The influence of the preparation method on the initial structure and deformation behavior of polystyrene (PS) - polyisoprene (PI) - PS (SIS) triblock copolymer elastomers was investigated using small-angle X-ray scattering (SAXS) and wide-angle X-ray diffraction (WAXD). Shear pressing (SP) and injection molding (IM) were used as the preparation methods. The samples exhibited a microphase-separated structure, in which the PS cylinders were packed in a hexagonal lattice for the entire sample. SP-SIS possessed a higher degree of microphase separation (DMPS) and an ordering of a microphase-separated structure (OMPSS), and lower degree of the PS cylinder orientation (DCO) than IM-SIS. Uniaxial tensile testing was performed along the parallel (//) and perpendicular (–|) directions to the PS cylinder orientation combining in situ SAXS/WAXD measurements. Young’s modulus and tensile strength of IM-SIS were lager and smaller than those of SP-SIS. A change in the PS cylinder orientation, which occurs for –| stretching, of IM-SIS occurred at larger strain than SP-SIS, indicating that the orientation of highly ordered PS cylinders are difficult to be changed due to their larger domains. It was found that the DCO relates to Young's modulus, yielding, and change in the PS cylinder orientation, while the OMPSS and DMPS relate to tensile strength.
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