Silicon is an ideal active material for lithium-ion battery anodes, due to its low potential and high theoretical capacity. However, extreme volume changes during lithiation and delithiation make reversibility and long cycle life difficult challenges. To properly understand these volume changes, a detailed electrochemical model is needed. Much previous modeling work has focused on particle-level effects such as intra-particle diffusion and cracking. Beyond this, some efforts have successfully utilized pseudo-2-dimensional (P2D) models to evaluate electrode-level phenomena — such as stress distribution and changes in electrode thickness and electrochemical potential. Nevertheless, some essential physics is still missing.Here, we present a new P2D model with improvements that provide a deeper level of understanding of porous silicon anode property changes during lithiation, to enable improved electrode design. Important among these improvements are the use of local state of lithiation as opposed to electrode average state of lithiation to better capture porosity and ionic conductivity changes; an effective electrolyte reservoir that properly addresses electrolyte volume-change requirements; advection of electrolyte and solid-state Li; and an extensive electrode-level plastic deformation model that has a dramatic effect on the model’s predictions.We use this model to test the efficacy of various electrode and cell design decisions. The model can make recommendations on casing design such as rigidity and thickness and the effect of other cell sandwich components e.g. different layers thickness on the electrochemical performance of the cell. Furthermore, using the revised swelling behavior predictions given by the mechanical model, we can provide recommendations for initial electrode porosity and binder volume fraction. Finally, the model as a whole allows us to provide recommendations that will accommodate particle expansion with the least detriment to ionic conductivity at various C-rates. Figure 1
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