Interpenetrating polymer networks (IPNs) based on triisocyanate-terminated poly(urethane-imide)s (PUIs) were prepared by in situ interpenetrating reactions between modified polyurethane (PU) with different ratios of polyimide (PI). The effects of PU, which was made from hydroxyl-terminated polybutadiene modified with triisocyanate, and the amounts of PI on the mechanical properties, thermal properties, and crystalline character of the IPNs were discussed. Triisocyanate-terminated PUI showed that the highest tensile strength was 38 times that of the diisocyanate-terminated materials. Supramolecular cross-linking from an additional hydrogen-bonding network of modified PU and the degree of interpenetration with a regular imide structure of PI were introduced, which accounted for the remarkable improvement in mechanical properties of IPNs. Preferable thermal stability and glass transition temperature for the hard segment of IPNs were rewarded with increasing PI content. X-ray diffraction revealed vigorous segmental mixing between the soft and hard segments of modified PUI. Scanning electron micrographs showed the “fibrous assembly” morphology and short-range-ordered structure of modified PUI.
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