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Volume fraction and width of ribbon-like crystallites control the rubbery modulus of segmented block copolymers

Abstract We discuss the origin of the plateau modulus enhancement (χ) in semi-crystalline segmented block copolymers by increasing the concentration in hard segments within the chains (XHS). The message we deliver is that the plateau modulus of these thermoplastic elastomers is greatly dominated by the volume fraction (Φ) and the width (W) of crystallites according to χ–1 ~ ΦW in agreement with a recent topological model we have developed. We start by a quick review of literature with the aim to extract χ(Φ) for different chemical structures. As we suspected, we find that most of the data falls onto a mastercurve, in line with our predictions, confirming that the reinforcement in such materials is mainly dominated by the crystallite’s content. This important result is then supported by the investigation of copolymer mixtures in which Φ is fixed, providing a similar reinforcement, while the chains compositions is significantly different. Finally, we show that the reinforcement can be enhanced at constant Φ by increasing W for a given class of block copolymers. This can be done by changing the process route and is again in good agreement with our expectations.