1. Introduction

In recent years, under a series of problems such as climate warming, air pollution, and energy crisis, battery electric vehicles have been rapidly developed and applied [1]. The main technology of electric vehicles consists of three parts: battery, motor and electronic control. In the field of batteries, lithium-ion batteries (LIBs) have become the first choice for electric vehicle batteries due to their advantages of high energy density, high charge-discharge efficiency, lower self-discharge rate, higher recyclability, and longer cycle life[2][3]。 However, with the increase in electric vehicles, frequent electric vehicle accidents have pushed the safety of electric vehicles to a new level, and battery failures account for more than 70% of electric vehicle fire accidents [4] 。 With the development of electric vehicles, batteries need to be able to charge and discharge at high currents, which will lead to a significant increase in the heat generated by electrochemical reactions inside the battery [5]. The accumulated heat of lithium-ion batteries will lead to a shortening of the service life of lithium-ion batteries. It can also cause more serious consequences, namely thermal runaway (TR), which is the most important safety issue for lithium-ion batteries [6]. When a lithium-ion battery experiences thermal runaway, it releases a large amount of heat in a short period of time, causing a fire or even an explosion [7].

The triggers of TR in lithium-ion batteries can be divided into three broad categories: mechanical abuse (shock, crushing, penetration, etc.), electrical abuse (overcharging, over-discharge, external short circuit, etc.), and thermal abuse [8]. The risk increases if the battery is operated in a high-energy battery pack, where thermal runaway can propagate from one cell to another, causing a chain reaction that causes thermal runaway propagation [9]. To support the widespread adoption of electric vehicles under a wide range of environmental conditions, and to meet the need for lifetime, longer range, and appropriate performance, while effectively suppressing the occurrence and propagation of thermal runaway, an effective and cost-effective battery thermal management system (BTMS) is required to ensure lithium-ionConditions of use of the battery [10].

Battery thermal management system (BTMS) technology is divided into active and passive categories according to its mechanism, active BTMS includes air-cooled, liquid-cooled, etc., and passive BTMS includes phase change materials, heat pipes, etc[11]。 Wu et al. [12] found that forced convection had a limited cooling effect on the battery, and the temperature distribution of the battery was uneven, and the thermal management was inconsistentIt didn't work out well. PCMs are able to respond to small temperature changes and absorb or release large amounts of heat [13]. Xu et al. [14] studied a novel phase change material for battery thermal management, and the results showed that its thermal management performance was excellent. The combination of an indirect cooling system and a direct flow cooling method through a cooling pipe can significantly improve the cooling effect [15]. At present, research on battery thermal management has focused on inhibiting TR propagation. Heat dissipation and thermal insulation are considered to be the two most common methods of preventing battery TR [16]. Feng et al. [17] concluded that TR propagation can be inhibited by increasing battery heat dissipation or adding thermal insulation between cells. In terms of heat dissipation, Xu et al. [18] studied the influence of heat dissipation fin parameters on the heat dissipation effect of the battery, and verified the thermal management of the system by combining air cooling and liquid coolingEffectiveness of the effect. In terms of thermal insulation, Sun et al. [19] studied different materials as thermal insulation layers between cells, and the structure showed that the use of thermal insulation layers can effectively inhibit the propagation of TR between cells. Although thermal insulation can effectively inhibit the propagation of TR, in extreme cases, if the heat cannot be dissipated in time, it will still spread to adjacent cells when it accumulates to a certain extentThe risk increases significantly [20]. Therefore, some researchers have adopted a variety of methods to inhibit TR propagation, but this will also make the battery module heavier and heavier, resulting in a decrease in the energy density of the battery system [21].Therefore, in order to balance the contradictory relationship between heat dissipation and heat insulation, and at the same time reduce the weight of the system as much as possible and save energy, the BTMS designed in this paper combines heat dissipation and heat insulation, which can not only effectively inhibit the propagation of TRIt can also take away the heat of the battery in time.

