Multiscale Investigation of the Diffusion Mechanism within the Solid–Electrolyte Interface Layer: Coupling Quantum Mechanics, Molecular Dynamics, and Macroscale Mathematical Modeling

The solid–electrolyte interface (SEI) layer has a critical role in Li-ion batteries' (LIBs) life span. The SEI layer, even in modern commercial LIBs, is responsible for more than 50% of capacity loss. Due to the inherent complexity in studying the SEI layer, many aspects of its performance and characteristics, including diffusion mechanisms in this layer, are unknown. As a result, most mathematical models use a constant value of the diffusion coefficient, instead of a variable formulation, to predict LIBs' properties and performance such as capacity fading and the SEI growth rate. In this work, by employing a multiscale investigation using a combination of quantum mechanics, molecular dynamics, and macroscale mathematical modeling, some equations are presented to evaluate the energy barrier against diffusion and the diffusion coefficient in different crystal structures in the inner section of the SEI layer. The equations are evaluated as a function of temperature and concentration and can be used to study the diffusion mechanism in the SEI layer. They can also be integrated with other mathematical models of LIBs to increase the accuracy of the latter.