Dynamic sustainable polyamide elastomer toward ultratough and fully recyclable self-healing ionic conductors

Abstract

The development of flexible ionic conductors with extreme elasticity, high ionic conductivity, desirable self-healing capacity and recyclability is a pressing need while challenging because the regulating of these performances is generally mutually exclusive. Herein, we report a dynamic double-crosslinking bio-based ionic conductive elastomer (DBICE), designed via the introduction of reversible covalent Diels-Alder motifs into a furan-functionalized biobased polyamide matrix, which realizes an ultratough, outstanding mechanical versatility (170.1 MJ m−3 toughness and 1342% elongation), unique self-healability (∼100% within 6 h), and capability to completely recycle and facilely reprocess. The specifically tailored ether-rich segments in the polyamide backbones with long-range ordering and selectively entrapped lithium-ion (Li+) provided high-efficient ion transport pathways, gaining remarkable room-temperature ionic conductivity of 1.66 × 10–3 S m−1. The resultant DBICE is assembled into a proof-of-concept flexible ionotronic sensor, exhibiting reliable resistivity sensing quality with high sensitivity and robust mechanosensation capability, and excellent recovery for the polymeric matrices and electronic components. This work provides a new molecular design principle for the sustainable development of advanced ionic conductors holding a great promise in wearable electronics or all-solid-state batteries.