An Integrated Design of a Polypseudorotaxane-Based Sea Cucumber Mimic

The development of integrated systems that mimic the multi-stage stiffness change of marine animals such as the sea cucumber requires the design of molecularly tailored structures. Herein, we used an integrated biomimicry design to fabricate a sea cucumber mimic using sidechain polypseudorotaxanes with tunable nano-to-macroscale properties. A series of polyethylene glycol (PEG)-based sidechain copolymers were synthesized to form sidechain polypseudorotaxanes with alpha-cyclodextrins (alpha-CDs). By tailoring the copolymers' molecular weights and their PEG grafting densities, we rationally tuned the sizes of the formed polypseudorotaxanes crystalline domain and the physical crosslinking density of the hydrogels, which facilitated 3D printing and the mechanical adaptability to these hydrogels. After 3D printing and photo-crosslinking, the obtained hydrogels exhibited large tensile strain and broad elastic-to-plastic variations upon alpha-CD (de)threading. These discoveries enabled a successful fabrication of a sea cucumber mimic, demonstrating multi-stage stiffness changes.

Automated summary

By tailoring the molecular weights and PEG grafting densities of the copolymers, the sizes of the formed polypseudorotaxanes crystalline domain and the physical crosslinking density of the hydrogels were rationally tuned, enabling 3D printing and mechanical adaptability. The obtained hydrogels exhibited large tensile strain and broad elastic-to-plastic variations after 3D printing and photo-crosslinking.