An Integrated Design of a Polypseudorotaxane‐Based Sea Cucumber Mimic. Issue 18 (24th March 2021)

• Record Type: Journal Article
• Authors: Li, Longyu; Lin, Qianming; Tang, Miao; Tsai, Esther H. R.; Ke, Chenfeng
• Is Part Of: Angewandte Chemie international edition. Volume 60:Issue 18(2021)
• Page Start: 10186
• Page End: 10193
• Publication Date: 2021-03-24
• Subjects: 3D printing -- biomimicry -- mechanically adaptive hydrogels -- polypseudorotaxane -- slide-ring gels; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.202017019
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: 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 α‐cyclodextrins (α‐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 α‐CD (de)threading. These discoveries enabled a successful fabrication of a sea cucumber mimic, demonstrating multi‐stage stiffness changes. Abstract : Cyclodextrin‐triggered stiffening: A sidechain polypseudorotaxane‐based sea cucumber mimic was designed from molecular entities, which exhibited multi‐stage shape persistence and stiffness variations.