Synergistically Improving the Thermal Conductivity and Mechanical Strength of PEEK/MWCNT Nanocomposites by Functionalizing the Matrix with Fluorene Groups

Nanofiller reinforcement is an effective method to prepare high thermally conductive polymer‐matrix composites. However, the poor dispersion of nanofillers and high interfacial thermal resistance between the filler and matrix seriously affect the thermal conductivity and mechanical properties of composites. To solve this problem, a small amount of conjugated fluorene group is introduced into the polymer chain of poly (ether ether ketone) (PEEK) to afford the fluorene‐functionalized copolymer matrix (FD‐PEEK). In an in situ polymerization procedure, the matrix non‐covalently binds to multi‐walled carbon nanotubes (MWCNT) to allow highly filled PEEK/MWCNT nanocomposites. With the filler dispersion and matrix–filler interfacial bonding improved, the prepared nanocomposites possess both high thermal conductivity and tensile strength. At the optimal ratio of 2 mol% fluorene groups in the polymer chain, the nanocomposite with 10 wt% MWCNT exhibits an excellent thermal conductivity of 2.41 W m−1 K−1, which is 868% higher than pristine PEEK, with tensile strength remaining 104.3 MPa. The PEEK/MWCNT nanocomposites can be further used as matrix resins to build double‐segregated network multi‐component composites, which contributes to an innovative strategy to design high‐performance thermally conductive materials. The introduction of the conjugated group bisphenol fluorene effectively improves the dispersion of multiwalled carbon nanotubes (MWCNT) in in situ polymerization and increases the interfacial bonding strength. The reduction of interfacial thermal resistance significantly enhances the thermal conductivity of the nanocomposite. Instead of pure resin, this copolymerized nanocomposite is used to prepare high thermal conductivity and high strength poly (ether ether ketone) (PEEK) composites.