Highly Stretchable, Recyclable, and Fast Room Temperature Self-Healable Biobased Elastomers Using Polycondensation

The substitution of petroleum-based self-healing elastomers with biobased counterparts is crucial to the global sustainable development of the rubber industry, which highly depends on the ease of the synthesis procedure. Herein, we show that highly stretchable, recyclable, and self-healable biobased elastomers were synthesized via condensation polymerization of succinic acid, adipic acid, sebacic acid, and 1,4-butanediol in the presence of a small amount of glycerol as a curing agent and 3,3′-dithiodipropionic acid as a dynamic covalent monomer. The macroscopic properties of our elastomers, including thermal, mechanical, stress relaxation, and self-healing performance, were finely regulated via microscopic chemical and topological structure. As such, a highly stretchable (up to ∼1700%), recyclable (almost without degradation of the mechanical performance over several repeats), rapid room temperature self-healable (in 20 min) biobased vitrimeric elastomer was achieved, which is the first aliphatic disulfide metathesis assisted self-healing polymer achieved at such low temperatures. The ease of the polycondensation with which the elastomers can be readily scaled up points to exciting opportunities for sustainable polymers with minimal environmental impact.