Heterogeneity Regulation of Bilayer Polysaccharide Hydrogels for Integrating pH- and Humidity-Responsive Actuators and Sensors.

Bilayer hydrogel-based actuators have attracted much interest because inhomogeneous structures are easily constructed in hydrogels. We used three kinds of polysaccharides, including anionic carboxymethyl cellulose (CMC), cationic chitosan (CS), and amphoteric carboxymethyl chitosan (CMCS), as both structure-constructing units and actuation-controlling units in this work to fabricate physically crosslinked poly(vinyl alcohol) bilayer hydrogels. The spatial heterogeneity was tuned by changing the types and concentrations of polysaccharides in different layers, to regulate pH- and humidity-driven actions of bilayer hydrogels. Based on the distortion of the ionic channel during the humidity-motivated deformation of bilayer hydrogels, a two-in-one flexible device integrating a humidity-driven actuator and humidity-responsive sensor was then developed, which could detect the alterations of environmental humidity in real time. Moreover, good tensile toughness and interfacial bonding as well as the strain-resistance effect endowed the bilayer hydrogels with the capability of identifying human motion as a strain sensor, unlocking more application scenarios. This work provides an overall insight into the heterogeneity regulation of bilayer hydrogels using polysaccharides as stimulus-responsive units and also proposes an interesting strategy of manufacturing hydrogel-based flexible devices with both actuating and sensing capabilities.