In this paper, the TR of the battery pack under six different schemes is analyzed, and a new type of BTMS composed of phase change material (PCM), thermal insulation material and liquid cooling is determined. The effects of cell spacing and water flow rate on battery cooling performance are then discussed. At the same time, the second main motivation of this study is to make BTMS not only effectively suppress TR propagation, but also save energy and reduce the impact on the energy density of the battery pack. Therefore, through comparative analysis, the final plan was determined.

The innovations in this work are as follows:

(1) In order to effectively inhibit TR propagation, a new type of BTMS combining phase change materials, thermal insulation materials and liquid cooling is proposed Through simulation comparison, the performance of the proposed scheme is significantly better than that of other schemes in the study.

(2) Through comparison, the effects of different cell spacing and liquid flow rate on battery temperature were analyzed.

(3) Through comparative analysis, the optimal combination of spacing and flow velocity is obtained, which improves the cooling effect and economy of BTMS.

2. Modeling and setup

2.1 Geometric construction

In the EV battery pack, the cells are arranged in an array. As shown in Figure 1, the BTMS studied in this paper is mainly composed of PCM, aerogel, cooling plate and cooling channel. 36 batteries were placed in the BTMS. When the spacing between cells is too large, a large amount of material will be consumed, which will increase the volume and mass of the whole system and reduce the energy density of the entire battery pack. When the cell interval is too small, the cooling performance of the battery will be reduced, increasing the risk of TR propagation. The lithium-ion battery pack is composed of two layers of aerogel and one layer of cooling plate, the thickness of the cooling plate is 3mm, the thickness of the aerogel varies with the cell spacing, and it is filled in the middle of the battery and the cooling plate, the phase change material is distributed on both sides of the battery, and the coolant is provided by the water pump to provide circulating power. In order to reduce energy consumption, the width of the runner is designed to be 2mm, and the serpentine cooling channel design has the advantages of increasing heat transfer per unit volume, reducing flow resistance, and reducing thermal stress. The geometric parameters of objects such as LIB, heater, PCM, and cooling plate are detailed in Table 1.

Figure 1 Schematic diagram of the new BTMS

Table 1

Key structural parameters of BTMS

Generally, the positive current collector of lithium-ion batteries is aluminum, the negative current collector is copper, and the positive active layer is a lithium-containing compound, which can be divided into lithium cobalt oxide, lithium manganese oxide, lithium iron phosphate, lithium titanate, and lithium nickel cobalt manganese oxide according to its chemical composition ( NMC), nickel-cobalt-lithium aluminate (NCA), etc., the latter two are called ternary materialsThe active layer of the negative electrode is a carbon material, usually graphite. The batteries used in electric vehicles are usually ternary materials or lithium iron phosphate, and the batteries in this study are prismatic NCM batteries. Prismatic batteries have the advantages of large capacity and few modules. The battery parameters are shown in Table 2.

Table 2

Battery parameters

Table 3

Aerogel thermophysical parameters

Table 4

PCM thermophysical parameters

2.2 Governing Equations and Boundary Conditions

Three models were involved in this study. The first is the lithium-ion battery electrochemical model, which is used to represent the chemical reaction processes inside the operation of the lithium-ion battery. The second is the heat transfer model, which is used to represent the heat generated by various chemical reactions and the transfer process of heat between various materials, which can calculate the spatial distribution and evolution of the temperature inside the battery. The third is the fluid model, which is used to represent the operating process of the coolant. By coupling the three models, the heat production model of the battery and the solid-liquid heat transfer model can be realized.

The charging and discharging process of lithium-ion batteries is reflected in the movement of lithium ions between the positive and negative electrodes and the embedding/de-intercalation of the positive and negative electrode materials, and the movement of an equal amount of electrons outside the battery. Based on Doyle and Newman et al. [22] [23].The proposed theory can be used to establish an electrochemical model of the battery. The model can explain the various chemical reactions that occur inside the battery, and then calculate the parameters of the battery, such as positive and negative electrode potential, current density, state of charge, lithium ion concentration, and heat participation. The internal chemical reaction process of lithium-ion batteries can be represented by equation (1).

