In-situ phase separation constructing robust hydrophobic ionogels with multifunction

Ionogels, as the promising alternative to hydrogels, have garnered great attention due to their excellent ionic conductivity, thermal stability, and non-volatility. However, the design and construction of robust hydrophobic ionogel still is a significant challenge at present, especially with a facile method. Herein, inspired by the two-phase structure of the dermis in human skin (stiff collagen fiber scaffold embedded in soft elastin matrix), a one-pot in-situ phase separation design strategy is proposed to construct the robust hydrophobic ionogel through the random copolymerization of hydrophobic monomers with the solubility difference in hydrophobic ionic liquid (IL). The resultant ionogel forms a homogeneously dual phase network containing solvent-rich soft domains and solvent-poor hard domains. The mechanical robustness can be synergistically achieved by the hard domain strong skeleton and the soft domain elastic matrix. Benefiting from multiple reversible interactions including hydrogen bonding, ion–dipole and ion-ion interactions, and physical entanglement, the ionogel shows strong IL retention, excellent self-healing, and regenerating abilities, while can adhere to different substrates. The unique phase separation structure brings temperature-dependent transparency and high-damping features. The ionogel also presents high ionic conductivity due to the abundance of movable ions. As application demonstrations, the ionogel is successfully used for dynamic pattern encryption, shock attenuation, and strain sensing. What’s more, this strategy can be also applied to improve the mechanical properties of hydrophobic ionogels based on other monomers. Hence, this work establishes an effective and general design strategy for hydrophobic ionogels demanding versatility.