Ultrasensitive Piezoresistive and Piezocapacitive Cellulose-Based Ionic Hydrogels for Wearable Multifunctional Sensing

Tactile sensors, namely, flexible devices that sense physical stimuli, have received much attention in the last few decades due to their applicability in a wide range of fields like the world of wearables, soft robotics, prosthetics, and e-skin. Nevertheless, achieving a trade-off among stretchability, good sensitivity, easy manufacturability, and multisensing ability is still a challenge. Herein, an extremely flexible strain sensor composed of a cellulose-based hydrogel is presented. A natural biocompatible carboxymethylcellulose (CMC) hydrogel endowed with ionic conductivity by sodium chloride (NaCl) was used as the sensitive part. Both the sensible layer and electrodes were investigated with an innovative approach for wearable sensor applications based on electrochemical impedance spectroscopy to find the best device configuration. The sensor, exploitable both as a piezoresistor and as a piezocapacitor, presents high sensitivity to external stimuli, together with an extreme stretchability of up to 600%, showing the best strain and temperature sensitivity among the ionic conductive hydrogel-based devices presented in the literature. The very high strain sensitivity enables the hydrogel to be implemented in wearable strain sensors to monitor different human motions and physiological signals, representing a valid solution for the realization of transparent, easily manufacturable, and low-environmental-impact devices.