On the origin of heating-induced softening and enthalpic reinforcement in elastomeric nanocomposites
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arXiv
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| Auteurs principaux: | , , |
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| Format: | Preprint |
| Publié: |
2025
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| _version_ | 1866909944576475136 |
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| author | Kawak, Pierre Bhapkar, Harshad Simmons, David S. |
| author_facet | Kawak, Pierre Bhapkar, Harshad Simmons, David S. |
| contents | Despite a century of use, the mechanism of nanoparticle-driven mechanical reinforcement of elastomers is unresolved. A major hypothesis attributes it to glassy interparticle bridges, supported by an observed inversion of the variation of the modulus E(T) on heating -- from entropic stiffening in elastomers to enthalpic softening in nanocomposites. Here, molecular simulations reveal that elastomer enthalpic softening can instead emerge from a competition over preferred nonequilibrium volumes between elastomer and nanoparticulate networks. A theory for this competition accounting for softening of the bulk modulus on heating predicts the simulated E(T) inversion, suggesting that reinforcement is driven by a volume-competition mechanism unique to co-continuous systems of soft and rigid networks. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2501_06971 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | On the origin of heating-induced softening and enthalpic reinforcement in elastomeric nanocomposites Kawak, Pierre Bhapkar, Harshad Simmons, David S. Soft Condensed Matter Mesoscale and Nanoscale Physics Materials Science Despite a century of use, the mechanism of nanoparticle-driven mechanical reinforcement of elastomers is unresolved. A major hypothesis attributes it to glassy interparticle bridges, supported by an observed inversion of the variation of the modulus E(T) on heating -- from entropic stiffening in elastomers to enthalpic softening in nanocomposites. Here, molecular simulations reveal that elastomer enthalpic softening can instead emerge from a competition over preferred nonequilibrium volumes between elastomer and nanoparticulate networks. A theory for this competition accounting for softening of the bulk modulus on heating predicts the simulated E(T) inversion, suggesting that reinforcement is driven by a volume-competition mechanism unique to co-continuous systems of soft and rigid networks. |
| title | On the origin of heating-induced softening and enthalpic reinforcement in elastomeric nanocomposites |
| topic | Soft Condensed Matter Mesoscale and Nanoscale Physics Materials Science |
| url | https://arxiv.org/abs/2501.06971 |