Environmentally Tolerant Multifunctional Eutectogel for Highly Sensitive Wearable Sensors

Flexible hydrogel sensors have found extensive applications. However, the insufficient sensing sensitivity and the propensity to freeze at low temperatures restrict their use, particularly in frigid conditions. Herein, a multifunctional eutectogel with high transparency, anti-freezing, anti-swelling, adhesive, and self-healing properties is prepared by a one-step photopolymerization of acrylic acid and lauryl methacrylate in a binary solvent comprising water and deep eutectic solvent (DES). The results from the molecular dynamics simulations and density functional theory indicate that the hydrogen bonds between DES and water mixtures possess better stability than those between water molecules. On the other hand, DES breaks down hydrogen bonds in water, providing eutectogels with excellent anti-freezing even at -60 °C. Cetyltrimethylammonium bromide is incorporated to establish stable hydrophobic interactions and electrostatic attractions with polymer chains in the eutectogel network, resulting in superior mechanical (elongation at break of 2890%) and anti-swelling (only 2% swelling in water over 7 days) properties. The eutectogel-based strain sensors exhibit remarkable sensitivity, achieving a gauge factor of up to 15.4. The multifunctional eutectogel sensors can monitor motion and transmit encrypted information at low temperatures, demonstrating considerable potential for applications in flexible electronics within low-temperature environments.