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JAIST Repository: 新規な血液適合性高分子としての超分子構造を有するポリロタキサン誘導体の設計とその生医学的応用のための評価

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(1)JAIST Repository https://dspace.jaist.ac.jp/. Title. 新規な血液適合性高分子としての超分子構造を有する ポリロタキサン誘導体の設計とその生医学的応用のた めの評価. Author(s). 朴, 亨達. Citation Issue Date. 2003-03. Type. Thesis or Dissertation. Text version. none. URL. http://hdl.handle.net/10119/2131. Rights Description. Supervisor:由井 伸彦, 材料科学研究科, 博士. Japan Advanced Institute of Science and Technology.

(2) Design of Supramolecular-structured Polyrotaxane Derivatives as Novel Blood Compatible Polymers and Their Evaluation for Biomedical Applications. Japan Advanced Institute of Science and Technology School of Materials Science, Yui Laboratory Hyung Dal Park (040017). This dissertation deals with the design of supramolecular-structured PRx derivatives as novel blood compatible polymers and their evaluation for biomedical applications. A polyrotaxane (PRx), a representative supramolecular architecture, consists of cyclic molecules (typically, cyclodextrins, CDs) with high potency for chemical modification and polymeric chains capped with bulky-end groups. “A synergistic concept”, hypothesized to design PRx derivatives as novel blood compatible polymers, is as follows: The unique properties of functional groups (-SO3 and -PEG-SO3) and the physicochemical interactions of the supramolecular-structured PRxs with blood or cell would synergistically play an important role in enhancing blood compatibility. As based on the hypothesis, PRxs in which ,-cyclodextrins (,-CDs) are threaded onto poly(ethylene glycol) (PEG)-block-poly(propylene glycol) (PPG)-block-PEG TM. triblock copolymers (Pluronic ) capped with bulky-end groups were prepared and chemicallymodified by the introduction of sulfonate-containing groups to hydroxyl groups of ,-CDs. PRx derivatives was then applied to surface modification of conventional biomedical polymer. PRx derivatives containing the sulfonate groups showed the synergistically enhanced anticoagulant activity. The incorporation of PRx derivatives lead to the enhanced hydrophilicity by the change of surface properties onto the polyurethane (PU) substrate. Modified PUs showed the stable entrapment of PRx derivatives and the enhanced mechanical properties after exposure to water as compared with PU control. Some of incorporated PRx derivatives repelled the proteins from closely approaching the surface areas, prevented platelets from activation by thrombin, and were effective as bacteria repellents. The important factors that contribute to the obtained results are estimated to be 1) the higher density of induced functional groups by the unique supramolecular structure of PRx and 2) the higher mobility (effective inhibition of steric hindrance by higher density) of functional groups by a spacer (e.g. PEG in PEG-SO3). These characteristics of PRx derivatives are expected to be useful in the design of the novel supramolecular structure-based biomaterials, in the surface modification of biomedical polymers, and in further applications for blood compatible device fabrication..

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