The reaction rate of the conventional intercalation and deintercalation (Eq (1)) can be calculated by Butler-Volmer equation(Eq.(2))[24]:

where is the local charge transfer current density, is the exchange current density, is the local surface overpotential, andThe charge transfer coefficients of the anode and cathode are the Faraday constant, the ideal gas constant, and the temperatureis the maximum concentration of lithium ions in the active material, is the particle surface concentration, and k represents the reaction rate coefficient.

The current exchange density can be expressed by Eq. (3):

where and is the reaction rate constants of the anode and cathode, respectivelyis the concentration of lithium ions in the active material, is the concentration of lithium ions in the electrolyte phase, and is the reference concentration of lithium ions in the electrolyte phase.

The internal chemical reaction of lithium batteries follows the conservation of mass. The separation diffusion equation of lithium in active solid particles satisfies Fick's second law [25]:

Ds represents the diffusion coefficient of lithium ions in the solid phase, t is the time, and r represents the lithium ions in the detached, The distance from the center of the active particle when embedded in the active particle.

S is the specific surface area, which is the solid phase volume fraction, and _R0 is the particle radius, i_nThe current density is transferred for the local charge.

The equation for the diffusion of lithium ions in the liquid phase [26] is given in Eq. (7).

In the above equation, the effective diffusion coefficient of lithium ions in the liquid phase is described. is the electrolyte volume fraction and t+ is the lithium ion transfer number.

At the same time, the conservation of charge in lithium-ion batteries follows Ohm's law, which can be described as [26]:

When the model is set, the positive and negative current collector boundaries can be set to constant charging current and zero potential to ground, respectively, and the fluxless boundary conditions can be set in the model to achieve the conservation of charge and the conservation of matter in the model.

In the operation of lithium batteries, various kinds of heat will be generated, and the heat production in the normal charging and discharging process is mainly composed of ohmic heat, reaction heat, polarization heat and the decomposition of various side reactions inside the battery to produce heat. When thermal runaway occurs in the battery, the main reason for the battery heating up is the decomposition reaction between the components inside the battery and the electrolyte due to the rupture of the separator. According to the law of conservation of energy, the heat production of lithium-ion batteries can be expressed as [27]:

where represents the reversible heat of the electrochemical reaction, the irreversible heat due to the polarization of the electrode, and the heat of the side reaction when TR occurs in the batteryIndicates the heat dissipated into the environment.

The reversible and irreversible heat of the electrochemical reactions that occur during the normal operation of the battery are as follows:

where əE_oc/əT stands for temperature coefficient, E and E_OC stands for Battery Voltage and Open Circuit Voltage.

Due to the increase in the temperature of heat production, when the battery does not apply any protective measures, it will produce convective heat transfer with the external environment, which can be described by Newton's law of cooling [28].

When TR occurs in the battery, four side reactions will occur successively with the increase of temperature, namely SEI film decomposition reaction, negative electrode and electrolyte reaction, positive electrode reaction and decomposition solution and electrolyte decomposition reaction. The heat generated by the four side reactions was Q _sei, Q_ne, and Q, respectively_pe, Q_e indicate that the total heat generated by the battery when it is TR is as follows Eq. (15）

Each side reaction will produce a large amount of heat, and when the heat accumulates to a certain extent, the battery will burn violently or even explode. The four side reactions all follow the Arrhenius equation, which is expressed as follows [29]:

Table 5 details the names of the parameters in the equation as well as the initial values.

The boundary conditions at the interface between the various materials and their surroundings are as follows:

where i stands for LIB, PCM, aerogel or cooling plate, kT is the thermal conductivity, h is the convective heat transfer coefficient, and Tamb is the ambient temperature.

