Effect of Cross-Link Density on Interphase Creation in Polymer Nanocomposites

The thermal and dynamic behavior of epoxy nanocomposites with varying cross-link density was tested via dynamic scanning calorimetry (DSC) in order to determine the influence of cross-link density on the creation of “interphase”, zones of altered polymer properties near polymer−particle interfaces. The results show that the inclusion of nanoparticles creates an increase in the glass transition temperature (Tg) at low cross-link density and a decrease in Tg at higher cross-link densities. This phenomenon suggests that two mechanisms work in tandem to alter the Tg of epoxy systems, with relative magnitudes determined by cross-link density: (1) network disruption at the nanotube−polymer interfaces leading to lower Tg and (2) interphase creation leading to retarded dynamics, resulting in higher Tg. Results show that as cross-link density increases, the length scale of cooperatively rearranging regions (CRRs) decreases. This decrease hinders communication of the dynamics between adjacent CRRs, thereby reducing...