Invariable resistance of conductive nanocomposite over 30% strain.

The dependence of the electrical resistance on materials' geometry determines the performance of conductive nanocomposites. Here, we report the invariable resistance of a conductive nanocomposite over 30% strain. This is enabled by the in situ-generated hierarchically structured silver nanosatellite particles, realizing a short interparticle distance (4.37 nm) in a stretchable silicone rubber matrix. Furthermore, the barrier height is tuned to be negligible by matching the electron affinity of silicone rubber to the work function of silver. The stretching results in the electron flow without additional scattering in the silicone rubber matrix. The transport is changed to quantum tunneling if the barrier height is gradually increased by using different matrix polymers with smaller electron affinities, such as ethyl vinyl acetates and thermoplastic polyurethane. The tunneling current decreases with increasing strain, which is accurately described by the Simmons approximation theory. The tunable transport in nanocomposites provides an advancement in the design of stretchable conductors.

Highly Conductive Strong Healable Nanocomposites via Diels-Alder Reaction and Filler-Polymer Covalent Bifunctionalization.

Healable stretchable conductive nanocomposites have received considerable attention. However, there has been a trade-off between the filler-induced electrical conductivity (σ) and polymer-driven mechanical strength. Here significant enhancements in both σ and mechanical strength by designing reversible covalent bonding of the polymer matrix and filler-matrix covalent bifunctionalization are reported. A polystyrene-block-poly(ethylene-ran-butylene)-block-polystyrene grafted with maleic anhydride forms the strong reversible covalent bonding with furfuryl alcohol through the Diels-Alder reaction. Small (7.5 nm) and medium (117 nm) nanosatellite particles are generated by in situ etching of silver flakes, enabling electron tunneling-assisted percolation. The filler-polymer covalent bifunctionalization is achieved by 3-mercaptopropanoic acid. Altogether, this results in high σ (108 300 S m-1 ) and tensile strength (16.4 MPa), breaking the trade-off behavior. A nearly perfect (≈100%) healing efficiency is achieved in both σ and tensile strength. The conductive nanocomposite figure of merit (1.78 T Pa S m-1 ), defined by the product of σ and tensile strength, is orders of magnitude greater than the data in literature. The nanocomposite may find applications in healable strain sensors and electronic materials.

Electron tunneling of hierarchically structured silver nanosatellite particles for highly conductive healable nanocomposites.

Healable conductive materials have received considerable attention. However, their practical applications are impeded by low electrical conductivity and irreversible degradation after breaking/healing cycles. Here we report a highly conductive completely reversible electron tunneling-assisted percolation network of silver nanosatellite particles for putty-like moldable and healable nanocomposites. The densely and uniformly distributed silver nanosatellite particles with a bimodal size distribution are generated by the radical and reactive oxygen species-mediated vigorous etching and reduction reaction of silver flakes using tetrahydrofuran peroxide in a silicone rubber matrix. The close work function match between silicone and silver enables electron tunneling between nanosatellite particles, increasing electrical conductivity by ~5 orders of magnitude (1.02×103 Scm-1) without coalescence of fillers. This results in ~100% electrical healing efficiency after 1000 breaking/healing cycles and stability under water immersion and 6-month exposure to ambient air. The highly conductive moldable nanocomposite may find applications in improvising and healing electrical parts.