Designing Tough, Printable, and Adaptable Eutectogels with Multinetworks via Synergy of Rapid Orthogonal Photopolymerizations and Solvent Effect in Seconds

Achieving a straightforward design of tough, printable, and adaptable polymeric eutectogels is still challenging in related fields due to the uncontrollable polymerization and solvent-exchanging processes, and inherent contrasting multiple networks. Here, we report a one-step synergistic strategy based on ruthenium chemistry-catalyzed photopolymerization and solvent effect for preparing high-performance eutectogels. This orthogonal ruthenium photochemistry helps multinetworks formation via phenol-coupling of gelatin and copolymerization of acrylamide (AAm) and [2-(methacryloyloxy)ethyl] trimethylammonium tetrafluoroborate (META) monomers in seconds. The obvious difference in the supramolecular interactions of free AAm monomers and polymerized units in P(AAm-co-META) with deep eutectic solvents (DESs) significantly promotes the microphase-separation behavior in eutectogels. Consequently, the in situ polymerization and microphase-separation behavior enable the as-prepared eutectogel materials to have excellent mechanical properties (stress of similar to 1.2 MPa), toughness (similar to 4.0 MJ m(-3)), elasticity, adaptivity, and conductivity (similar to 0.5 S m(-1) at room temperature). Also, the critical strength of the resultant eutectogels can be modulated by varying the DES constituents. This rapid and well-controlled synergistic approach is compatible with extrusion printing techniques to make flexible sensors with high sensitivities and response times to detect pressure in a range of 0-500 kPa. Such a general and simple strategy has application potential in biological, engineering, and material sciences.