Synergistic Dual-Cross-Linking Gelation: Exploring the Impact of Metal–Ligand Complexation on Ionogel Performance

Owing to the growing interest in wearable ionotronics, the demand for ionogels with outstanding mechanical and electrochemical characteristics has increased dramatically. Nevertheless, it remains challenging to simultaneously enhance the mechanical robustness and conductivity of ionogels because of their trade-off relationship. In this work, we propose physically/chemically dual-cross-linked ionogels designed to improve the mechanical strength without reducing ionic conductivity by introducing metal-ligand complexation only within the physically cross-linked domains. In particular, the impact of metal-ligand complexation, a crucial parameter in this strategy, on ionogel performance is systematically examined using various metal ions. The mechanical resilience and thermal stability of ionogels are effectively enhanced with Co³⁺ having the highest coordination number, which can be explained by the highest metal-ligand complexation (i.e., chemical cross-linking) density. Additionally, there is no degradation in ionic conductivity when compared to the pristine ionogel because these complexations occur within physically cross-linking domains that are irrelevant to the ion conductive channels. The dual-cross-linked ionogels are successfully applied to alternating-current electroluminescent displays (ACEDs). Moreover, a versatile mixed-emitter strategy is suggested to improve practicality, enabling the realization of frequency-controlled multicolor ACEDs.