Abstract
Automotive battery manufacturers are working to improve individual cell and overall pack design by increasing their performance, durability, and range, while reducing cost and active material volume change is one of the more complex aspects that needs to be considered during this process. To improve the balance between cost, stability, performance, and volume change behavior, some cell designers have introduced the use of multiple active materials within the same composite electrode. For example, LiMn2O4 (LMO) and LiNi1/3Co1/3Mn1/3O2 (NMC) active materials are both included in cathodes to benefit from this balance. In anodes, some designers have included both silicon and graphite to maximize gravimetric capacity while maintaining a tolerable degree of volume expansion to prevent damage to the cell and pack structure.While the inclusion of multiple active materials can be used to better tune electrode performance, stability, and volume change for specific applications, the modeling of these electrodes is significantly more complicated. Previously, Albertus et. al developed a model to account for multiple active materials within the same positive electrode.(1) Their model took the concept of a pseudo-two dimensional Li-ion cell model and incorporated multiple pseudo second-dimensions, which correlates to the radial direction of a theoretical active material particle. Therefore, they could account for each active material separately, where previously, an average particle radius, average film resistance, and average equilibrium potential would be assumed for the total electrode.In the study shown here, we build upon this modeling concept by incorporating our previously developed mechano-electrochemical equations to account for active material volume change.(2-5) Figure 1 shows an example of equilibrium potentials for two anode active materials as a function of lithiation fraction. The difference between these equilibrium potentials will dictate the preferential lithiation of the materials, and thus, the rate at which each material undergoes lithiation-based volume change. This allows for the simulation of volume change in diffusion-governed (high rate) or kinetic-governed (low rate) charge and discharge.The relationships between anode/cathode capacity, electrode voltages, and active material volume will be discussed. References P. Albertus, J. Christensen and J. Newman, Journal of The Electrochemical Society, 156, A606 (2009).T. R. Garrick, K. Higa, S.-L. Wu, Y. Dai, X. Huang, V. Srinivasan and J. W. Weidner, Journal of The Electrochemical Society, 164, E3592 (2017).T. R. Garrick, X. Huang, V. Srinivasan and J. W. Weidner, Journal of The Electrochemical Society, 164, E3552 (2017).T. R. Garrick, K. Kanneganti, X. Huang and J. W. Weidner, Journal of The Electrochemical Society, 161, E3297 (2014).D. J. Pereira, J. W. Weidner and T. R. Garrick, Journal of The Electrochemical Society, 166, A1251 (2019).D. J. Pereira, M. A. Fernandez, K. C. Streng, X. X. Hou, X. Gao, J. W. Weidner, and T. R. Garrick, Journal of The Electrochemical Society, 167, 080515 (2020). Figure 1. Equilibrium potential as a function of lithiation fraction for two anode active materials. Figure 1
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