Heat-Induced Supramolecular Organogels Composed of α-Cyclodextrin and "Jellyfish-Like" β-Cyclodextrin-Poly(ε-caprolactone)

ABSTRACT In general, the complexation and gelation behavior between biocompatible poly(ε‐caprolactone) (PCL) derivatives and α‐cyclodextrin (α‐CD) is extensively studied in water, but not in organic solvents. In this article, the complexation and gelation behavior between α‐CD and multi‐arm polymer β‐cyclodextrin‐PCL (β‐CD‐PCL) with a unique “jellyfish‐like” structure are thoroughly investigated in organic solvent N,N‐dimethylformamide and a new heat‐induced organogel is obtained. However, PCL linear polymers cannot form organogels under the same condition. The complexation is characterized by rheological measurements, DSC, XRD, and SEM. The SEM images reveal that the complexes between β‐CD‐PCL and α‐CD present a novel topological helix porous structure which is distinctly different from the lamellar structure formed by PCL linear polymers and α‐CD, suggesting the unique “jellyfish‐like” structure of β‐CD‐PCL is crucial for the formation of the organogels. This research may provide insight into constructing new supramolecular organogels and potential for designing new functional biomaterials. © 2013 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2013, 51, 1598–1606 While there have been a large number of reports on gelation between poly(ε‐caprolactone) (PCL) derivatives and CDs, hydrogels are more commonly reported than organogels. A heat‐induced organogel is obtained by multi‐arm polymer β‐CD‐PCL with a unique “jellyfish‐like” structure and α‐CD in DMF. SEM images reveal the tendency of the organogel to form a novel topological helix porous structure. This research may provide a new method to construct supramolecular organogels with the potential for new functional biomaterials.