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  1. Free, publicly-accessible full text available January 1, 2023
  2. Introduction of nanoparticulate additives can dramatically impact elastomer mechanical response, with large enhancements in modulus, toughness, and strength. Despite the societal importance of these effects, their mechanistic origin remains unsettled. Here, using a combination of theory and molecular dynamics simulation, we show that low-strain extensional reinforcement of elastomers is driven by a nanoparticulate-jamming-induced suppression in the composite Poisson ratio. This suppression forces an increase in rubber volume with extensional deformation, effectively converting a portion of the rubber's bulk modulus into an extensional modulus. A theory describing this effect is shown to interrelate the Poisson ratio and modulus across a matrix of simulated elastomeric nanocomposites of varying loading and nanoparticle structure. This model provides a design rule for structured nanoparticulates that maximizes elastomer mechanical response via suppression of the composite Poisson ratio. It also positions elastomeric nanocomposites as having a qualitatively different character than Poisson-ratio-matched plastic nanocomposites, where this mechanism is absent.
  3. Please see the paper deposited
  4. Coupling agents are intended to promote filler dispersion by providing a bridge between the filler and the rubber phase. This study investigated the ability of a novel physical coupling agent, poly(butadienegraft-pentafluorostyrene) in a mixture with polypentafluorostyrene, to improve rubber-filler interactions and suppress filler-filler networking in carbon-black-reinforced styrene-butadiene rubber (SBR), and thereby decrease hysteresis. The electron-rich aromatic rings of carbon black are involved in areneperfluoroarene interactions with the electron-poor pentafluorostyrene aromatic rings of the coupling agent. The SBR chains in the rubber compound have an affinity for the polybutadiene backbone of the coupling agent. The interactions between carbon black and the coupling agent were analyzed using Raman spectroscopy, transmission electron microscopy, zeta potential measurements, surface area measurements, and scanning electron microscopy. Filler flocculation analysis showed that the coupling agent improves the dispersion and lowers the energy of dissipation. The hysteresis loss, quantified in terms of loss tangent values at 60 C, was reduced by up to 12% due to the coupling agent's promotion of better filler-rubber interactions. The influence of the PPFS graft length was also studied.