1. Introduction
Global oil resources will eventually dry up and fossil-fueled vehicles are a major source of greenhouse emissions. There is an ongoing global trend of electrifying transportation, and as a result, intensive research is being conducted into electric vehicles and hybrid electric vehicles (EVs and HEVs) [
1,
2]. Lithium-ion batteries have become the most promising choice for EVs due to their high energy density and long cycle life [
3,
4]. For EV applications, battery management systems (BMSs) are necessary to prevent Li-ion batteries from overheating and overcharging and avoid potential thermal runaway. Currently, BMSs cannot store and process large amounts of data while managing the battery’s state of charge (SOC), voltage, and temperature in real time [
5,
6,
7]. To address this shortcoming, additional research is needed to develop reduced-order models (ROM) that can both model complex battery mechanisms and provide real-time management data. Applications of machine learning (ML) and artificial intelligence (AI) are fertile areas for eventual solutions to this problem.
Models that describe battery dynamic processes at all levels are not feasible. Therefore, mechanistic battery models, referred to as full-order models (FOMs), need to be tailored to specific purposes that require a deep understanding of a particular aspect of the battery’s operation and performance. Many mechanistic models have been developed specifically to describe battery thermal behavior [
8,
9,
10,
11,
12]. In general, models for analysis and diagnosis purposes employ detailed simulations of the battery’s physics and, thus, are often multidimensional, multiphysics models and are computationally slow. Models for control and optimization applications are usually computationally fast, but provide a limited description of the underlying physics. The most commonly used mechanistic model for single-battery cells is a lumped parameter simplification of a FOM called the pseudo-two-dimensional (P2D) model. Even given P2D simplifications of battery homogeneity and a constant electrode thickness, P2D models still use more than fifteen parameters specific to a particular battery and their computational cost is still too high for control and optimization applications. On the other hand, P2M parameters are too lumped to provide much insight into the underlying phenomena [
13,
14]. Decades of research have been conducted to develop reduced-order models (ROMs) that adequately retain the robustness of FOMs without excessive computational complexity. The state of the art for the various methods of achieving Li-ion battery ROMs has recently been reviewed in the literature [
15,
16]. We limit our following discussion of such methods to equivalent circuit models (ECMs), their model-based extensions, and the single-particle model approximation. These methods are most pertinent since our ROM, developed in the following sections, is a single-particle application and is most likely to be used instead of or alongside an ECM.
ECMs that do not consider fundamental physics have been extensively used to imitate the relationships between battery input and output systems while offering real-time computation [
17,
18,
19,
20,
21,
22]. ECMs use electrical circuits to simulate lithium-ion cells utilizing capacitors to shape the battery capacity, while variable resistors and controlled-voltage sources shape the temperature effect or SOC variations. Black-box modeling is another extensively applied method to provide real-time computation. It relies on developing an equivalent transform function with different inputs and outputs. Like ECMs, this method depends on experimental data for a specified battery [
23]. ECMs and transform functions are generally implemented in a “mixed approach” along with thermal and aging models, as shown in
Figure 1 [
24].
Model-based methods have been developed that have greatly enhanced the basic ECM. Some of the predominant model-based methods have been recently reviewed in the literature including the Luenberger, sliding mode, Kalman filter, and proportional integral (PIO) methods [
25,
26,
27,
28,
29,
30]. Model-based methods have a battery model at their core that uses measured current and voltage signals to provide a closed-loop estimation method. These methods typically use static models where model parameters are applied offline and assumed to not change over time. However, these models often do not ensure sufficient accuracy over a broad range of operation conditions and long time frames. In light of this, efforts have been made towards online model adaptation methods, including population-based optimization, dual filtering, and least squares (LS)-based methods such as moving window LS, continuous-time LS, and recursive least squares (RLS) [
31,
32,
33].
