This paper describes the experimental findings of the study of a series of PU/epoxy composites, which formed interpenetrating networks and have shape‐memory properties. The morphological variation for different chemical compositions and the influences of morphology on mechanical performance and shape‐memory behavior are discussed. Length and mass fraction of polyethylene glycol (PEG) units are chosen as the key parameters in this study. The molecular weight of PEG was varied from 400 (as such PEG units are unable to crystallize) to 1500, 4000, and 6000, which are crystallizable. It was shown that the crystallization of PEG units is the key parameter, which determines the mechanical performance and shape‐memory behavior of PU/epoxy composites in this study. DMTA results show the linear dependence of glass transition temperature and tensile strength, elongation, and other mechanical parameters on the amount of PEG in PU/epoxy composites independently of the amount of PEG unit lengths. The maximal value of shape fixation rate was achieved for 30–40 mass percentage of PEG 4000 (4.5 × 10−2 s−1 at Tg + 20°C) or PEG 6000(4.1 × 10−2 s−1 at Tg + 20°C) in PU/epoxy composites.
A set of aromatic-oxyaliphatic polyurethanes (PUs) with different mass fractions of components also containing fluorinated fragments was synthesized and studied using various solid-state NMR techniques and dielectric spectroscopy. In contrast to the common model suggested by Cooper and Tobolsky in 1966, the rigid domains of microphase separated PUs are formed, not only by units containing urethane bonds, but also by oxyethylene fragments that form a common rigid phase. The urethane bonds and oxyethylene fragments are incorporated into both rigid and soft phases. Good agreement with the Cooper and Tobolsky model is observed only when solubility parameters are significantly different for the hard and soft segments, such as hydrocarbon aromatics and perfluoroaliphatic blocks.
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