Versatile ionic liquid gels formed by dynamic covalent bonding and microphase separated structures

It is challenging for ionic liquid gels to achieve the combination of rapid self-healing with high toughness. Here, ionic liquid gels (DI-PR) were prepared from readily available materials. A dynamic covalently bonded oxime-carbamate was prepared from polycaprolactone diol, isophorone diisocyanate and dimethylethyleneglyoxime, followed by addition of the “rigid-flexible” cross-linking agent rutin to chemically cross-link the polymer chains and afford the ionic liquid gels, DI-PR. The tensile strength, elongation at break and toughness of the DI-PR gels were as high as 16.5 MPa, 1132.6%, and 52.6 MJ m⁻³, respectively. The toughness is similar to that of natural silkworm silk (70 MJ m⁻³) and wool (60 MJ m⁻³). After stretching, the DI-PR can rebound within 1 s, their room temperature self-healing rate is as high as 92%, they remain functional over the temperature range −50 °C to 140 °C and the interface with a steel plate has an adhesion toughness of >2000 J m⁻². These properties mean that the DI-PR gels are particularly suitable for use as anticorrosion coatings for submarine and underground gas and oil pipelines. The use of rutin, which combines rigid quercetin-based structural units with flexible glycoside-based structural units, as a cross-linking agent, provides a new method for improving the toughness of soft materials through its synergistic interaction with hard and soft chain fragments of polyurethanes.