AbstractA series of polydimethylsiloxane–urea acrylate prepolymers was synthesized by reacting aminopropyl‐terminated polydimethylsiloxane (ATPS) with isocyanatoethyl methacrylate (IEM). The oligomers were cured using ultraviolet radiation in the presence of different reactive diluents. Three systems were prepared with varying ATPS soft segment molecular weight. All of the samples were transparent. However, microphase separation was indicated by the observation of two glass transition temperatures attributed to separate ATPS and IEM/reactive diluent phases. Increasing ATPS molecular weight led to a lower rubbery phase transition temperature and a smaller rigid phase volume fraction. These effects were reflected in lower modulus and tensile strength at room temperature, and higher elongation at break. An increase in the reactive diluent content resulted in an increase in Young's modulus and the ultimate tensile strength of these materials. Increasing reactive diluent content caused the rubbery phase transition peak to decrease in magnitude without changing its position and shifted the hard segment transition to higher temperature. The tensile strengths and moduli of these materials were higher than those reported in the literature for other polydimethylsiloxane and urethane acrylate materi
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