Design of Co‐Cured Multi‐Component Thermosets with Enhanced Heat Resistance, Toughness, and Processability via a Machine Learning Approach

Abstract Designing heat‐resistant thermosets with excellent comprehensive performance has been a long‐standing challenge. Co‐curing of various high‐performance thermosets is an effective strategy, however, the traditional trial‐and‐error experiments have long research cycles for discovering new materials. Herein, a two‐step machine learning (ML) assisted approach is proposed to design heat‐resistant co‐cured resins composed of polyimide (PI) and silicon‐containing arylacetylene (PSA), that is, poly(silicon‐alkyne imide) (PSI). First, two ML prediction models are established to evaluate the processability of PIs and their compatibility with PSA. Then, another two ML models are developed to predict the thermal decomposition temperature and flexural strength of the co‐cured PSI resins. The optimal molecular structures and compositions of PSI resins are high‐throughput screened. The screened PSI resins are experimentally verified to exhibit enhanced heat resistance, toughness, and processability. The research framework established in this work can be generalized to the rational design of other advanced multi‐component polymeric materials.