Meso‐Scale Modeling of Glide Phase Transformations in Layered Intercalation Compounds

ABSTRACT Many layered intercalation compounds undergo a series of structural phase transformations during the insertion of guest ions that result in a change in stacking sequence within their 2D building blocks. From the crystallographic viewpoint, a change in stacking sequence can be achieved through glide of such 2D building blocks. Glide transformations are especially common in layered Na intercalation compounds, such as and , where is one or any combination of transition metals. While these compounds are promising electrode materials for Na‐ion batteries, the mechanical damage that arises during a glide phase transformation prevents their widespread use in current battery technology. A fundamental understanding of the mechanisms with which glide phase transformations occur is necessary to overcome the degradation accompanying the electrochemical cycling of layered Na intercalation compounds. In this contribution, we develop a chemo‐mechanical model of glide phase transformations that explicitly treats the unique anisotropic cohesive properties of layered intercalation compounds at the meso‐scale. The model is capable of predicting the nucleation and growth of new stacking sequences due to fluxes of intercalating guest ions and the formation of partial dislocations that separate coherently coexisting phases having different stacking sequences.