At the same time, when protective measures are applied, the heat transfer between the battery and the various materials should satisfy the basic heat transfer equation shown in Eq. (26) [19].

where ρ, C_p, and dT/dτ represent the corresponding correspondingsDensity, specific heat capacity and temperature rise of the components, λx, λy, λz represents the thermal conductivity in the X, Y, and Z directions, respectively.

Table 5

Physical and kinetic parameters and initial values of the TR model [30].

In addition, the initial and ambient temperatures of the entire system are 25 °C, and the convective heat transfer coefficient h with the environment is 10 W/(^m2 °C)

For modeling a fluid model, you first need to determine whether the fluid flow is laminar or turbulent. Eq. (27) calculates the Reynolds number of the coolant Re[31]. When the Reynolds number is less than 2300, it is laminar flow [32]. The flow velocities discussed in this study range from 0.01 m/s to 0.04 m/s, combined with the material properties in Table 3, show that the maximum fluid Reynolds number for all cases in this study is less than 2300, so the fluid flow state is laminar.

where ρc represents the coolant density, μ represents the dynamic viscosity, and uc represents the average velocity of the coolant in the cooling channel, DhIndicates the hydraulic diameter.

The fluid is assumed to be an incompressible continuous fluid. The flow of coolant can be described by the Nass-Stokes (N-S) equations, including the continuity equation, the momentum conservation equation, and the energy conservation equation [33], as follows:

where u is the velocity vector, f is the force applied per unit volume, p is the pressure, and the dynamic viscosity is the μ.

2.3 Simulation Steps

The Lithium-Ion Battery Interface, Solid and Liquid Heat Transfer interfaces, and other interfaces are built into the COMSOL Multiphysics software to simulate the battery electrochemistry, heat transfer, and fluid models used in this study.

First, the parameters used in the model are set in the software, the geometry is built, and the corresponding material properties are added. Secondly, add physics interfaces, set boundary conditions and initial values, and reasonably divide the area mesh. Finally, add the study and set the solver configuration. The study is divided into three steps: the steady-state solver is mainly for the fluid, which can stabilize the steady flow of the fluid during the simulation; The current distribution initialization solver enables the initial values of the electrochemical model to be used for calculations, for example. The transient solver is used to compute the results of the coupling of the individual physics and to output the parameters of the model as a function of time. The time-dependent solution time and step size can be adjusted appropriately according to the model.

3. Verify the model through experiments

3.1 Grid independence check

Meshing is a key step in simulation research, and reasonable meshing can save computing resources and improve the accuracy of the model. The purpose of the mesh independence check is to find the appropriate number of meshes, which can be considered as a mesh when the result error is less than 5% as the number of meshes increases to a certain extentThe division is reasonable. In this study, a new type of BTMS was used to check the grid independence under four mesh numbers. See Table 6 for details

3.2 Model Validation

Wang conducted an experimental study on the electrochemistry of lithium batteries, established the model based on its electrochemical model parameters, and compared and verified it with its experimental structure, and the results showed that the simulation and experimental data had a good fit, which verified the feasibility of the battery electrochemical-thermal coupling model.

The prismatic lithium-ion battery was selected for the experiment, and the cathode active layer material was NMC111. The material of the negative active layer of the battery is graphite; The material of the positive current collector is aluminum foil, and the material of the negative current collector is copper foil. By coupling the heat generation of the model electrochemical model and the temperature of the heat transfer module of the solid heat transfer module, the temperature change model of the battery during charging can be obtained. Set the initial state of charge of the battery to 0.1, the cut-off charge voltage to 4.2V, the surface heat dissipation coefficient of the battery to be 10/(m2 °C), and the ambient temperature to be 25°C. The charging rate of 1C and 3C were used to simulate and calculate, and the calculation results were compared with the experimental results, as shown in Figure 2.

