Leveraging high-throughput molecular simulations and machine learning for the design of chemical mixtures

Mixtures of chemical ingredients, such as formulations, are ubiquitous in materials science, but optimizing their properties remains challenging due to the vast design space. Computational approaches offer a promising solution to traverse this space while minimizing trial-and-error experimentation. Using high-throughput classical molecular dynamics simulations, we generated a comprehensive dataset of over 30,000 solvent mixtures to evaluate three machine learning approaches that connect molecular structure and composition to property: formulation descriptor aggregation (FDA), formulation graph (FG), and Set2Set-based method (FDS2S). Our results demonstrate that our new FDS2S approach outperforms other approaches in predicting simulation-derived properties. Formulation-property relationships can reveal important substructures and identify promising formulations at least two to three times faster than random guessing. The models show robust transferability to experimental datasets, accurately predicting properties across energy, pharmaceutical, and petroleum applications. Our research demonstrates the utility of high-throughput simulations and machine learning tools to design formulations with promising properties.