Entropy-Driven Ultratough Blends from Brittle Polymers.

Polymer blends with synergetic performance play an integral part in modern society. The discovery of compatible polymer systems often relies on strong chemical interactions. By contrast, the role of entropy in polymers is often neglected. In this work, we show that entropy effect could control the phase structure and mechanical behaviors of polymer blends. For weakly interacting polymer pairs, the seemingly small mixing entropy favors the formation of nanoscale cocontinuous structures. The abundant nanointerfaces could initiate large plastic deformations by crazing or shear, thus, transforming brittle polymers (elongation < 9%) into superductile materials (elongation ∼ 146%). The resultant polymer blends display high transparency, strength (∼70 MPa), and toughness (∼60 MJ/m3) beyond most engineering plastics. The principle of entropy-driven blends may also be applied in other polymer systems, offering a strategy to develop mechanically robust bulk polymeric materials for emerging applications such as biomedicine and electronics.

Super Tough and Self-Healable Poly(dimethylsiloxane) Elastomer via Hydrogen Bonding Association and Its Applications as Triboelectric Nanogenerators.

Poly(dimethylsiloxane) (PDMS) as one of the electron-drawing materials has been widely used in triboelectric nanogenerators (TENG), which is expected to generate electron through friction and required to endure dynamic loads. However, the nature of the siloxane bond and the low interchain interaction between the methyl side groups result in low fracture energy in PDMS elastomers. Here, a strategy that combined the advantages of the dynamic of hierarchical hydrogen bonding and phase-separation-like structure was adopted to improve the toughness of PDMS elastomers. By varying both stronger and weaker hydrogen bonding within the PDMS network, a series of super tough (up to 24,000 J/m2), notch-insensitive, transparent, and autonomous self-healable elastomers were achieved. In addition, a hydrophilic polymeric material (PDMAS-U10) was synthesized as the conductive layer. A transparent TENG was fabricated by sandwiching the PDMAS-U10 between two pieces of the PDMS elastomer. Despite its hydrophilic nature, PDMAS-U10 exhibit strong adhesion interaction with hydrophobic PDMS elastomers. As such, a tough (16,500 J/m2), self-healable (efficiency ∼97%), and transparent triboelectric nanogenerator was constructed. A self-powered system employing the TENG is also demonstrated in this work.