveness, the BTMS can be applied either alone or in combination, but it should meet several criteria: high reliability, easy maintenance, low power consumption, and insignificant mass.
Different numerical modeling approaches have been used to investigate the thermal behavior of Li-ion batteries. They vary from 1D thermal models without thermal interaction among the cells, to complex 3D thermal models which consider non-isothermal and heat generation rates. Jollyn et al. [
13] developed a 1D transient battery model based on daily cycles, such as 12 min and 72 min. They found that a proper PCM thickness was 1.75 mm when the maximum temperature decrease was 12.9 °C. Greco et al. [
14] performed simplified battery thermal management using a PCM/compressed expanded natural graphite (CENG) composite. Their 1D solutions were in good agreement with their 3D results. Hallaj et al. [
15] successfully demonstrated that the maximum temperature at the core of a battery pack was 80 °C with a small temperature variation of 3 °C at a 10 A discharge rate. Furthermore, they designed a battery pack integrating a PCM matrix with a significant decrease in charge time and weight for plug-in hybrid vehicles.
In the field of Li-ion battery research, for a 1D model, Hallaj et al. [
16] developed a transient-state battery prototype with a thermally homogenous domain. An example is the Sony US18650 battery, which can be scaled up to a Li-ion cell of 100 Ah capacity in safe operating conditions. Sato et al. [
17] categorized the heat-generating factors of reaction in a battery as reaction heat, polarization heat, and joule heat. Yi et al. [
18] estimated temperature variations over time from electrochemical reactions and ohmic heat. They found that under a constant discharge rate, the potential density on the electrodes is a function of discharge time.
Akeiber et al. [
19] predicted the heat storage capacity of a PCM of paraffin (40% oil and 60% wax) by solving a 1D numerical model. Fortunato et al. [
20] obtained a 2D solution for different temperature profiles and total melting times with a PCM. Samar et al. [
21] investigated 2D melting procedures for paraffin wax in ANSYS Fluent software, and showed that a PCM container induced a faster melting process.
In the present study, a 1D and a 3D Li-ion battery model were evaluated and compared with experimental data under 3C and 5C discharge rates. For a 3D model, two common approaches have been developed: the equivalent circuit model and the Newman, Tiedemann, Gu, and Kim (NTGK) model; the latter was used here. The main objective was to investigate the effect of PCM thickness and thermal conductivity on thermal management performance using the CFD technique with an NTGK model.
3. Results and Discussion
In this study, the effect of the thickness and thermal conductivity of a PCM on the cooling performance of a Li-ion battery are investigated. The PCM was of three different thicknesses, 0.5 mm, 0.55 mm, and 0.6 mm, and the thermal conductivity of the PCM was enhanced based on the practical application.
3.1. Effect of PCM Thickness
The major drawback with most organics, particularly the family of paraffins, is that they possess low thermal conductivity. A thin PCM easily melts fully and does not produce sufficiently effective temperature reduction. With a thick PCM there is a solid region farther from the battery and a superheated liquid region next to the battery, so instead of behaving as a thermal sink, the PCM may behave as a thermal isolator.
As shown in
Figure 8, the maximum temperatures of the Li-ion batteries without a PCM were 64.86 °C and 86.83 °C at the end of the 3C and 5C discharge rates, respectively. As mentioned previously, the best temperature range is 25 °C to 40 °C and the safe temperature range is −20 °C to 60 °C for Li-ion battery operation. Moreover, the capacity fade of Li-ion cells can be 36.21% after 800 cycles when the operating temperature is around 45 °C, and the loss can even reach 70.56% after 500 cycles when the operating temperature is approximately 55 °C. At the 3C discharge rate, a PCM with a thickness of 0.6 mm or thinner can maintain the battery temperature in a safe condition. With a 0.6 mm thick PCM layer, the maximum temperature can decrease by 1.28 °C or 6.54 °C, depending on the fast or slow discharge rate.
Three stages along the temperature elevation curve clearly exist in the battery with a PCM (
Figure 8).
