Work

Interfacial Chain Mobility in Polymer–Silica Elastomers Governs the Balance between Biocompatibility and Tissue-Like Mechanics

Year: 2026
Type: preprint
Abstract: Soft biological tissues combine biocompatibility, viscoelastic energy dissipation and J-shaped nonlinear elasticity, yet the molecular principles for reproducing these properties in artificial soft materials remain unclear. Here we identify interfacial chain mobility, rather than interaction strength, as a key parameter governing tissue-like mechanics in composite elastomers. Using non-aggregated silica particles dispersed in biocompatible PMEA and PMEO2MA networks, we decouple polymer–particle interactions from filler aggregation. Strong multipoint interactions in PMEO2MA create a constrained interphase that suppresses chain mobility and promotes premature stiffening. By contrast, moderate PMEA–silica interactions preserve interfacial mobility while enabling efficient stress transfer. This balance produces J-shaped elasticity through finite chain extensibility and pronounced hysteresis through reversible interfacial stress transfer. Our results reveal complementary molecular origins of nonlinear elasticity and energy dissipation, establishing interfacial chain mobility as a design principle for biointegrated soft materials combining flexibility, damping, biocompatibility and tissue-like mechanical performance.
Source: ChemRxiv
Language: English
Open Access status: green
OpenAlex ID: W7213441800
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