A facile solvent-exchange strategy is devised to fabricate anti-drying, self-healing and transparent organohydrogels for stretchable humidity sensing applications.

Ionic hydrogels, a class of intrinsically stretchable and conductive materials, are widely used in soft electronics. However, the easy freezing and drying of water-based hydrogels significantly limit their long-term stability. Here, a facile solvent-replacement strategy is developed to fabricate ethylene glycol (Eg)/glycerol (Gl)-water binary antifreezing and antidrying organohydrogels for ultrastretchable and sensitive strain sensing within a wide temperature range. Because of the ready formation of strong hydrogen bonds between Eg/Gl and water molecules, the organohydrogels gain exceptional freezing and drying tolerance with retained deformability, conductivity, and self-healing ability even stay at extreme temperature for a long time. Thus, the fabricated strain sensor displays a gauge factor of 6, which is much higher than previously reported values for hydrogel-based strain sensors. Furthermore, the strain sensor exhibits a relatively wide strain range (0.5−950%) even at −18 °C. Various human motions with different strain levels are monitored by the strain sensor with good stability and repeatability from −18 to 25 °C. The organohydrogels maintained the strain sensing capability when exposed to ambient air for nine months. This work provides new insight into the fabrication of stable, ultrastretchable, and ultrasensitive strain sensors using chemically modified organohydrogel for emerging wearable electronics.

It is essential to impart the thermal stability, high sensitivity, self-healing, and transparent attributes to the emerging wearable and stretchable electronics. Here, a facile solvent replacement strategy is exploited to introduce ethylene glycol/glycerol (Gly) in hydrogels for enhancing their thermal sensitivity and stability synchronously. For the first time, we find that the solvent plays a key role in the thermal sensitivity of hydrogels. By adjusting the water content in hydrogels using a simple dehydration treatment, the thermal sensitivity is raised to 13.1%/°C. Thanks to the ionic transport property and water–Gly binary solvent, the organohydrogel achieves an unprecedented thermal sensitivity of 19.6%/°C, which is much higher than those of previously reported stretchable thermistors. The mechanism for the thermal response is revealed by considering the thermally activated ion mobility and dissociation. The stretchable thermistors are conformally attached on curved surfaces for the practical monitoring of minute temperature change. Notably, the uncovered Gly-organohydrogel avoids drying and freezing at 70 and −18 °C, respectively, reflecting the excellent antidrying and antifreezing attributes. In addition, the organohydrogel displays ultrahigh stretchability (1103% strain), self-healing ability, and high transparency. This work sheds light on fabricating ultrasensitive and stretchable temperature sensors with excellent thermal stability by modulating the solvent of hydrogels.

An ultrastretchable thermistor that combines intrinsic stretchability, thermal sensitivity, transparency, and self-healing capability is fabricated. It is found the polyacrylamide/carrageenan double network (DN) hydrogel is highly sensitive to temperature and therefore can be exploited as a novel channel material for a thermistor. This thermistor can be stretched from 0 to 330% strain with the sensitivity as high as 2.6%/°C at extreme 200% strain. Noticeably, the mechanical, electrical, and thermal sensing properties of the DN hydrogel can be self-healed, analogous to the self-healing capability of human skin. The large mechanical deformations, such as flexion and twist with large angles, do not affect the thermal sensitivity. Good flexibility enables the thermistor to be attached on nonplanar curvilinear surfaces for practical temperature detection. Remarkably, the thermal sensitivity can be improved by introducing mechanical strain, making the sensitivity programmable. This thermistor with tunable sensitivity is advantageous over traditional rigid thermistors that lack flexibility in adjusting their sensitivity. In addition to superior sensitivity and stretchability compared with traditional thermistors, this DN hydrogel-based thermistor provides additional advantages of good transparency and self-healing ability, enabling it to be potentially integrated in soft robots to grasp real world information for guiding their actions.