Phase-locked constructing dynamic supramolecular ionic conductive elastomers with superior toughness, autonomous self-healing and recyclability

Stretchable ionic conductors are considerable to be the most attractive candidate for next-generation flexible ionotronic devices. Nevertheless, high ionic conductivity, excellent mechanical properties, good self-healing capacity and recyclability are necessary but can be rarely satisfied in one material. Herein, we demonstrate a novel ionic conductor design, dynamic supramolecular ionic conductive elastomers (DSICE), via “phase-locked” strategy, wherein “locking soft phase” polyether backbone conducts lithium-ion (Li⁺) transport and the combination of dynamic disulfide metathesis and stronger supramolecular quadruple hydrogen bonds in the hard domains contributes to the self-healing capacity and mechanical versatility. The dual-phase design performs its own functions and the conflict among ionic conductivity, self-healing capability, and mechanical compatibility can be thus defeated. The well-designed DSICE exhibits high ionic conductivity (3.77×10⁻³ S m⁻¹ at 30°C), high transparency (92.3%), superior stretchability (2615.17% elongation), strength (27.83 MPa) and toughness (164.36 MJ m⁻³), excellent self-healing capability (~99% at room temperature) and favorable recyclability. This work provides a new strategy for designing the advanced ionic conductors and offers promise for flexible iontronic devices or solid-state batteries.