Lithium iron phosphate (LiFePO
4) is the most frequently used phosphate-based cathode material in Li-ion batteries. LiFePO
4 has a strong tendency to separate into solid high-Li+-concentration and low-Li+-concentration phases, leading to the battery’s characteristic broad voltage plateau at room temperature [
34,
35,
36,
37,
38,
39]. Traditionally, mathematical models of intercalation dynamics in LiFePO
4 cathodes were based on spherical diffusion or the shrinking core concept [
40,
41,
42]. However, recent experimental and theoretical progress suggests that a more realistic SPM should encompass a phase field model for equilibrium and nonequilibrium solid-solution transformations [
43,
44,
45,
46,
47]. A phase-field model is a computational method for modeling morphological and microstructure evolution in materials. They have been proposed for solid-state phase transformations, grain growth and coarsening, microstructure evolution in thin films, and crack propagation [
48,
49,
50,
51]. Research is currently underway that seeks to bridge the gap between phase-field mesoscale models and macro battery properties. For example, (Yuan et al. [
52], 2021) recently used a phase field modeling approach to develop a physics-based, fully coupled model that bridges dendrite and crack propagation at the micro level with macrostate battery charging and discharging [
53]. Another application (Zeng & Bazant [
54], 2013) demonstrated a method for estimating the voltage plateau of LiFePO
4 batteries based on the Cahn–Hilliard phase field model solution for a single cathode particle. Our ROM was motivated by (Zeng & Bazant, 2013), and the spatial mass transfer elements of our 3-D COMSOL® Multiphysics finite element solution are similar to their 1-D, isotropic, and isothermal solution. The major enhancement of our single-particle model (SPM) is that it is a multiphysics thermal model that fully couples the battery cell’s heat transfer model. Statistically, we relate the SPM simulation to battery cell property estimation. Specifically, the plateauing effect of the battery’s voltage response at higher ambient temperatures and the apparent diffusion-controlled behavior at lower temperatures are related to the SPM by statistical inference. Our SPM is a specific example of a widely used method for order reduction in P2D based on a single-particle model that aims to enhance computational run time while retaining elements of the underlying physics, as opposed to an ESM [
55,
56]. In the single-particle thermal model preparation, the local potential and concentration gradients in the electrolyte phase were ignored and accounted for by utilizing a lumped solution resistance term. Likewise, the potential gradient in the solid phase of the electrodes was dismissed, and the porous electrode was considered as a large number of individual particles, all subjected to the same conditions. These assumptions are generally only valid under relatively low current rates and the SPM is not recommended for high-power applications, such as fast EV charging and operations involving high-power pulses, but it is well-suited to daily EV driving, where the operating ranges are less extreme. These shortcomings of the SPM are not prohibitive for our ROM since we did not attempt to model the battery voltage response by directly scaling up the SPM, but sought to only retain enough information from the SPM to make statistical inferences concerning the macro battery properties. The ROM was realized by subjecting the raw simulation results from the COMSOL
® Multiphysics simulation data to principal component analysis (PCA) to determine the lowest-order simulation dataset capable of fitting the experimental data using deep neural network (DNN) regression. We validated our SPM based on available experimental data for the A123 Systems 26650 2.3 Ah battery [
57].
3. Results and Discussion
As shown in
Figure 7, the DNN is a simple feed forward neural network (FNN) with nine hidden layers, consisting of five linear layers and four elementwise scaled exponential linear layers (SELU). The DNN has a rank five vector input for training and a scaler output. The residual plot and error report for the predicted and experimental values are also shown in
Figure 7. The important things to note in the error report for the trained DNN predictor function is the regression correlation coefficient and the speed of the processing of examples in this case on a desktop computer CPU. We tested and verified the DNN for a 1 C discharge rate for ambient temperatures ranging from 253 to 298 K, as shown in
Figure 9. Also, in
Figure 9, the model results are compared to the experimental results for discharge rates ranging from 6.8 to 20.5 C for an ambient temperature of 298 K [
65].
We tested the DNN predictor function using the road test: Up Mount Sano in Huntsville, AL [
66]. This is an extreme road test and we had to input a moving average of the current data.
Figure 10 shows the DNN fit for the road test data for 15, 30, and 60 second update times for the moving average. Longer update time on the order of 60 seconds would be necessary for updating the SPM. If shorter than 15 seconds updating is necessary it would be necessary to modify the DNN at the expense of computation complexity perhaps requiring on-board GPU capability.
Figure 9.
(Top): Voltage response of DNN for temperature range 253–298 K and 1 C discharge. (Bottom): Thermal model validation for fast discharge at ambient temperature of 298 K.
Figure 9.
(Top): Voltage response of DNN for temperature range 253–298 K and 1 C discharge. (Bottom): Thermal model validation for fast discharge at ambient temperature of 298 K.
Figure 10.
Onboard DNN predictor function testing for road test: “Up Mount Sano in Huntsville, AL” for 15, 30 and 60 second updating.
Figure 10.
Onboard DNN predictor function testing for road test: “Up Mount Sano in Huntsville, AL” for 15, 30 and 60 second updating.
Author Contributions
Conceptualization, R. Painter; methodology, R. Parthasarathy, R. Painter; formal analysis, R. Painter.; investigation, R. Painter; resources, L. LI, L. Sharpe, S., Keith Hargrove data curation, R. Painter; writing—original draft preparation, R. Painter; writing—review and editing, R. Parthasarathy, R. Painter; visualization, R. Painter.; supervision, L. Li, L. Sharpe, S. Keith Hargrove; project administration, L. Li, L. Sharpe, S. Keith Hargrove.; funding acquisition, L. Li, L. Sharpe, S. Keith Hargrove. All authors have read and agreed to the published version of the manuscript.