A Highly Conductive, Self-Recoverable, and Strong Eutectogel of a Deep Eutectic Solvent with Polymer Crystalline Domain Regulation

It is desirable to fabricate an antifatigue gel for skin-mimicking sensors on the demand of long-term durability in practical usage. Here, we developed a physically cross-linked eutectogel based on a poly(vinyl alcohol)/poly(acrylic acid) (PVA/PAA) binary polymer skeleton and a deep eutectic solvent (DES). In this eutectogel, uniformly distributed PVA crystalline domains acted as stable physical cross-linkers, and high-density hydrogen bonds possessed great reversibility. Such a polymer network structure was expected to endow this eutectogel with excellent mechanical strength, stretchability, and a self-recovery ability. Specifically, this eutectogel exhibited a superior tensile strength of 2.6 MPa, a fracture strain of 680%, and a fracture toughness of 8.39 MJ m–3. In cyclic stretching/releasing tests with a fixed strain of 100%, this eutectogel could recover its mechanical properties within a 600 s resting time. Based on this self-recoverable eutectogel, a reliable flexible sensor was fabricated, which possessed good sensitivity and stability over a wide strain range (1–300%). More importantly, the flexile sensor was able to maintain a highly repeatable response signal during 1000 consecutive stretching/releasing cycles, showing outstanding long-term durability. Given the excellent sensing performance, this eutectogel has promising potential in wearable electronics, human–machine systems, and soft robotics.