Abstract
Non-equilibrium phase transformation and effect of interfacial Li flux on miscibility gap in two-phase transformation of LiFePO4 have been explored in this study. Our previously developed “Mushy-Zone” (MZ) model, accounting for sluggish Li diffusion across the two-phase interface, has been employed to study the non-equilibrium phase transformation in LiFePO4 materials of Li-ion batteries. Phase transformation rate, variation of two-phase miscibility gap, and interfacial Li composition profiles have been studied for different particle shapes at varying discharge rates. Sluggish Li flux across the two-phase interface, which is believed to be the origin of the kinetically-induced non-equilibrium phase transformation, has been calculated to explain the obtained results. It is found that small particle sizes (radii of 20 nm) and slow discharge rates tend to create homogenous phase transformation (i.e., shrunk or no miscibility gap). Two-phase transformation is remarkably delayed for spherical particles at low discharge rates, leading to a lower capacity compared to that of plated-shaped particles. However, at higher discharge rates spherical particles show better capacity.
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