Accelerating Discovery of High Fractional Free Volume Polymers from a Data-Driven Approach

Abstract

As a fundamental structure characteristic in polymers, fractional free volume (FFV) plays an indispensable role in governing polymer properties and performance. However, the design of new high-FFV polymers is challenging. In this study, we report a data-driven approach and aim to accelerate the discovery of high-FFV polymers. First, a computational method is proposed to calculate FFV, and a two-step fragmentation method is developed to construct a fragment library for digital representation of polymer structures. Data mining is employed to identify promising fragments for high FFV. Subsequently, machine learning (ML) models are trained using a data set with 1683 polymers and their excellent transferability is demonstrated by out-of-sample predictions in another data set with 11,479 polymers. Finally, the ML models are used to screen ∼1 million hypothetical polymers, and 29,482 polymers with FFV > 0.2 are shortlisted; representative high-FFV polymers are validated by molecular simulations, and design strategies are highlighted. To further facilitate the discovery of new high-FFV polymers, we develop an online interactive platform https://ffv-prediction.herokuapp.com, which allows for rapid FFV predictions, given polymer structures. The data-driven approach in this study might advance the development of new high-FFV polymers and further explore quantitative structure-property relationships for polymers.