Glassy polymers are extremely difficult to self-heal below their glass transition temperature (Tg) due to the frozen molecules. Here, we fabricate a series of randomly hyperbranched polymers (RHP) with high density of multiple hydrogen bonds, which showTgup to 49 °C and storage modulus up to 2.7 GPa. We reveal that the hyperbranched structure not only allows the external branch units and terminals of the molecules to have a high degree of mobility in the glassy state, but also leads to the coexistence of “free” and associated complementary moieties of hydrogen bonds. The free complementary moieties can exchange with the associated hydrogen bonds, enabling network reconfiguration in the glassy polymer. As a result, the RHP shows amazing instantaneous self-healing with recovered tensile strength up to 5.5 MPa within 1 min, and the self-healing efficiency increases with contacting time at room temperature without the intervention of external stimuli.

Development of novel and versatile strategies to construct conductive polymer composites with low percolation thresholds and high mechanical properties is of great importance. In this work, we report a facile and effective strategy to prepare polyaniline@cellulose nanowhiskers (PANI@CNs)/natural rubber (NR) nanocomposites with 3D hierarchical multiscale structure. Specifically, PANI was synthesized in situ on the surface of CNs biotemplate to form PANI@CNs nanohybrids with high aspect ratio and good dispersity. Then NR latex was introduced into PANI@CNs nanohybrids suspension to enable the self-assembly of PANI@CNs nanohybrids onto NR latex microspheres. During cocoagulation process, PANI@CNs nanohybrids selectively located in the interstitial space between NR microspheres and organized into a 3D hierarchical multiscale conductive network structure in NR matrix. The combination of the biotemplate synthesis of PANI and latex cocoagulation method significantly enhanced the electrical conductivity and mechanical properties of the NR-based nanocomposites simultaneously. The electrical conductivity of PANI@CNs/NR nanocomposites containing 5 phr PANI showed 11 orders of magnitude higher than that of the PANI/NR composites at the same loading fraction,; meanwhile, the percolation threshold was drastically decreased from 8.0 to 3.6 vol %.

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