Facile Solvent Regulation for Highly Strong and Tough Physical Eutectogels with Remarkable Strain Sensitivity

Physical eutectogels have great potential for applications in many fields due to their electrical conductivity, broad temperature stability, and biocompatibility. However, the preparation of high-performance physical eutectogels in a simple, efficient, and cost-effective way remains a challenge. In this study, a facile but efficient solvent regulation strategy was proposed to construct a highly robust poly(vinyl alcohol) (PVA) physical eutectogel. Hydrogen bonds within the polymer-containing deep eutectic solvent system were dynamically regulated by the introduction–removal of water to induce the formation of a uniform and dense polymer cross-linked network, which imparted excellent mechanical properties to the resulting eutectogel. For the eutectogel with 15 wt % PVA, the tensile strength and toughness were 1.67 MPa and 6.81 MJ m–3, respectively, which were at a high level among existing physical eutectogels. This high-performance eutectogel was available as a strain sensor and exhibited high sensitivity. In addition, this eutectogel can be endowed with a directional muscle-like stretching performance through convenient mechanical training. The easy scalability and low cost made our method an effective strategy for developing high-performance physical eutectogels, which would further promote the application of such materials in areas such as wearable electronics and soft robotics.