Unveiling State-of-Charge Effects on Elastic Properties of LiCoO2 via Deep Learning and Empirical Models

Abstract

This study investigates the mechanical properties of LiCoO2 (LCO) cathode materials under varying states of charge (SOCs) using both an empirical Buckingham potential model and a machine learning-based Deep Potential (DP) model. The results reveal a substantial decrease in Young's modulus with decreasing SOC. Analysis of stress factors identified pairwise interactions, particularly those involving Co3+ and Co4+, as key drivers of this mechanical evolution. The DP model demonstrated superior performance by providing consistent and reliable predictions reflected in a smooth and monotonic stiffness decrease with SOC, in contrast to the large fluctuations observed in the classical Buckingham potential results. The study further identifies the increasing dominance of Co4+ interactions at low SOCs as a contributor to localized stress concentrations, which may accelerate crack initiation and mechanical degradation. These findings underscore the DP model's capability to capture SOC-dependent mechanical behavior accurately, establishing it as a robust tool for modeling battery materials. Moreover, the calculated SOC-dependent mechanical properties can serve as critical input for continuum-scale models, improving their predictive capability for chemo-mechanical behavior and degradation processes. This integrated multiscale modeling approach can offer valuable insights for developing strategies to enhance the durability and performance of lithium-ion battery materials.