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    Friction, abrasion and crack growth behavior of in-situ and ex-situ silica filled rubber composites
    (Basel : MDPI, 2020) Vaikuntam, Sankar Raman; Bhagavatheswaran, Eshwaran Subramani; Xiang, Fei; Wießner, Sven; Heinrich, Gert; Das, Amit; Stöckelhuber, Klaus Werner
    The article focuses on comparing the friction, abrasion, and crack growth behavior of two different kinds of silica-filled tire tread compounds loaded with (a) in-situ generated alkoxide silica and (b) commercial precipitated silica-filled compounds. The rubber matrix consists of solution styrene butadiene rubber polymers (SSBR). The in-situ generated particles are entirely different in filler morphology, i.e., in terms of size and physical structure, when compared to the precipitated silica. However, both types of the silicas were identified as amorphous in nature. Influence of filler morphology and surface modification of silica on the end performances of the rubbers like dynamic friction, abrasion index, and fatigue crack propagation were investigated. Compared to precipitated silica composites, in-situ derived silica composites offer better abrasion behavior and improved crack propagation with and without admixture of silane coupling agents. Silane modification, particle morphology, and crosslink density were identified as further vital parameters influencing the investigated rubber properties. © 2020 by the authors.
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    A nonequilibrium model for particle networking/jamming and time-dependent dynamic rheology of filled polymers
    (Basel : MDPI, 2020) Robertson, Christopher G.; Vaikuntam, Sankar Raman; Heinrich, Gert
    We describe an approach for modeling the filler network formation kinetics of particle-reinforced rubbery polymers—commonly called filler flocculation—that was developed by employing parallels between deformation effects in jammed particle systems and the influence of temperature on glass-forming materials. Experimental dynamic viscosity results were obtained concerning the strain-induced particle network breakdown and subsequent time-dependent reformation behavior for uncross-linked elastomers reinforced with carbon black and silica nanoparticles. Using a relaxation time function that depends on both actual dynamic strain amplitude and fictive (structural) strain, the model effectively represented the experimental data for three different levels of dynamic strain down-jump with a single set of parameters. This fictive strain model for filler networking is analogous to the established Tool–Narayanaswamy–Moynihan model for structural relaxation (physical aging) of nonequilibrium glasses. Compared to carbon black, precipitated silica particles without silane surface modification exhibited a greater overall extent of filler networking and showed more self-limiting behavior in terms of network formation kinetics in filled ethylene-propylene-diene rubber (EPDM). The EPDM compounds with silica or carbon black filler were stable during the dynamic shearing and recovery experiments at 160 °C, whereas irreversible dynamic modulus increases were noted when the polymer matrix was styrene-butadiene rubber (SBR), presumably due to branching/cross-linking of SBR in the rheometer. Care must be taken when measuring and interpreting the time-dependent filler networking in unsaturated elastomers at high temperatures.