From a starting temperature of less than 28 °C, it grows markedly. It takes about the first 3 s (5 s) to reach the limitation for the 5C (3C) discharge rate. The slope was similar to the one without PCM. The energy storage relies solely on low sensible heating (in this case, 2150 J/kg·K).
During the melting process, the battery temperature drops into the phase change temperature range. The temperature increases slightly since thermal energy is absorbed as the heat of transformation. Under the 3C discharge rate, this process occurred in 20 s to increase the temperature to ~31 °C. The PCM started to melt from the inner to the outer layer, and then melted entirely.
Finally, the PCM was at a liquid state with both low thermal conductivity and low specific heat. The temperature of the battery climbed considerably again but the slope was still less than the one without a PCM. The predicted temperatures had almost identical trends in their final stages.
Figure 9 is a close-up of the battery temperature change at the initial stage of the discharging process. Under the high discharge rate of 5C, it took 17.4 s to rise above 40 °C. This process could be extended to 34.8 s when the PCM thickness was 0.5 mm. Similarly, with the 3C discharge rate, it took much longer (40.3 s) to reach 40 °C. This operation could take up to 144.3 s with a 0.5 mm thick PCM.
As shown in
Figure 10, at the end of the discharging process the battery temperature linearly varied with the thickness of the PCM. When the thickness decreased by 0.05 mm, the temperature also declined 5.3 °C at the 5C discharge rate. This compares with a decline of 2.7 °C at the low discharge rate of 3C.
3.2. Effect of PCM Thermal Conductivity
The response time is a substantial factor in the design of a PCM system. There are several approaches to improve heat dissipation, such as enhancing the thermal conductivity, setting the ullage space far from the heat source via a potential container, and installing the PCM in the heat flow path. It is generally agreed that a material that has a high energy storage capacity will have low thermal conductivity. Therefore, much research interest has been focused on enhancing the thermal conductivity of PCMs.
Recently, Venkateshwar et al. [
29] investigated heat storage performance when embedding aluminum metal foam (MF) in n-octadecane. They used Equations (21) and (22) to determine the effective thermal conductivity of that PCM–MF composite, given as:
With the porosity set to 0.972, the structure with a thermal conductivity of 2.394 W/m·K conducted faster than pure n-octadecane without sacrificing the available volume.
Sari et al. [
30] examined the transient thermal influence of paraffin absorbed into expanded graphite (EG). They determined that the PCM composite, with a 10% mass fraction of EG, had stable properties. The thermal conductivity of the PCM–EG linearly varied with the mass fraction of the EG. Compared with pure n-octadecane, the thermal conductivity could reach 0.828 W/m·K when integrated with the proper amount of EG.
In a macroscopic approach, the use of carbon fibers (CF) was considered by Fukai et al. [
31] as an advanced technique. The effective thermal conductivity of the PCM composite was around three times higher than the pure PCM at
, as calculated in the following formula:
As a result, the thermal conductivity of paraffin combined with CF was 0.678 W/m·K.
Figure 11 shows the battery temperature change during the discharging process under natural convection. The higher the thermal conductivity of the PCM composite is, the more effective the heat dissipation capacity is. Additionally, aluminum foams make the melting process more uniform. The thermal improvements of PCM composites are summarized in
Table 5. At the end of the discharging process, the percentage of temperature reduction with PCM–MF was about 1.2 and 1.3 times higher than with PCM–EG and PCM–CF, respectively.
3.3. Comparison of 1D Calculation and 3D Simulation
We compared our 1D analysis and a 3D simulation of the 0.5 mm thick PCM–MF model. A hexahedral grid was generated for the battery and the PCM domain, while the ambient air domain was divided by polyhedral elements, as shown in
Figure 12. The bottom was set to be adiabatic and the other surfaces were set to atmospheric pressure. For the pressure–velocity coupling, the ANSYS Fluent coupled algorithm was employed. A second-order interpolation scheme was used to approximate the convection terms in the momentum, energy, and potential equations, whereas a PREssure STaggering Option (PRESTO) scheme was selected for the pressure field. For the conjugate heat transfer problem, the following assumptions were applied:
Only natural laminar convection took place in the ambient environment.
