Using the recently developed Cahn-Hilliard reaction (CHR) theory, we present a simple mathematical model of the transition from solid-solution radial diffusion to two-phase shrinking-core dynamics during ion intercalation in a spherical solid particle. This general approach extends previous Li-ion battery models, which either neglect phase separation or postulate a spherical shrinking-core phase boundary under all conditions, by predicting phase separation only under appropriate circumstances. The effect of the applied current is captured by generalized ButlerVolmer kinetics, formulated in terms of the diffusional chemical potential in the CHR theory. We also consider the effect of surface wetting or de-wetting by intercalated ions, which can lead to shrinking core phenomena with three distinct phase regions. The basic physics are illustrated by different cases, including a simple model of lithium iron phosphate (neglecting crystal anisotropy and coherency strain).
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