Diamond nanothread reinforced polymer composites: Ultra-high glass transition temperature and low density

Diamond nanothread (DNT), a novel carbon-based nanomaterial exhibiting ultra-light density and outstanding mechanical properties, has attracted intensive attentions in polymer composites. This study investigates the influences of DNT on the glass transition temperature (T_g) of poly (methyl methacrylate) (PMMA) composites and reveals the glass-rubber transition mechanism through molecular dynamics simulation. We demonstrates that DNT exhibits better improvement than other carbon-based nanomaterials in enhancing the T_g of PMMA composite, suggesting that DNT is a promising reinforcement for polymer nanocomposite with higher service temperature and better mechanical performances. Significantly, we find that interfacial interactions including van der Waals interaction and mechanical interlocking play an important part in glass transition of PMMA composite. The transition from glassy state to rubbery is induced through the interfacial debonding brought by the enlargement of free volume at the interface. According to the interfacial degrading mechanism, cross links between DNT reinforcement and PMMA chains are introduced to provide bidirectional hindrance for free motions of polymer chains, resulting in a 70 K enhancement of T_g of PMMA composites. These findings not only shed light to the prospective application of DNT in advanced nanocomposite, but also provide important guidance to improve the reinforcing efficiency of nanomaterials in engineering application, such as building and aerospace industry.