Hexagonal boron nitride nanosheets/graphene nanoplatelets/cellulose nanofibers-based multifunctional thermal interface materials enabling electromagnetic interference shielding and electrical insulation

Thermal interface materials (TIMs) that block electromagnetic interference (EMI) and current leakage are essential for high-density, high-power devices and compact form factors of electronic and mobility platforms. However, their coupled thermal-electrical-electromagnetic characteristics involve mismatches in thermal conductivity, electrical insulation, and EMI shielding, limiting the multifunctionality. Herein, a sandwich-like structural design that rationally combines graphene nanoplatelets (GNPs), hexagonal boron nitride nanosheets (BNNSs) and cellulose nanofibers (CNFs) is presented toward multifunctional trilayer TIMs enabling high thermal conductivity, EMI shielding, electrical insulation, mechanical compatibility and flame retardancy. The top and bottom BNNSs serve as electrically insulating yet thermally conductive layers while the GNPs in the central layer mitigate EMI and the CNFs as a binder complete the mechanical properties for the lamella-like trilayers. The resulting TIM exhibits a high in-plane thermal conductivity (25.5 W/m·K), and the LED cooling system using the TIM demonstrates the capability of reducing the operating temperature. Furthermore, it shows a high-volume resistivity (4.12 × 1013 Ω cm) and EMI shielding effectiveness (29.0 dB) at X-band frequencies. Its mechanical robustness is confirmed with tensile strength and elongation of 65.0 MPa and 2.36 %, and the high flame retardancy is validated. The outcomes will inspire tailoring multifunctional TIMs using lamellar structures that optimally combine micro/nanomaterials. [Display omitted] •Sandwich-structural GNPs/BNNSs/CNFs are designed for multifunctional trilayer TIMs.•GNP layers provide in-plane thermally conductive paths and EMI shielding capability.•BNNS layers enable electrical insulation via blocking current and flame retardancy.•Incorporating CNFs into GNPs and BNNSs reinforces mechanical strength/compatibility.•Developed TIMs offer multifunctionality to overcome complex interfacial challenges.