Searching for Mechanically Superior Solid-State Electrolytes in Li-Ion Batteries via Data-Driven Approaches

Abstract

Li-ion solid-state electrolytes (SSEs) have great potential, but their commercialization is limited due to interfacial contact stability issues and the formation and growth of dendrites. In this study, a machine learning regression algorithm was implemented to screen for mechanically superior SSEs among 17,619 candidates. Elasticity information (14,238 structures) was imported from an available database, and their machine learning descriptors were constructed using physiochemical and structural properties. A surrogate model for predicting the shear and bulk moduli exhibited R-2 values of 0.819 and 0.863, respectively. The constructed model was applied to predict the elastic properties of potential SSEs, and first-principles calculations were conducted for validation. Furthermore, the application of an active learning process, which reduced the prediction uncertainty, was clearly demonstrated to improve the R-2 score from approximately 0.6-0.8 by adding only 32-63% of new data sets depending on the type of modulus. We believe that the current model and additional data sets can accelerate the process of finding optimal SSEs to satisfy the mechanical conditions being sought.