A Repeatable Self-Adhesive Liquid-Free Double-Network Ionic Conductor with Tunable Multifunctionality

Liquid-free ionic conductors (LFICs) have promising applications in flexible electronics because most ionic conductors currently suffer from ionic liquid leakage or water evaporation issues. However, it has been a formidable challenge for LFICs to achieve long-term repeated self-adhesion on different substrates, especially on soft biological tissues. Based on the double-network design concept, we first fabricate a series of repeatable self-adhesive liquid-free double-network ionic conductors (SALFDNICs), consisting of stretchable first poly(AA-ChCl)-type supramolecular deep eutectic polymer networks and stiff second polydopamine (PDA) networks, which can maintain sufficient dynamic hydrogen bonds and catechol groups in the ionic conductors by preventing the overoxidation of dopamine, thus balancing the contradiction between adhesion and cohesion in liquid-free ionic conductors. Therefore, SALFDNICs can instantly form various interface interaction forces with multiple substrates (adhesion strength up to 757 N/m) and firmly adhere to various substrates for 20 detachment-reattachment cycles with a reduction in adhesion strength of less than 15%. Furthermore, SALFDNICs also have other comprehensive properties, such as optimum self-healing properties (self-healing efficiency of 90%), good stretchability (strain at break of 1200%), and promising conductivity (2.31 × 10–2 S m–1). Therefore, we believe that the extraordinary performance of SALFDNICs is important for improving device integration and the further development of flexible electronics.