Abstract

It remains challenging to simultaneously realize mechanical robustness, malleability, and functionality in elastomers via facile yet efficient methods. Herein, a simple strategy for the biomimetic heterogeneous design is proposed to achieve mechanically strong, malleable, and functionalized elastomers. We demonstrate the strategy by straightforward mechanical mixing of a highly cross-linked vitrimeric elastomer with a homogeneous gum and subsequent curing, resulting in heterogeneous vitrimeric elastomers (hetero-VEs). The hetero-VEs comprise two phases: a hard phase with dense cross-links and a soft matrix with few cross-links, with excellent interface between the two phases. The hard phases can be deformed upon loading, dissipating energy, which significantly improves the overall mechanical performance of the hetero-VEs. When conductive fillers are incorporated into the soft matrix, due to the volume exclusion effect of the hard phases, the resultant hetero-VEs exhibit high conductivity with a small fraction of fillers. In view of the facile and generic preparation process, this strategy should be a promising way to reinforce and functionalize many vitrimeric elastomer systems.

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