Cationic Cellulose Nanocrystals-Based Nanocomposite Hydrogels: Achieving 3D Printable Capacitive Sensors with High...

Hydrogel ionotronics are intriguing soft materials that have been applied in wearable electronics and artificial muscles. These applications often require the hydrogels to be tough, transparent, and 3D printable. Renewable materials like cellulose nanocrystals (CNCs) with tunable surface chemistry provide a means to prepare tough nanocomposite hydrogels. Here, we designed ink for 3D printable sensors with cationic cellulose nanocrystals (CCNCs) and zwitterionic hydrogels. CCNCs were first dispersed in an aqueous solution of monomers to prepare the ink with a reversible physical network. Subsequent photopolymerization and the introduction of Al³⁺ ion led to strong hydrogels with multiple physical cross-links. When compared to the hydrogels using conventional CNCs, CCNCs formed a stronger physical network in water that greatly reduced the concentration of nanocrystals needed for reinforcing and 3D printing. In addition, the low concentration of nanofillers enhanced the transparency of the hydrogels for wearable electronics. We then assembled the CCNC-reinforced nanocomposite hydrogels with stretchable dielectrics into capacitive sensors for the monitoring of various human activities. 3D printing further enabled a facile design of tactile sensors with enhanced sensitivity. By harnessing the surface chemistry of the nanocrystals, our nanocomposite hydrogels simultaneously achieved good mechanical strength, high transparency, and 3D printability.