Copolymer-grafted cellulose nanocrystal induced nanocomposite hydrogels with enhanced strength, high elasticity and adhesiveness for flexible strain and pressure sensors

Recently, the application of cellulose nanocrystals (CNCs) in the field of hydrogel sensors has attracted much attention. However, it remains challenging to construct CNC-reinforced conductive hydrogels with a combination of enhanced strength, low hysteresis, high elasticity and remarkable adhesiveness. Herein, we present a facile method to prepare conductive nanocomposite hydrogels with the above-mentioned properties by reinforcing chemically crosslinked poly(acrylic acid) (PAA) hydrogel with rational-designed copolymer-grafted CNCs. The copolymer-grafted CNCs interact with PAA matrix to form carboxyl-amide conventional hydrogen bonds and carboxyl-amino ionic hydrogen bonds, among which the ionic hydrogen bonds with rapid recovery capability are critical to the low hysteresis and high elasticity of hydrogel. The introduction of copolymer-grafted CNCs endowed the hydrogels with enhanced tensile/compressive strength, high resilience (>95 %) during tensile cyclic loading, rapid self-recovery during compressive cyclic loading and improved adhesiveness. Thanks to the high elasticity and durability of hydrogel, the assembled hydrogel sensors exhibited good cycling repeatability and durability in detecting various strains, pressures and human motions. The hydrogel sensors also showed satisfying sensitivity. Hence, the proposed preparation method and the obtained CNC-reinforced conductive hydrogels would open new avenues in flexible strain and pressure sensors for human motion detection and beyond.