Zn^{2 +}-Mediated Densification of Amorphous Network in Ternary Eutectogel for Wireless Assistive Monitoring

The trade-off between mechanical robustness and ionic conductivity in gel materials impedes their application in flexible electronics. Herein, a eutectogel is engineered via a synergistic strategy that integrates a ternary deep eutectic solvent (DES) (choline chloride/ethylene glycol/zinc chloride) with dynamic Zn^{2 +} coordination. Through in situ photopolymerization of 1-vinylimidazole in the ternary DES, a dynamically cross-linked organic-inorganic hybrid network is constructed. Crucially, Zn^{2 +} ions play a dual role: they form reversible Zn^{2 +}-imidazole coordination sites, enhancing the mechanical properties with an elongation at break of 1100% and a Young's modulus of 0.23 MPa, while inducing coordination-driven densification of the amorphous network. This compaction effect tightens the polymer network without triggering crystallization, while accessible ion-transport pathways are retained within the amorphous network. Consequently, the eutectogel exhibits a high ionic conductivity of 0.38 mS cm^{- 1}, overcoming the typical conductivity loss in high-strength gels. Using these properties, a flexible strain-sensing system with Bluetooth transmission is developed. It can capture real-time motor signals and convert them into visual commands, highlighting its potential for wireless assistive monitoring, particularly in rehabilitation for hemiplegic patients. This work provides a promising strategy for achieving a balance between mechanical robustness and ionic conductivity in soft materials by regulating the amorphous structure.