Water training initiates spatially regulated microstructures with competitive mechanics in hydroadaptive polymers

Abstract The strategy using water as a medium for dynamic modulation of competitive plasticity and viscoelasticity provides a unique perspective to attain adaptive materials. We reveal sustainable polymers, herein cellulose phenoxyacetate as a typical example, with unusual water-responsive dual-mechanic functionalities addressed via a chronological water training strategy. The temporal significance of such water-responsive mechanical behaviors becomes apparent considering that a mere 3-minute exposure or a prolonged 3-hour exposure to water induced different types of mechano-responsiveness. This endows the materials with multiple recoverable shape-changes during water and air training, and consequently even underlines the switchability between the pre-loaded stable water shapes (> 20 months) and the sequentially fixed air shapes. Our discovery exploits the competitive mechanics initiated by water training, enabling polymers with spatially regulated microstructures via their inherently distinct mechanical properties. Insights into the molecular changes represents a considerable fundamental innovation, can be broadly applicable to a diverse array of hydroadaptive polymers.