Stress-Induced Intercalation Instability

We present a linear stability analysis to demonstrate that a flat coherent phase boundary formed by the (de)intercalation of solutes into a compound is unstable against perturbations with wavelengths larger than a critical wavelength. This critical wavelength is controlled by the competition between the interface energy and the elastic strain energy caused by the misfit between the solute-rich and solute-poor phases. It increases with the distance between the phase boundary and free surface of the compound, and so the instability is most pronounced when the boundary is close to the surface at the early stage of the (de)intercalation process. Numerical calculations show that such instability leads to non-uniform intercalation behavior. We find that uniform intercalation cannot be achieved unless the phase boundary moves at a speed greater than a critical velocity. Estimate of the magnitude of this velocity suggests that the stress-induced intercalation instability is generally operative in intercalation compounds used for battery applications.