Dynamic Metal-Ligand Coordination-Assisted Ionogels for Deformable Alternating Current Electroluminescent Devices

Overcoming the trade-off between the mechanical robustness and conductivity of ionic conductors is a crucial challenge for deformable ionotronics. In this work, we propose a simple but effective gelation strategy for selectively improving the mechanical robustness of ionogels without compromising their ionic conductivity. To achieve this, we introduce dynamic metal-ligand coordination chemistry into the ionic liquid (IL)-insoluble domains of a physically crosslinked ionogel network structure. As a result, the overall mechanical property is remarkably improved with the aid of additional chemical crosslinking. This strategy does not require any additional heat/light (UV) treatments to induce chemical crosslinking. The homogeneous physically/chemically dual crosslinked ionogel films can be readily obtained by simply casting a solution containing Ni²⁺ sources, copolymer gelators, and ILs. The effects of adjusting fundamental parameters on the ionogel properties are investigated systematically. The optimized mechanically robust and highly conductive ionogels are successfully employed as deformable ionic electrodes in alternating-current electroluminescent displays, indicating their high practicality. Overall, these results validate that exploiting metal-ligand coordination dynamic bonding is an extremely straightforward strategy for selectively improving the mechanical characteristics of conductive ionogels, which are promising platforms for deformable ionotronics.