In nature, anisotropic movements and deformations of plants can be triggered by environmental humidity variations to achieve various biological functions. Due to the orientation of cellulose fibrils, anisotropic deformations occur when the tissue swells and expands. Inspired by biological systems, many stimuli-responsive polymeric materials have been designed for programmable actuators. However, it remains a challenge to achieve a fast-actuating speed and fracture-healable ability for programable actuators, which limits their applications as sensors, wearables, and packaging devices. Nanocellulose have been recognized as an ideal templating and reinforcing element in actuators. Herein, we fabricated a thin film cellulose-based actuator with polyvinyl alcohol and polystyrene sulfonate as reinforcement. Driven by moisture, the actuators bend in programmable directions when prepared by different routines. Furthermore, the actuator shows an elongation-at-break of 77%. Ultra-Small-Angle X-ray Scattering (USAXS) and scanning electron microscopy reveals the formation of voids and the increase in local crystallinity at the necking region of the stretched film. When examining the same region with USAXS for a hydration - dehydration cycle, the changes in the void size and the film crystallinity are fully reversible, which shows the programmable and self-healing ability of the actuator and highlights its potential as smart packaging.

Cellulose-based programmable, robust, and self-healable actuators for smart packaging

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