Abstract:With the miniaturization and high-frequency evolution of antennas in 5G/6G communications, aerospace, and transportation, polymer composite papers integrating superior wave-transparent performance and thermal conductivity for radar antenna systems are urgently needed. Herein, a down-top strategy was employed to synthesize poly(p-phenylene benzobisoxazole) precursor nanofibers (prePNF). The prePNF was then uniformly mixed with fluorinated graphene (FG) to fabricate FG/PNF composite papers through consecutively suction filtration, hot-pressing, and thermal annealing. The hydroxyl and amino groups in prePNF enhanced the stability of FG/prePNF dispersion, while the increased π-π interactions between PNF and FG after annealing improved their compatibility. The preparation time and cost of PNF paper was significantly reduced when applying this strategy, which enabled its large-scale production. Furthermore, the prepared FG/PNF composite papers exhibited excellent wave-transparent performance and thermal conductivity. When the mass fraction of FG was 40 wt%, the FG/PNF composite paper prepared via the down-top strategy achieved the wave-transparent coefficient (|T|2) of 96.3% under 10 GHz, in-plane thermal conductivity (λ∥) of 7.13 W m−1 K−1, and through-plane thermal conductivity (λ⊥) of 0.67 W m−1 K−1, outperforming FG/PNF composite paper prepared by the top-down strategy (|T|2 = 95.9%, λ∥ = 5.52 W m−1 K−1, λ⊥ = 0.52 W m−1 K−1) and pure PNF paper (|T|2 = 94.7%, λ∥ = 3.04 W m−1 K−1, λ⊥ = 0.24 W m−1 K−1). Meanwhile, FG/PNF composite paper (with 40 wt% FG) through the down-top strategy also demonstrated outstanding mechanical properties with tensile strength and toughness reaching 197.4 MPa and 11.6 MJ m−3, respectively.