LAUSR

Abstract While most self-healing elastomers are mechanically weak, using the most commonly used carbon black (CB) to reinforce self-healing elastomers has not been reported. The possible reason is that the introduction of carbon black will cause complex changes in molecular dynamics, which leads to unpredictable self-healing effects. Herein, carbon black is introduced into a self-healing ionomer based on brominated butyl rubber (BIIR) grafted with tert-butyl pyridine (BP). Interestingly, the hierarchical microstructure and multilevel molecular dynamics of ionomers are well regulated by the strong interfacial π-cation interactions between CB and ionic aggregates. The strong interfacial interaction leads to high content of bound rubber, uniform dispersion of CB and compact physical network. Although such structural change has negligible influence on the segmental motion, it enhances the relaxation time and activation energy of ionic clusters, and thus endows the ionomer with high mechanical properties. Meanwhile, the structural change leads to higher relaxation temperature, thereby increasing the self-healing temperature. Despite this fact, the healing efficiency can still be regulated between 50% and 100%, depending on the filler content and temperature. Moreover, the CB reinforced ionomer is re-processable and recyclable. This study demonstrates that CB reinforcement is feasible to improve the mechanical properties of self-healing elastomers.