Modulating the stiffness of polymer nanocomposites with high energy dissipation via interfacial coupling

Flexible polymer materials with extraordinary energy dissipation have attracted surging interest in emerging soft bioelectronics. Traditional damping materials rely on internal friction caused by chain segment relaxation activated by glass transition or supramolecular dissociation. However, this mechanism inherently suffers from a narrow damping range and a compromised modulus. Beyond these constraints, a distinct softening process becomes pronounced at elevated temperatures, governed by the thermodynamically driven decrease in chain friction, which leads to a sharp decline in modulus. Here, we present an interphase dynamic coupling confinement in complex fluid nanocomposites for deriving materials with high energy dissipation and thermosetting at high temperatures. This is realized by temperature-driven switches in the Flory-Huggins parameter between infused dynamically asymmetric fluids and nanoparticle interphase, thus bridging the percolation network in confinement. Using proportionately interphase-modified nanoparticles, we demonstrate that the prepared nanocomposites exhibit a thermally induced modulus increase with high damping performance (loss factor >0.4) across wide temperature (−30°C to 150°C) and frequency (10 −2 to 10 6 Hz) intervals. Moreover, the modulus ratio between the upper and lower bounds of the effective damping temperature range surpasses that of conventional elastomeric materials.