Marine Amoebae-Inspired Salting Hydrogels to Reconfigure Anisotropy for Reprogrammable Shape Morphing

Reprogrammable shape morphing is ubiquitous in living beings and highly crucial for them to move in normal situations, even to survive under dangerous conditions. There is increasing interest in using asymmetric hydrogel structures to understand and mimic living beings' shape morphing upon an external trigger in a controlled way. However, these asymmetric or heterogeneous configurations cannot be further modified once the polymer hydrogels are prepared. Therefore, it is a great challenge to achieve reprogrammable shape morphing using the existing hydrogels. Inspired by marine amoebae, which transform into several different morphologies according to the various external salt concentrations, a new strategy is developed for salting hydrogels to reconfigure their anisotropy toward reprogrammable shape morphing. Polyampholyte hydrogels with equal stoichiometric COO^- and N⁺(CH₃)₃ groups were first swollen in HCl/NaCl solution. After being then transferred into water, they first swollen again by water uptake driven by the osmotic pressure, and then were spontaneously deswollen due to increase in internal pH and dialysis of ions leading to deprotonation of COOH to COO^- and regeneration of COO^-/N⁺(CH₃)₃ electrostatic attraction. This work provides a novel strategy to reconfigure anisotropy of hydrogel soft actuators and to open up an avenue for reprogrammable shape morphing.