Ionogels with favorable mechanical robustness, high conductivity, and excellent resistance to tear and fatigue are crucial for portable energy devices and/or flexible electronics. However, the intrinsic plasticizing effect and network dilution caused by ionic liquids (IL) compromise their mechanical robustness. Herein, a confinement-locking strategy is developed to produce mechanically robust and fatigue-resistant phase-separate ionogels. First, a portion of soft segments is confined within the hard domains to buffer stress and facilitate hydrogen bonding (H-bonding) assemblies reorganization. Second, the IL are confined within soft phases, which eliminates the interference with hard segments and consequently enhances the stability of H-bonding networks. The synergistic effects of robust H-bonding networks, extensive supramolecular interactions between soft segments (polycaprolactone, PCL) and IL, strain-induced crystallization of PCL, and stress-damping by confined soft segments endow the ionogel with an exceptional combination of tensile strength (∼45.4 MPa), fracture toughness (256.1 MJ·m- 3), elongation at break (1576.6%), elastic recovery (>91%), ionic conductivity (1.04 mS·cm-1), tear strength (∼108.1 kJ·m- 2), and a record-high fatigue threshold (8796 J·m- 2), enabling the ionogel with great potential in perceptive artificial ligaments.
Keywords: confinement‐locking; fatigue resistance; hydrogen bonding; ionogel; strength.
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