A robust supramolecular ionic elastomer with efficient self-healing and excellent ionic conductivity for strain...

Ionic conductive elastomers (ICEs), as vital components for flexible electronics and human-machine interfaces, face a persistent challenge in reconciling mechanical robustness with ionic conductivity and self-healing capacity. Herein, a high-performance ICE was developed by constructing a coordination-driven supramolecular network utilizing epoxidized natural rubber (ENR) and chitosan hydrochloride (CSCl). In this integrated architecture, LiO coordination bonds and interfacial hydrogen bonds serve as dynamic molecular bridges, coupling the rigid CSCl moieties with the flexible ENR matrix. The rigid CSCl segments function as multifunctional supramolecular junctions, which not only provide robust mechanical reinforcement but also utilize their dense polar groups to trigger the accelerated dissociation of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), thereby elevating the local charge carrier concentration. Complementarily, the flexible ENR matrix, characterized by superior segmental mobility and a loosely coordinated environment, establishes rapid transport pathways for the liberated Li⁺ while imparting exceptional self-healing capabilities to the system. Benefiting from the synergy of this supramolecular integration, the resulting ICE simultaneously achieves a tensile strength of 9.2 MPa, a toughness of 22 MJ/m³, a conductivity of 3.8 × 10^-2 S/m, and a self-healing efficiency of 93%. These properties enable sensitive motion and respiration sensing, demonstrating significant potential for advanced wearable electronics.