Influence of dispersion states on the performance of polymer-based nanocomposites

Although nanoparticle-modified polymers have tremendous promise in many applications, particularly dielectric energy storage, true nanoscale dispersion is extremely difficult to achieve. In this paper, we carefully engineer various dispersion states of titania nanoparticles in polyvinylidene fluoride and analyze their impact on dielectric behavior and energy storage ability. In particular, we compare nanocomposites prepared using commercially available nanoparticles to those we prepared using in situ and ex situ synthesis of nanoparticles. SEM and TEM studies showed that the in situ case leads to the best dispersion. Interestingly, dielectric permittivity was most influenced by dispersion state where the in situ case showed a higher increase, however, dielectric breakdown and energy storage density were less affected by dispersion and more affected by procedure that minimized residues and impurities. The in situ technique, in particular, showed nanoscale dispersion, low dielectric loss and higher energy storage density. In terms of mechanical behavior, all three cases showed a similar performance in the rubbery region, whereas the impact of dispersion was more pronounced in the glassy region. In fact, the trend was opposite to the dielectric permittivity where nanoscale dispersion resulted in a lower storage modulus likely due to the lower effective mechanical load transfer going to the nanoscale. The results of our study shed some light on the role of dispersion quality and processing techniques in affecting the final dielectric, mechanical and breakdown behavior of TiO2-based polymer nanocomposites.