Abstract
Silicon is novel Li-ion battery anode chemistry with exceptional theoretical energy densities. However, this alloying material has significant challenges with non-passivating solid-electrolyte interface (SEI) formation and significant chemo-mechanics issues. These issues have been studied extensively at the particle-level. However, extensive SEI formation and dynamic particle chemo-mechanics need to be accounted for when designing the overall electrode microstructure. For example, Si particle expansion can result in electrolyte pore-closure. During charging (Si lithiation), Si particles near the separator lithiate faster than Si near the current-collector. Thus, Si particles near the separator begin to expand faster and close-off electrolyte access to particles near the current collector. This heterogeneous through-plane lithiation then results in low overall electrode utilization, especially at high rates (i.e.,>1 C). The “choking off” effect is a result of a strong feedback between heterogeneous lithiation, Si expansion, and electrolyte pore closure.To aid in Si electrode design and account for dynamic particle expansion/contraction, the standard pseudo-2D battery model is reformulated to account for finite-strain chemo-mechanics. This model explores the trade-offs between initial electrode porosity, electrode thickness, rate-capability, and external pressure. Additionally, the model implements simplified SEI growth dynamics to explore how SEI growth effects should be accounted for in electrode design.The Figure illustrates polarization responses for a 1C charge for a Si/NMC532 cell. The different colors indicate different initial anode porosities. As shown in Figure a, the low initial porosity cases results in significant polarization, but additional gains after 50% initial porosity are significantly diminished. These results are shown for an external pressure of 15 psi. Figure b illustrates the cell thickness as a function of time. As illustrated, the lower porosity case starts at a shorter initial thickness. For all cases, the cell thickness increases as Si lithiates/expands. Figure c illustrates the anode porosity at the cut-off voltage as a function of anode thickness. As shown, the lower initial porosity case has significant pore-closure on the right-side at the separator interface. The higher initial porosity cases have increased anode lengths because the Si utilization is improved due to the reduced pore-closer effects. The graphic illustrates the main features of the reformulated pseudo-2D battery model. Figure 1
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