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A theoretical investigation of the effects of elastic coherency on thethermodynamics, kinetics, and morphology of intercalation in single LiFePO4nanoparticles yields new insights into this important battery material.Anisotropic elastic stiffness and misfit strains lead to the unexpectedprediction that low-energy phase boundaries occur along {101} planes, whileconflicting reports of phase boundary orientations are resolved by a partialloss of coherency in the {100} direction. Elastic relaxation near surfacesleads to the formation of a striped morphology, whose characteristic lengthscale is predicted by the model and yields an estimate of the interfacialenergy. The effects of coherency strain on solubility and galvanostaticdischarge are studied with a reaction-limited phase-field model, whichquantitatively captures the influence of misfit strain, particle size, andtemperature on solubility seen in experiments. Coherency strain stronglysuppresses phase separation during discharge, which enhances rate capabilityand extends cycle life. The effects of elevated temperature and the feasibilityof nucleation are considered in the context of multi-particle cathodes.

Coherency strain and the kinetics of phase separation in LiFePO4