Exploiting Synergistic Experimental and Computational Approaches to Design and Fabricate High-Performance Elastomer

Silicone elastomers (SRs) are of great scientific and technological importance due to their resistance to low temperatures. However, the glass transition temperature (Tg) of existing SRs is not low enough to satisfy its utilization in the extremely low-temperature environment. Meanwhile, crystallization often occurs at the low-temperature, making it difficult for SRs to maintain their original properties in the extremely low-temperature environment. Here, by combining molecular dynamics (MD) simulation and experiment, a novel low-temperature resistance and crystalline-free SR (Epoxidized-Methyl-Ethyl-Vinyl Silicone Elastomer, also referred to E-MEVQ) is fabricated by random copolymerization of three different siloxane repeat units (dimethyl-siloxane, diethyl-siloxane and methyl-epoxy-siloxane). We showed that the Tg of E-MEVQ computed from MD simulations using three different methods (specific volume, nonbond potential energy and conformational transition versus temperature) agrees well with that of the as-synthesized E-MEVQ determined by Differential Scanning Calorimetry. The Tg is approximately -130 °C, much lower than that of Polydimethylsiloxane (PDMS), and the E-MEVQ is in the amorphous state without any crystallization. This novel silicone elastomer is expected to be widely applied in the field of smart devices, sensors, and medical equipment under extreme situations. Our work also provides a promising framework for designing and fabricating high-performance elastomeric polymer materials via simulation and experiment.