Figure 2

Figure 2(a) and (b) represent the changes of battery voltage and temperature over time at different charging rates, respectively, where the scattered points are the experimental data and the line segments are the simulation results. Fig. 2(c) and (d) are the error plots of the temperature and experimental data of the battery at 1C and 3C charging rates, respectively. It can be seen that the experimental and simulated data are in good agreement with time at different magnifications. There are some errors in the voltage and temperature of the experimental and simulated batteries, which may be due to the aging of the experimental battery and the errors caused by the environment, but the relative errors are within the allowable range.

Based on the electrochemical-thermal coupling model of lithium batteries, the thermal runaway model of lithium-ion batteries was established, and the effectiveness of the thermal runaway model of lithium-ion batteries was verified by comparing with Huang's experimental data. In the thermal runaway experiment, the battery selected is a ternary (Li(Ni1/3Co1/3Mn1/3)O2) lithium battery, and the nominal capacity of the battery is40Ah, the charging voltage is 2.75V, and the cut-off voltage is 4.2V.

Figure 3

The battery model is shown in Figure 3, the heater is a heating plate with a thickness of 3mm that fits the battery completely, and the heating power of the heater is 400W100%SOC。 The convective heat transfer coefficient between the battery and the environment is 10W/(m2 °C) and the ambient temperature is 25°C. The temperature probe in the model is consistent with the experiment, and the point probe is arranged between the heater and the battery. Figure 4 shows the comparison between the simulation results and the experimental data.

Figure 4.

Fig. 4(a) is the temperature-time image of the experiment and simulation during the TR occurrence of the battery, and Fig. 4(b) is the error image of the experiment and simulation. In the experiment, there is some heat exchange between the bottom of the battery and the bottom plate, and there is also a gap between the heater and the battery, which leads to an increase in thermal resistance, all of which lead to errors between the simulation and the experimental data, because the relative errors mentioned above are in a small rangeTherefore, it can be considered that the model effectively realizes the simulation analysis.

4. Results and Discussion

4.1 Influence of different pathways on inhibiting thermal runaway propagation

In this paper, the thermal runaway propagation of the battery pack under different schemes is discussed. The battery pack model is shown in Figure 4, the battery thermal runaway model is the model of the previous simulation control, and the heater size is the same size as the battery, which acts as the battery that is experiencing thermal runaway. The heating power of the heater is 500W, and the heating time is 1500s.

Figure 5

Table 3 summarizes the specific measures taken under the different programmes. Electric heaters are used as well as cells where thermal runaway occurs, transferring heat to the system to simulate thermal runaway propagation of the battery pack. In order to control the variables, the effects of the different schemes are more intuitively distinguished, in each case, the cell spacing is 5mm, the convective heat transfer coefficient at the boundary is 10W (m-2 K-1), the ambient temperature and the initial system temperature are all the same25℃。 In scenarios 4 and 6, the flow velocity at the coolant inlet is 0.02m/s and the relative static pressure at the coolant outlet is 0 Pa with no slip in wall conditions. The physical parameters of PCM, aerogel, and liquid cooling materials in the scheme are listed in Table 2.

Table 3 Specific measures for different scenarios

Figure 6 (a) Unprotected battery temperature-time image (b) Aerogel battery temperature- Time image

(c) PCM cell temperature-time image (d) Coupling battery temperature using aerogel and liquid cooling- Time image

(e) PCM and liquid-cooled coupled battery temperature-time images

(f) Temperature-time images of integrated aerogel, PCM, and liquid-cooled coupled batteries