The initial temperature of the battery and the PCM were set to the same as the ambient temperature (25 °C).
There was no flow in the PCM liquid phase.
The data from the late stage of the analysis for the 1D calculation was excluded because it was too noisy; nevertheless, we found that the 1D and 3D solutions matched well when extending the results while maintaining the curve slope (
Figure 13). This agreed with the results of Greco et al. [
14], who showed that cooling paths were totally dissimilar in the initial periods of the analytical and computational approaches, but they definitely matched at the end stages.
Figure 14 shows the temperature uniformity in the 3D Li-ion battery model. At the low discharge rate of 3C, the tmperature disparity in the cell was maintained under 5 °C. At the higher discharge rate of 5C, it markedly escalated due to sudden heat generation. However, the PCM exhibited outstanding improvement, with a 6.6 °C peak difference of temperature.
At the center plane of the cell, two monitoring lines were selected to explore the temperature change at z = 0.1245 m and y = 0.1135 m, as depicted in
Figure 15a.
Figure 15b shows the temperature along the vertical line at the end of discharging. There was a large difference of 15.5 °C between the top and bottom positions under the 5C rate without a PCM. The use of PCM–MF caused a sudden change in temperature in the lower area of the cell at the 3C discharge rate, due to a liquid mushy PCM zone. It can be seen in
Figure 15c that the temperature varied slightly in the horizontal direction and tended to be more stable when the PCM was applied. All of the differences were below 1 °C. Because the heat source was concentrated in the region close to the current collecting tabs, the temperature variation was clearly greater in the vertical direction than in the horizontal direction.
Basically, the temperature distribution on the battery surface can be divided into two parts: an upper region with higher temperature and a lower region with lower temperature. Without a PCM, the battery temperature increased more continuously and homogeneously from the bottom to the top under the 3C discharge rate. This difference was 6.8 °C. However, there was greater difference in temperature (18.8 °C) under the 5C discharge rate. The highest temperature was located near the positive and negative tabs, as shown in
Figure 16.
Similar trends were observed in the case with the PCM. However, there was a smaller temperature difference at the 3C as well as the 5C discharge rates because thermal energy from the battery was absorbed into latent heat. The maximum temperature was located at the negative tab (left tab), which was not cooled by the PCM. For this reason, an active cooling method, such as forced convection, may be necessary. The differences in temperature were 4.5 °C and 8.2 °C on the entire battery surface under 3C and 5C discharge rates, respectively.
Depending on the amount of heat generated, the PCM can be partly or totally melted. The PCM remained in the mushy zone in the lower region under the 3C discharge rate, while it completely transformed to a liquid state under the 5C discharge rate.
4. Conclusions
A 1D thermal management model of a large-format Li-ion battery (52.3 Ah) with different PCM properties was evaluated. This pouch-type battery was sandwiched between two n-octadecane layers, and the heat generation agreed well with experimental data under both the 3C and 5C discharge rates. The diffusion equation that governed the thermal transfer capacity in the PCM was also solved simultaneously. By considering different PCM thicknesses and thermal conductivities, a potential model was proposed, which was an assemblage with aluminum foam embedded in n-octadecane. The average conductivity of the resulting enhanced PCM–MF was 2.394 W/m·K. The maximum temperature of the Li-ion battery reached 86.8 °C after 550 s under the 5C discharge rate and 64.9 °C after 900 s under the 3C discharge rate without a cooling system. It was shown that the 0.5 mm thick PCM–MF composite reduced the maximum battery temperature to 49.7 °C and 33.9 °C at the 5C and 3C discharge rates, respectively.
Then, 3D transient thermodynamic simulations were carried out with an NTGK model using ANSYS Fluent software. Based on comparison with these 3D simulations, we found that the 1D analysis was capable of accurately estimating the heat dissipation by the PCM–MF at the end stage of discharging. The 1D approach clearly produced reliable results in predicting the thermal behavior of the PCM–MF cooling and was superior in practical application terms with its low cost and less time consumption.
Further study on the thermal behavior of active cooling systems with PCMs will be necessary.