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Sharing the Load: Stress Redistribution Governs Fracture of Polymer Double Networks.

ABSTRACT: The stress response of polymer double networks depends not only on the properties of the constituent networks but also on the interactions arising between them. Here, we demonstrate, via coarse-grained simulations, that both their global stress response and their microscopic fracture mechanics are governed by load sharing through these internetwork interactions. By comparing our results with affine predictions, where stress redistribution is by definition homogeneous, we show that stress redistribution is highly inhomogeneous. In particular, the affine prediction overestimates the fraction of broken chains by almost an order of magnitude. Furthermore, homogeneous stress distribution predicts a single fracture process, while in our simulations, fracture of sacrificial chains takes place in two steps governed by load sharing within a network and between networks, respectively. Our results thus provide a detailed microscopic picture of how inhomogeneous stress redistribution after rupture of chains governs the fracture of polymer double networks.

SUBMITTER: Tauber J

PROVIDER: S-EPMC8482750 | biostudies-literature | 2021 Sep

REPOSITORIES: biostudies-literature

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Sharing the Load: Stress Redistribution Governs Fracture of Polymer Double Networks.

Tauber Justin J Rovigatti Lorenzo L Dussi Simone S van der Gucht Jasper J

Macromolecules 20210916 18

The stress response of polymer double networks depends not only on the properties of the constituent networks but also on the interactions arising between them. Here, we demonstrate, via coarse-grained simulations, that both their global stress response and their microscopic fracture mechanics are governed by load sharing through these internetwork interactions. By comparing our results with affine predictions, where stress redistribution is by definition homogeneous, we show that stress redistr ...[more]

PMID: 34602652

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Project description:BackgroundLow-stress resin-based composites (RBCs) are available to the clinician, some using stress relaxation mechanisms on the basis of network reconfiguration, modulated photopolymerization, or chain transfer reactions. This study investigated those materials in terms of their overall stress relaxation and their relationship with polymerization kinetics and compared them with an experimental low-stress thiourethane (TU) material.MethodsExperimental composites (bisphenol-A-diglycidyl dimethacrylate, urethane dimethacrylate, and triethylene glycol dimethacrylate [50:30:20 mass ratio]; 70% barium aluminosilicate filler; camphoroquinone, ethyl-4-dimethylaminobenzoate, and 2,6-di-tert-butyl-4-methylphenol [0.2:0.8:0.2% by mass]) with or without TU oligomer (synthesized in-house) and commercial composites (SureFil SDR Flow+ Posterior Bulk Fill Flowable Base [SDR Flow+] [Dentsply Sirona], Filtek Bulk Fill Posterior Restorative [3M ESPE], and Filtek Supreme Ultra Universal Restorative [3M ESPE]) were tested. Polymerization kinetics (near-infrared) and polymerization stress (Bioman) were evaluated during light-emitting diode photoactivation at 100 mW/cm2 for 20 seconds. Stress relaxation was assessed using dynamic mechanical analysis. Data were analyzed with a 1-way analysis of variance and Tukey test (α = 0.05).ResultsThe kinetic profiles of all materials differed substantially, including more than a 2-fold difference in the rate of polymerization between TU-modified composites and SDR Flow+. TU-modified RBCs also showed more than a 2-fold higher conversion at the onset of deceleration vs the experimental control and commercial materials. RBCs that used stress reduction mechanisms showed at least a 34% reduction in polymerization stress compared with the controls and significantly reduced the amount of early-onset stress buildup. SDR Flow+ and the TU-modified RBCs showed the greatest amount of viscoelastic stress relaxation postpolymerization.ConclusionsThe novel TU-modified materials showed similar or improved performance compared with commercial low-stress RBCs, showing that chain transfer may be a promising strategy for stress reduction, both during polymerization and after polymerization.

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Sharing the Load: Stress Redistribution Governs Fracture of Polymer Double Networks.

Publications

Sharing the Load: Stress Redistribution Governs Fracture of Polymer Double Networks.

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