Abstract
In current paper, we demonstrated that molecular dynamics and glass transition of rubber can be controlled by constructing attractive interface between rubber matrix and fillers. Based on a combination of experiments and molecular simulations, it was revealed that interfacial segmental mobility was reduced and glass transition temperatures (Tgs) of epoxidized natural rubber (ENR) were significantly improved due to in situ polymerization of zinc dimethacrylate (ZDMA). During curing, ZDMA polymerizes in rubber matrix, resulting in the appearance of nanodispersion phases of poly-ZDMA (PZDMA). It was demonstrated that coordination interaction exists between epoxy groups and PZDMA in interfacial regions. Furthermore, using dynamic Monte Carlo simulations, it was observed that the interfacial regions that have highest content of epoxy groups exhibit lowest segmental mobility. Then, the increase of ZDMA content leads to the rise of the fraction of absorbed interfacial segments, and thus the Tgs of filled rubbers are improved.
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