Asynchronous Reaction Toward Hierarchical Crosslinking Polymer Networks

Ionogels have emerged as promising materials in soft iontronics, with their network structure playing a pivotal role in determining performance and enabling diverse applications. Refining the network architectures of ionogels through chemical design is a promising strategy. This Concept article summarizes our recent progress in the design of polymeric ionogel networks. Our methodology exploits the pronounced disparity in chemical reactivity among functional groups, thereby achieving the spontaneous formation of these hyperbranched clusters through asynchronous reactions. These hyperbranched clusters spontaneously assemble via hydrogen-bonding interactions, thereby constructing hierarchical cross-linked polymer networks. This network design endows polyurea ionogels with high strength, exceptional toughness, low hysteresis, and fluorescence. We have summarized the applications of such ionogels in emerging fields, including flexible sensing, electroluminescent devices, and nanogenerators. Finally, the application prospects and future development directions of these materials are discussed. This network design strategy is expected to provide new insights for developing functionalized ionogels.