Classification of the Crystal Structures of Orthosilicate Cathode Materials for Li-Ion Batteries by Artificial Neural Networks

Abstract

The crystal structures of orthosilicate cathode materials play a critical role in determining the physical and chemical properties of Li-ion batteries. Accurate predictions of these crystal structures are essential for estimating key properties of cathode materials in battery applications. In this study, we utilized crystal structure data from density functional theory (DFT) calculations, sourced from the Materials Project, to predict monoclinic and orthorhombic crystal systems in orthosilicate-based cathode-based materials with Li-Si-(Fe, Mn, Co)-O compositions. An artificial neural network (ANN) model with a 6-22-22-22-1 architecture was trained on 85% of the data and tested on the remaining 15%, achieving an impressive accuracy of 97.3%. The model demonstrated strong predictive capability, with only seven misclassifications from 267 datasets, highlighting its robustness and reliability in predicting the crystal structure of orthosilicate cathodes. To enhance interpretability and model reliability, we employed the Index of Relative Importance (IRI) to identify critical features influencing predictions. Additionally, a user-friendly graphical user interface was also developed to facilitate rapid predictions, enabling researchers to explore structural configurations efficiently and accelerating advancements in battery materials research.