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

Chen, Jing; Gao, Yiyang; Shi, Lei; Yu, Wei; Sun, Zongjie; Zhou, Yifan; Liu, Shuang; Mao, Heng et al. · Nat Commun · 2022

basic_science · Level V

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Abstract

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 propose an ionic conductor design, dynamic supramolecular ionic conductive elastomers (DSICE), via phase-locked strategy, wherein locking soft phase polyether backbone conducts lithium-ion (Li<sup>+</sup>) 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<sup>-3</sup> S m<sup>-1</sup> at 30 °C), high transparency (92.3%), superior stretchability (2615.17% elongation), strength (27.83 MPa) and toughness (164.36 MJ m<sup>-3</sup>), excellent self-healing capability (~99% at room temperature) and favorable recyclability. This work provides an interesting strategy for designing the advanced ionic conductors and offers promise for flexible ionotronic devices or solid-state batteries.