AbstractWhile improving the thermal conductivity of composites, single‐size carbon nanotubes (CNT) often degrade their mechanical properties due to the agglomerates. To overcome this limitation, this study reported thermoplastic resin matrix composites synergistically reinforced with small, medium, and large‐size carbon nanotubes (S‐CNT, M‐CNT, and L‐CNT). Using the thermal conductivity (λ) and mechanical properties (flexural strength [F], compressive strength [C] and tensile strength [T]) as the response values, we conducted 21 sets of mixing design experiments and developed the associated quadratic term models. Further multi‐objective optimization was carried out for the above response values. Optimized multiscale CNT synergistically modified composites (S‐CNT, M‐CNT, and L‐CNT contents of 1.25, 7.02, and 2.56 wt%) exhibited a λ value of 1.168 W/mK, which was 121% higher than that of pure composite and also superior to the same content of S‐CNT‐ (1.031 W/mK), M‐CNT‐ (1.016 W/mK), and L‐CNT‐modified composites (0.983 W/mK). Additionally, the optimized composite demonstrated excellent mechanical properties (F = 1482 MPa, C = 848 MPa, and T = 1759 MPa), which were 13%, 11%, and 13% higher than those of the pure composites, respectively, and also surpassed those of the S‐CNT‐, M‐CNT‐and L‐CNT‐modified composites.Highlights Using three different scales of carbon nanotubes modified CF/PPBESK composites. Polynomial modeling of composite's thermal conductivity and mechanical properties. Synergistic interactions between carbon nanotubes to improve the composite's thermal conductivity and mechanical properties.
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