Discovery of novel Li SSE and anode coatings using interpretable machine learning and high-throughput multi-property screening

All-solid-state batteries with Li metal anode can address the safety issues surrounding traditional Li-ion batteries as well as the demand for higher energy densities. However, the development of solid electrolytes and protective anode coatings possessing high ionic conductivity and good stability with Li metal has proven to be a challenge. Here, we present our informatics approach to explore the Li compound space for promising electrolytes and anode coatings using high-throughput multi-property screening and interpretable machine learning. To do this, we generate a database of battery-related materials properties by computing Li+ migration barriers and stability windows for over 15,000 Li-containing compounds from Materials Project. We screen through the database for candidates with good thermodynamic and electrochemical stabilities, and low Li+ migration barriers, identifying promising new candidates such as Li9S3N, LiAlB2O5, LiYO2, LiSbF4, and Sr4Li(BN2)(3), among others. We train machine learning models, using ensemble methods, to predict migration barriers and oxidation and reduction potentials of these compounds by engineering input features that ensure accuracy and interpretability. Using only a small number of features, our gradient boosting regression models achieve R-2 values of 0.95 and 0.92 on the oxidation and reduction potential prediction tasks, respectively, and 0.86 on the migration barrier prediction task. Finally, we use Shapley additive explanations and permutation feature importance analyses to interpret our machine learning predictions and identify materials properties with the largest impact on predictions in our models. We show that our approach has the potential to enable rapid discovery and design of novel solid electrolytes and anode coatings.

Automated summary

This study presents an informatics approach using high-throughput screening and machine learning to explore the Li compound space for solid electrolytes and anode coatings, identifying promising candidates and predicting their performance using machine learning models. The approach shows potential for rapid discovery and design of novel battery materials.