Silica–silane coupling agent interphase properties using molecular dynamics simulations

In this paper, strength of the interphase between silica and glycidoxypropyltrimethoxy silane (GPS) coupling agent has been studied using molecular dynamics (MD) simulations. Silica–GPS interphase model is created by coupling the hydroxylated silica surface with monolayer-hydroxylated GPS molecules. The interphase model is subjected to mode-I (normal), mode-II (shear) and mixed-mode (normal–shear) mechanical loading to determine the interphase cohesive traction–separation (T–S) response (i.e., cohesive traction law). In MD simulations, atomic interactions are modeled with the reactive force field ReaxFF. Effects of interphase thickness and GPS bond density on the T–S response are studied. Simulation results indicate that interphase strength decreases with increase in the interphase thickness before attaining a plateau level at higher thickness. For a particular thickness, strength improves significantly with increase in the GPS bond density with the silica surface. Damage mode is adhesive at the silica interface at lower thickness and transitions to mixed mode and cohesive failure within the silane interphase at higher thickness. Mixed-mode T–S responses are bounded by the mode-I and mode-II responses. Characteristic parameters of the continuum-level potential-based cohesive zone model (PPR–CZM) are determined by fitting the MD-based mode-I and mode-II T–S responses with PPR–CZM functional. Development of the PPR–CZM parameters enables bridging length scales from the MD to the continuum scale for fracture modeling of the fiber–matrix interphase in composites subjected to mixed-mode loading. Results on mode-I and mode-II unloading are also presented.