Chemical Gradients in Polymer-Modified Paper Sheets—Towards Single-Layer Biomimetic Soft Robots

Biomimetic actuators are typically constructed as functional bi- or multilayers, where actuating and resistance layers together dictate bending responses upon triggering by environmental stimuli. Inspired by motile plant structures, like the stems of the false rose of Jericho (Selaginella lepidophylla), we introduce polymer-modified paper sheets that can act as soft robotic single-layer actuators capable of hygro-responsive bending reactions. A tailored gradient modification of the paper sheet along its thickness entails increased dry and wet tensile strength and allows at the same time for hygro-responsiveness. For the fabrication of such single-layer paper devices, the adsorption behavior of a cross-linkable polymer to cellulose fiber networks was first evaluated. By using different concentrations and drying procedures fine-tuned polymer gradients throughout the thickness can be achieved. Due to the covalent cross-linking of polymer with fibers, these paper samples possess significantly increased dry and wet tensile strength properties. We furthermore investigated these gradient papers with respect to a mechanical deflection during humidity cycling. The highest humidity sensitivity is achieved using eucalyptus paper with a grammage of 150 g m⁻² modified with the polymer dissolved in IPA (~13 wt%) possessing a polymer gradient. Our study presents a straightforward approach for the design of novel hygroscopic, paper-based single-layer actuators, which have a high potential for diverse soft robotic and sensor applications.