Rational design of novel electrochemical energy storage systems with flexible designs, cheaper prices and more efficiency to meet the power storage needs of everything from handheld gadgets to electric cars heavily relies on the availability of advanced experimental and computational tools. One of the emerging computational tools in the discovery and design of materials is the phase field method. It is widely used for describing phase transformations and kinetics of microstructural evolution in materials sciences. One of its features is the diffuse interface, i.e. a region of space where two (or more) phases are assumed to mix. For electrochemical systems, the interface as the reacting zone plays a very important role. The diffusive nature of the electrical double layer across the electrode-electrolyte interface makes it more suitable for a description with phase field.

In this work, the phase field method is employed to study the kinetics of intercalation. The classical and the finite interface dissipation (FID) phase field methods are used. With the former, a systematic assumption of a linear temperature vs. concentration phase diagram for modeling the electrode-electrolyte coexistence is found to work well for higher partitioning coefficient. It was found that the rate constant is an exponential function of the partitioning coefficient. Moreover, it is possible to see that the activation energy required for intercalation is lower than the activation energy for de-intercalation, which is in agreement with both experiments and atomistic calculations. This work emphasizes on the non-equilibrium behavior especially at the beginning of interaction between electrode particles and electrolyte, with slow evolution of equilibrium. This was investigated using the FID model. One of its pivotal flux contributions is permeation which is caused by chemical potential difference across the interface. It is scaled by a material parameter dubbed “permeability”, which was originally estimated by the interdiffusion coefficient. A new approach to estimate this quantity for non-equilibrium electrochemistry is formulated based on the Butler-Volmer kinetics and its estimation from electrochemical measurement systems such as cyclic voltammetery and electrochemical impedance spectroscopy is shown. The simulation results on the influence of size, morphology and distribution of active particles on the kinetics of intercalation will be discussed. Furthermore, industrial exploitation of the simulation results for reverse engineering of electrode materials for high performance batteries will be described.