3D Printable Organohydrogel with Long-Lasting Moisture and Extreme-Temperature Tolerance for Flexible Electronics

Hydrogels with high electrical conductivity and mechanical stretchability are promising materials for flexible electronics. However, traditional hydrogels are applied in short-term usage at room temperature or low temperature due to their poor water-retention ability and freezing-tolerance property. Here, a dually cross-linked glycerol–organohydrogel (GL–organohydrogel) based on GL and acrylic acid was synthesized in a GL–water binary solvent. Fe3+ ions working as an electrolyte were added to improve the conductivity of the organohydrogel and form coordination interactions between Fe3+ ions and carboxyl groups of acrylic acid. The strong hydrogen bonding between GL and water molecules firmly lock water in the organohydrogel network, thereby endowing the GL–organohydrogel with the antifreezing property, long-term stability, and moisture lock-in capability. Our organohydrogel could endure extremely low temperature (−80 °C) over 30 days without freezing and retain its water content (almost 100% of its initial state) after being stored at room temperature (25 °C, 54% humidity) for 30 days. It also demonstrated desired stretchable properties, conductivity, three-dimensional (3D) printability, and self-healing ability. A wearable data glove was constructed by using the GL–organohydrogel and digital light processing technology. This work opens a new avenue for developing hydrogels with long-term stability, moisture lock-in capability, and extreme-temperature tolerance for stretchable electronics.