Modeling of Lithiation in Silicon Electrodes

Energy is the lifeblood of modern society. Lithium-ion batteries are critically important for portable electronics, electric vehicles, and grid-level energy storage. Silicon is a promising high-capacity electrode material for next-generation lithium-ion batteries. However, it is prone to electrochemically induced mechanical degradation that can consume active lithium and result in fast capacity fade. In this chapter, we present the continuum and atomistic models of deformation and stress generation during electrochemical lithiation of silicon particles and thin films. The associated simulation results are compared with in situ and ex situ experiments, thus providing insights into electrochemically driven mechanical degradation in silicon electrodes.