無

In recent years attention has been expanded from supramolecular chemistry to supramolecular polymer chemistry, because of more sophisticated structural and functional achievement of supramolecular polymers. For example, in living system, various supramolecular polymers play important roles in maintaining life, such as double helix DNA, microtubules and microfilaments. This dissertation mainly focuses on the synthesis and structural investigation of supramolecular polymers inclusion complexation based on cyclodextrins. The discussion begins with detailed introduction and then in the second chapter, the supramolecular self assembled structures prepared from cyclodextrin based pseudo-polyrotaxanes and their assembled behavior investigation using various techniques like, transmission electron microscope (TEM), scanning electron microscope (SEM), synchrotron wide angle X-ray diffraction (WAXD), dynamic light scattering (DLS), cofocal laser scanning microscope (CLSM), polarized optical microscope (POM), UV-vis spectroscopy (UV-Vis) and Fourier-transform infrared (FTIR) were discussed. Macromolecular pseudo-polyrotaxanes were prepared through solution mixing method in which, the poly sebacic acid (PSA), polyaniline (PAni) were used as a guest matrix and α -cyclodextrin, β-cyclodextrin used as a host matrix.
The third chapter of the dissertation includes the design and supramolecular inclusion complexes (ICs) of α-Cyclodextrin (α-CD) and biodegradable polysebacic acid (PSA) that were prepared by using two different of pH values (pH 7 and pH 10). Interestingly, ICs prepared at pH 7 shows turbidity and then into white precipitate, while IC prepared at pH 10 forms into a clear solution, indicating the pH dependent behavior of the ICs and its formationof supramolecular assembly varies significantly by changing the pH. Moreover, we also found that by changing the pH, the affinity of the guest with the CD cavity differs from strong intermolecular hydrogen bonding to weak electrostatic interaction between PSA and α-CD. Besides, the crystallization of PSA is found to be suppressed by the addition of α-CD. The self-assembly of the obtained ICs are described by dynamic light scattering and transmission electron microscope and also ICs models are discussed describing the cyclodextrin pseudo-polyrotaxanes in order to find possible explanation for pH sensitivity.
The fourth chapter of the dissertation explains the design and synthesis of a cyclodextrin based “hairy urchin” shape PAni which was achieved from a simple microemulsion polymerization technique in the presence of β-cyclodextrin (β-CD). Ferric chloride (FeCl3) has played a role as a structural directing agent to fabricate the polymer as hairy urchin like structure/nano-rods via a cooperative interaction between FeCl3 and DoTAC in an aqueous medium. Host-guest inclusion complex of β-cyclodextrin with aniline was used as a monomer. It has been revealed that the formation of the supramolecular complexes of PAni with β-CD due to host-guest interaction is indispensable for the fabrication of these unique PAni nanostructures, and a suitable β-CD to aniline molar ratio is essential to their exclusive formation. Different varieties of PAni nanostructures, such as hairy urchin, branched particles consisting of rod-like branches, regular rod-like particles were obtained in the presence of FeCl3. Also, in the absence of FeCl3, predominant product of regular spherical particles and wire like aggregation exhibiting faceted surfaces were obtained.
The last chapter of the dissertation describes the synthesis of “Chrysanthemum-snowball” shaped PAni and its aligned supramolecular morphology obtained from simplepolymerization technique with self assembly method. It was found that, unique morphology of PAni with chrysanthemum-snowball like particles could be appropriately regulated by turning the concentration of monomer complex (β-CD/Ani complex) to oxidant. The amount of monomer complex has played a role as a structural regulating agent to fabricate the inclusion polymer as chrysanthemum-snowball structure/nanorods via an intermolecular interaction such as hydrogen bonding between β-CD, π-π interactions and cooperative interaction between PAni with FeCl3 in an aqueous medium. Different varieties of self-aligned PAni nanostructures, such as rod-like, flower-like assembled particles consisting of small length rod-like assemble regular chrysanthemum-snowball like particles were obtained. The morphological evolution of chrysanthemum-snowball like aggregation structures under different temperatures is examined. After observing their growth process, a tentative interpretation has been proposed to elucidate the formation of the PAni hierarchical structures.

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