The inclusion of graphene nanoplatelets (GNP) in segmented block copolymers offers a route to manipulate microphase separation for tailoring the mechanical properties of thermoplastic elastomers. GNP loading, lateral size, surface chemistry, interactions with the copolymer hard (HS) and soft (SS) segments and the relative ratio of HS:SS determine the mechanical properties achievable. To test this hypothesis, two different GNPs with similar surface chemistry but which differed in lateral dimensions by one order of magnitude (GNP1, ∼2μm and GNP2, ∼20μm) were melt mixed with three different poly(ether-block-amide)s (PE-b-A)s with variable HS and SS content from high to low. The inclusion of the larger lateral sized GNP2 had a more pronounced effect on PE-b-A morphology as it was more effective at hindering SS chain mobility resulting in microphase separation and suppression of the glass transition temperature (Tg) of the PE-b-A with the largest SS content. At low loadings GNP2 preferentially locates to the HS region, inducing reorganisation of this phase resulting in increased microphase separation. Strain induced crystallisation (SIC) phenomena were also observed for the lowest HS content PE-b-A, behaviour not evident for the PE-b-A with the largest HS content as the SS are not long enough to allow SIC. Inclusion of GNP2 to the PE-b-A with the largest HS content resulted in the largest increase in Young’s modulus (E) of 46%, tensile strength (σ) of 37% and elongation at break (ε) of 53% relative to the unfilled polymer.
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