Hydrophobic and hydrophilic polyrotaxane based movable cross-linkers for thermo-sensitive poly(N-isopropylacrylamide) gels

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A novel hydrogel has been fabricated using vinyl modified polyrotaxane as a cross-linker. A sparsely dispersed propylene oxide modified α-cyclodextrins which were threaded into the long polyethylene glycol (Mw = 35000) and were trapped by bulky 1-adamantanamine molecules was used as a hydrophilic polyrotaxane, HPR. HPR was modified by a small amount 2-acryloyloxyethylisocyanate monomer to obtain a water soluble polyrotaxane-based movable cross-linker, MHPR. Polymer gels, prepared by free radical polymerization of thermo-sensitive monomer N-isopropylacrylamide (NIPA) in presence of MHPR cross-linker, gave transparent, soft and flexible, mechanically strong and fast thermo-sensitive gels. The gel changes its volume isotropically and reaches rapidly to the equilibrium shrunken state after a temperature jump. The hydrophilicity of the cross-linker retains the homogeneity in the gel network and restricts the formation of aggregated globules, which permits the poly(NIPA) chains along with macrocycles to move or rotate freely inside the gel networks under deformation. The movability of the cross-links can strongly minimize their localized stress during deformation. The fascinating characteristics of the gel was compared and contrasted with the gels prepared using using hydrophobic polyrotaxane-based multifunctional and bi-functional N,N'-methylene-bis-acrylamide cross-linkers.
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