Generative AI-Driven Discovery of Next-Generation Electrolytes for Alkali Metal Batteries.

Recent advances in artificial intelligence (AI) are revolutionizing materials science by unlocking unprecedented capabilities in designing novel compounds and accurately predicting their properties. Among these, graph-based machine learning (ML) algorithms have garnered significant attention for their ability to capture complex atomic interactions and use them as effective descriptors. In this study, we integrated state-of-the-art generative AI (Gen AI) and ML techniques with quantum mechanical calculations to discover novel next-generation electrolytes for alkali metal batteries. We developed a Generative Adversarial Network (GAN) framework incorporating a graph-based generator and discriminator models to generate novel electrolyte candidates. The GAN model was trained on a subset of approximately 1 million molecules from the GDB-11 database, which enabled the generation of 30,000 unique and chemically valid molecules. Concurrently, a Message Passing Neural Network (MPNN) model was trained for property prediction by utilizing the QM9 dataset. Using the trained MPNN model, we predicted the properties of the newly generated molecules and screened the candidates based on the criteria of negative standard enthalpy of formation and a wide HOMO-LUMO gap. First-principles density functional theory (DFT) calculations were conducted for additional screening and to evaluate key thermodynamic and electrochemical properties, including standard enthalpy of formation, oxidation potential, and reduction potentials. Finally, a set of 26 promising candidates was acquired with outstanding electrochemical characteristics. Our findings demonstrate the potential of AI-driven approaches to discover high-performance, stable, and efficient electrolytes as promising alternatives to conventional organic electrolytes for next-generation energy storage systems.