Regulating surface energy and establishing covalent bonds to enhance interface interaction between m‐BN and polyphenylene oxide for 5G applications

Abstract Incorporation of boron nitride (BN) into polymers is a promising method to obtain composites with high thermal conductivity, low dielectric constant (D_k), and dielectric loss (D_f), while the practical applications are limited by the poor interface between BN and polymer because of surface energy mismatch and absence of covalent bond connection between them. Herein, polydopamine (PDA) with good adhesion is deposited onto the BN. Then, a different amount of silane coupling agent containing vinyl reactive groups is grafted onto PDA‐coated BN. In this way, the surface energy of modified BN (m‐BN) can be adjusted to ensure BN contacts well with polymers. Moreover, reactive groups were introduced on BN for further reaction. Subsequently, covalent bonds between the m‐BN and the polyphenylene oxide (PPO) were established in situ during the curing process. The effects of the m‐BN surface energy on interface quality and thermal conductivity of composites are investigated. The m‐BN/PPO composite achieves a through‐plane thermal conductivity of 5.87 W/m·K and a low D_f value of 1.53 × 10⁻³, as well as a low coefficient of thermal expansion (CTE) value (7.8 ppm/K) when the m‐BN loading is 32.6 vol%. This research provides a simple and efficient strategy for fabricating high‐performance composites for high‐frequency applications. Highlights Hexagonal boron nitride was modified successfully by combining non‐covalent and covalent modifications. Regulating surface energy and establishing covalent bonds enhances interface interaction between BN and polyphenylene oxide. Modified BN/polyphenylene oxide composites display improvements in thermal conductivity and dimensional stability as well as dielectric loss. Provides a feasible strategy for designing polymer composites with high thermal conductivity, dimensional stability, and low dielectric loss for 5G applications.