Highly Elastic, Self-Healing, Recyclable Interlocking Double-Network Liquid-Free Ionic Conductive Elastomers via Facile Fabrication for Wearable Strain Sensors

Liquid-free ionic conductive elastomers (ICEs) are ideal materials for wearable strain sensors in increasingly flexible electronic devices. However, developing recyclable ICEs with high elasticity, self-healability, and recyclability is still a great challenge. In this study, we fabricated a series of novel ICEs by in situ polymerization of lipoic acid (LA) in poly(acrylic acid) (PAA) solution and cross-linking by coordination bonding and hydrogen bonding. One of the obtained dynamically cross-linked interlocking double-network ICEs, PLA–PAA 4-1% ICE, showed excellent mechanical properties, with high elasticity (90%) and stretchability (610%), as well as rapid self-healability (mechanical self-healing within 2 h and electrical recovery within 0.3 s). The PLA–PAA 4-1% ICE was used as a strain sensor and possessed excellent linear sensitivity and highly cyclic stability, effectively monitoring diverse human motions with both stretched and compressed deformations. Notably, the PLA–PAA 4-1% ICE can be fully recycled and reused as a new strain sensor without any structure change or degradation in performance. This work provided a viable path to fabricate conductive materials by solving the two contradictions of high mechanical property and self-healability, and structure stability and recyclability. We believe that the superior overall performance and feasible fabrication make the developed PLA–PAA 4-1% ICE hold great promise as a multifunctional strain sensor for practical applications in flexible wearable electronic devices and humanoid robotics.