Percolation to Jamming in Polymethylvinylsiloxane/Silica Nanocomposites

Researchers have conducted extensive experimental and theoretical studies on the jamming transition of colloidal and granular suspensions, but the existence and characteristics of jamming transition in nanoparticle-filled polymers remain elusive. In this work, two kinds of polymethylvinylsiloxane/silica nanocomposites were studied. A liquid-solid transition was found at the silica volume fraction of about 5 vol%, corresponding to the percolation of particle agglomerates. At higher silica content (about 10 vol%), a solid-solid transition was found in yield stress, equilibrium modulus, and the contact stress between agglomerates. The characteristic length of the particle network and inter-molecular distance also showed a transition at this transition. This transition corresponds to the simultaneous jamming of particles inside agglomerates and between agglomerates. This bi-level jamming behavior is distinct from the well-known jamming behavior in soft or hard particulate suspensions. Moreover, the dependence of the yield stress and equilibrium modulus on the distance to the jamming concentration differs from the simulations using simple interaction models like harmonic and Hertzian models. It implies that the interfacial viscoelastic layer may offer additional attractive and adhesive interactions between nanoparticles, which is critical in the jamming of polymer nanocomposites.