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Materials Science at Oregon State University

Phase Field Modeling of Intercalation Kinetics: a Finite Interface Dissipation Approach

Date: Thursday, Apr 7th
Presenter: Dr. Nega Alemayehu,

Abstract


One of the major challenges for the success of many clean energy technologies is energy storage. Intercalation electrode materials are promising for electrochemical energy storage. 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 non-equilibrium behavior especially at the beginning of interaction between electrode particles and electrolyte, with slow evolution of equilibrium, was investigated using the Finite Interface Dissipation 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 called “permeability of the interface”, which was originally estimated by the interdiffusion coefficient for diffusion couples. A new way 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 discussed. An investigation of the influence of geometry and size on the kinetics of intercalation of Li storage particles was performed. It was found that the rate of intercalation relies exponentially on the size of particles. Moreover, particles with high eccentricity and uniform arrangements show faster kinetics of intercalation. Furthermore, potential future applications for this model will be discussed.