Since selectively swollen thermoplastic elastomer gels (TPEGs) afford a wide range of beneficial properties that open new doors to developing elastomer-based technologies, we examine the unique structure-property behavior of TPEGs composed of olefinic block copolymers (OBCs) in this study. Unlike their styrenic counterparts typically possessing two chemically different blocks, this class of multiblock copolymers consists of linear polyethylene hard blocks and poly(ethylene--α-octene) soft blocks, in which case, microphase separation between the hard and the soft blocks is accompanied by crystallization of the hard blocks. Here, we prepare olefinic TPEGs (OTPEGs) through the incorporation of a primarily aliphatic oil that selectively swells the soft block and investigate the resultant morphological features through the use of polarized light microscopy and small-/wide-angle X-ray scattering. These features are correlated with thermal and mechanical property measurements from calorimetry, rheology, and extensiometry to elucidate the roles of crystallization and self-assembly on gel characteristics and establish useful structure-property relationships.
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