Deep Eutectic Solvent-Induced Microphase Separation and Entanglement of PVA Chains for Tough and Reprocessable Eutectogels for Sensors

A high-strength PVA-based eutectogel has been synthesized by a strategy of solvent-induced microphase separation. Here, PVA was dissolved in water, and green solvent DES (choline chloride/glycerol) was introduced to induce PVA to undergo microphase separation, leading to poorly solvated domains and highly solvated domains. In poorly solvated domains, the PVA chains were folded and crystallized, and the formed crystalline domains served as physical cross-linkers. Such cross-linking structures endowed the eutectogels with remarkable mechanical properties, showing strength in tension reaching up to 1.2 MPa and elongation at a break of 405%, with rupture toughness of 3.23 MJ m–3. Meanwhile, the as-obtained eutectogel possessed reprocessability and could be recycled through high-temperature dissolution and recasting. In addition, the eutectogel also exhibited excellent frost resistance, and its ionic conductivity could still reach 0.62 mS cm–1 at −40 °C. In addition, the eutectogel can maintain a stable output signal during a multiple strain cycle, showing the potential application in the flexible sensor. The eutectogel is capable of detecting the bending movement of joints and identifying the different bending angles of fingers, showing a certain applied potential in motion detection of the human body.