C60 fullerene/thermoplastic polyurethane elastomer (PUE) composites were prepared by using the roll-mixing method. Initially, the PUEs, with various hard segment contents (HSC), were synthesizedwith poly (oxytetramethylene) glycol (PTMG), 4,4'-diphenylmethane diisocyanate (MDI) and 1,4-butanediol (BD) by the prepolymer method. To control the HSC, a molar ratio of PTMG/MDI/BD was varied at 1/2/1, 1/3/2 and 1/4/3. The effects of HSC in PUEs on the relationship between tensile properties and microphase-separated structure of C60/PUE composites were investigated using a tensile test, dynamic mechanical analysis (DMA) and differential scanning calorimetry (DSC) after annealing at 80 and 120℃. Tensile strength of the PUE composites was already improved at a fullerene concentration of 100ppm, moreover, that of the PUE composites with higher HSC increased with an increasing amount of C60, as annealing at higher temperature. The results of DSC and DMA indicate that the aggregation structure of hard segments in the PUEs has been influenced by the presence of the fullerene. It was found that the direct addition of a small amount of fullerene is a valuable modifying method of PUEs.
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