Low-temperature strain-sensitive sensor based on cellulose-based ionic conductive hydrogels with moldable and self-healing properties

Bioelectronics based on high-performance conductive ionic hydrogels, which can create novel technological interfaces with the human body, have attracted significant interest from both academia and industry. However, it is still a challenge to fabricate hydrogel sensor with integration of good mechanical properties, fast self-healing ability and flexible strain sensitivity below 0 °C. In this paper, we present a moldable, self-healing and adhesive cellulose-based ionic conductive hydrogel with strain-sensitivity, which was prepared by forming dual-crosslinked networks using poly(vinyl alcohol) (PVA) with borax, calcium chloride (CaCl2), zinc chloride (ZnCl2) and 2,2,6,6-tetramethylpiperidine-1-oxyl oxidized cellulose nanofibril (TCNF). The hydrogel exhibited fast self-healing within 10 s, moderate modulus of 5.13 kPa, high elongation rate of 1500 % and excellent adhesion behavior on various substrates. Due to multiple hydrogen bonding and the presence of CaCl2 and ZnCl2, the hydrogel presented a reduced freezing point as low as -41.1 °C, which enabled its application as a low-temperature strain sensor. The proposed hydrogel provides a simple and facile method for fabricating multi-functional hydrogels that can be used as suitable strain sensors for applications such as wearable electronic sensor, soft robotics and electronic skins in a wide temperature range.