In Scheme 1, the air around the battery is quickly heated, and heat accumulation leads to thermal runaway of the battery pack, as shown in Figure 6(a),1The secondary reactions of the battery began to occur one after another around the 1800s, and the temperature rose rapidly, reaching a maximum temperature of 620°C around the 2000s, and only at intervals800s successively caused TR in No. 2 and No. 3 batteries, and it can be seen that there are no protective measuresThe thermal runaway of the battery is very easy to propagate, and once the thermal runaway of the battery occurs, it will cause great danger; In Scenario 2, as can be seen in Figure 6(b), the thermal runaway time of the battery is compared to the scheme1 In advance, because PCM due to the high thermal conductivity, not only can not delay the thermal runaway time, but even accelerate the thermal runaway propagation between batteriesHowever, the maximum temperature of the battery thermal runaway is reduced to below 600°C; In Scheme 3, as can be seen from Figure 6(c), while aerogel delays the propagation of heat from a thermal runaway cell to a normal cell, However, the system dissipates heat poorly, resulting in thermal runaway of the battery pack.In scheme 4, a cooling plate is used to place it between the cells, as can be seen in Figure 6(d).Removing heat through the cooling water has a good effect on suppressing the thermal runaway of the battery, the battery does not occur TR, and the maximum temperature of the No. 1 battery in the battery pack is only 90°CAround; In scheme 5, the structure of the PCM is adjusted, the PCM material is removed between the cells, and the PCM material is placed on both sides of the battery. And the cells are aerogel between them, and the simulation results are shown in Figure 7(e), the batteries have no thermal runaway, and the maximum temperature of the No. 1 battery is 73°C. It shows that the heat transfer between cells is reduced by aerogel, and the PCM has a good effect on heat dissipation on both sides of the battery, but due to the limited heat dissipation effect of PCM, the battery cools down slowly in the future. Scheme 6 is a new type of BTMS studied in this paper, compared with scheme 5, cooling plates are added between the cells to remove the heat of the battery pack, and the simulation results show that aerogel and PCM are usedCoupling with liquid cooling is the best effect on battery heat dissipation, through phase change materials and liquid cooling to take away heat, thermal insulation materials to delay the spread of heat, through the coupling of the three, the relationship between heat dissipation and heat insulation can be balanced, as shown in Figure 6(f) shows that the maximum temperature of the No. 1 battery is reduced to only 60°C. Compared with other schemes, scheme 6 not only successfully inhibits the occurrence of TR, but also reduces the maximum temperature of the battery to 60°C, and the simulation structure shows that scheme 6The new BTMS has very good performance.

Fig. 7(a)-(f) shows the three-dimensional temperature distribution of each scheme at different times. Through these temperature charts, the heat transfer process and the comparison of cooling effects can be more intuitively observed.

Figure 7 Temperature distribution at different times with different measures: (a) unprotected; (b) the use of aerogel; (c) the use of PCM;

(d) the use of aerogel and liquid cooling; (e) the use of PCM and liquid cooling; (f) Use of aerogel, PCM and liquid cooling

4.2 Effect of flow rate and cell spacing

In the above studies, an integrated thermal management system is highly effective in blocking the spread of thermal runaway. For integrated battery packs using aerogel, PCM, and liquid-cooled coupling, the effects of cooling water flow rate and cell spacing on cell temperature are studied separately below.

When studying the effect of cell spacing, the coolant flow rate was set to 0.02 m/s, and the thermal insulation material filled between the cells as the cell spacing increased, and Figure 8 shows the temperature of cell No. 1 at different cell spacing.

Figure 8

When studying the cooling water flow rate, the cell spacing is 2 mm, and Figure 10 shows the temperature of No. 1 battery with different flow rates.

Figure 9

4.3 Improvement of battery thermal management system

Combined with the appeal study, considering the energy consumption and the overall energy density of the battery pack, the solution with a cooling water flow rate of 0.03m/s and a cell spacing of 6mm was finally adopted. Figure 11 shows the temperature time of each cell in this scheme, and the maximum temperature of battery 1 is only 43°C.

Figure 10

The temperature distribution of the middle section of the battery can be observed by observing the temperature distribution of the middle section of the battery, as shown in Figure 12, at 4000s, the temperature difference of the middle section of the No. 1 battery is less than thatAt 2°C, the temperature difference between No. 2 and No. 3 batteries is smaller, only less than 1°C, indicating that the integrated solution can better prevent thermal runaway of the battery pack. And it does not cause damage to the battery.

Figure 11

5. Conclusion

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