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End date: 2020 × Start date: 2012 × DDC: 530 × Subject: Elastomers ×

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    Local chain deformation and overstrain in reinforced elastomers: An NMR study
    (Washington, DC : American Chemical Society, 2013) Pérez-Aparicio, R.; Schiewek, M.; Valentín, J.L.; Schneider, H.; Long, D.R.; Saphiannikova, M.; Sotta, P.; Saalwächter, K.; Ott, M.
    A molecular-level understanding of the strain response of elastomers is a key to connect microscopic dynamics to macroscopic properties. In this study we investigate the local strain response of vulcanized, natural rubber systems and the effect of nanometer-sized filler particles, which are known to lead to highly improved mechanical properties. A multiple-quantum NMR approach enables the separation of relatively low fractions of network defects and allows to quantitatively and selectively study the local deformation distribution in the strained networks matrix on the microscopic (molecular) scale. We find that the presence of nondeformable filler particles induces an enhanced local deformation of the matrix (commonly referred to as overstrain), a slightly increased local stress/strain heterogeneity, and a reduced anisotropy. Furthermore, a careful analysis of the small nonelastic defect fraction provides new evidence that previous NMR and scattering results of strained defect-rich elastomers cannot be interpreted without explicitly taking the nonelastic defect fraction into account.
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    Quantifying Rate-and Temperature-Dependent Molecular Damage in Elastomer Fracture
    (College Park, Md. : APS, 2020) Slootman, Juliette; Waltz, Victoria; Yeh, C. Joshua; Baumann, Christoph; Göstl, Robert; Comtet, Jean; Creton, Costantino
    Elastomers are highly valued soft materials finding many applications in the engineering and biomedical fields for their ability to stretch reversibly to large deformations. Yet their maximum extensibility is limited by the occurrence of fracture, which is currently still poorly understood. Because of a lack of experimental evidence, current physical models of elastomer fracture describe the rate and temperature dependence of the fracture energy as being solely due to viscoelastic friction, with chemical bond scission at the crack tip assumed to remain constant. Here, by coupling new fluorogenic mechanochemistry with quantitative confocal microscopy mapping, we are able to quantitatively detect, with high spatial resolution and sensitivity, the scission of covalent bonds as ordinary elastomers fracture at different strain rates and temperatures. Our measurements reveal that, in simple networks, bond scission, far from being restricted to a constant level near the crack plane, can both be delocalized over up to hundreds of micrometers and increase by a factor of 100, depending on the temperature and stretch rate. These observations, permitted by the high fluorescence and stability of the mechanophore, point to an intricate coupling between strain-rate-dependent viscous dissipation and strain-dependent irreversible network scission. These findings paint an entirely novel picture of fracture in soft materials, where energy dissipated by covalent bond scission accounts for a much larger fraction of the total fracture energy than previously believed. Our results pioneer the sensitive, quantitative, and spatially resolved detection of bond scission to assess material damage in a variety of soft materials and their applications. © 2020 authors. Published by the American Physical Society.