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Hierarchical Effects of Cyclodextrin Ring Positioning in Triblock-Copolymer Polyrotaxanes on Microphase-Separated Structures
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DOI：10.1039/D6NJ01334A.png)
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Abstract
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Hierarchical effects that propagate from molecular scale and polymer assembly to higher-order structures have attracted increasing attention. In this study; we synthesized two types of triblock copolymer-based polyrotaxanes (PRs) comprising β-CyD and EO75PO29EO75 (PR-CR93%) or EO124PO47EO124 (PR-CR60%); and investigated how the β-CyD positions in solution influence the microphase-separated structures of solvent-cast solids. In DMSO-d6; the β-CyD distribution along the polymer axis changed upon addition of D2O. This behavior differed depending on whether β-CyD could cover the entire PPO segment.When complete coverage was possible; β-CyD preferentially occupied the hydrophobic PPO segment; when it was not; the PPO segments formed micelles and β-CyD relocated to the flanking PEO chains. This solution-state localization of β-CyD along the axis promoted the formation of ordered structures in the cast samples. These results demonstrate that the conformational freedom of the PR rings is tunable and exerts ripple effects on higher-order self-assembled structures.
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