To solve the problem of excessive heat accumulation in the electronic packaging field, a novel series of hybrid filler (BN@CNT) with a hierarchical “line-plane” structure was assembled via a condensation reaction between functional boron nitride(f-BN) and acid treated carbon nanotubes (a-CNTs). The reactions with different mass ratios of BN and CNTs and the effect of the obtained hybrid filler on the composites’ thermal conductivity were studied. According to the results, BN@15CNT exhibited better effects on promoting thermal conductivity of polybenzoxazine(PBz) composites which were prepared via ball milling and hot compression. The thermally conductive coefficient value of PBz composites, which were loaded with 25 wt% of BN@15CNT hybrid fillers, reached 0.794 W· m−1· K−1. The coefficient value was improved to 0.865 W· m−1· K−1 with 15 wt% of BN@15CNT and 10 wt% of BN. Although CNTs were adopted, the PBz composites maintained insulation. Dielectric properties and thermal stability of the composites were also studied. In addition, different thermal conduction models were used to manifest the mechanism of BN@CNT hybrid fillers in enhancing thermal conductivity of PBz composites.

In this work, polydimethylsiloxane (PDMS)-based composites with high thermal conductivity were fabricated via a three-dimensional hybrid boron nitride@silver nanowires (BN@AgNWs) filler thermal network, and their thermal conductivity was investigated. A new thermal conductive BN@AgNWs hybrid filler was prepared by an in situ growth method. Silver ions with the different concentrations were reduced, and AgNWs crystallized and grew on the surface of BN sheets. PDMS-based composites were fabricated by the BN@AgNWs hybrid filler added. SEM, XPS, and XRD were used to characterize the structure and morphology of BN@AgNWs hybrid fillers. The thermal conductivity performances of PDMS-based composites with different silver concentrates were investigated. The results showed that the thermal conductivity of PDMS-based composite filled with 20 vol% BN@15AgNWs hybrid filler is 0.914 W/(m·K), which is 5.05 times that of pure PDMS and 23% higher than the thermal conductivity of 20 vol% PDMS-based composite with BN filled. The enhanced thermal conductivity mechanism was provided based on the hybrid filler structure. This work offers a new way to design and fabricate the high thermal conductive hybrid filler for thermal management materials.

Normally, the effective dispersion of thermal conductive fillers is a prerequisite for ensuring thermally conductive networks formed in polymer composites. In this work, a facile method was provided by using cellulose to alter the distribution state of boron nitride (BN) for the preparation of high thermally conductive polylactic acid (PLA). After powder mixing and hot‐pressing process, the Cellulose@BN was located at the boundaries of PLA granules to form consecutive thermally conductive networks with more compact structure. Morphology observation and FTIR spectra confirmed that BN edges absorbed on the cellulose surface under the intermolecular hydrogen bond interaction between PLA and BN. At the BN content of 25 wt%, contrasted with traditional BN/PLA segregated polymer composites (SPCs), thermal conductivity coefficient of Cellulose@BN/PLA SPCs improved by 53.5% from 0.71 to 1.09 Wm−1 K−1. This enhancement could be attributed to the reason that the cellulose regulated stripe aggregation allowed the BN connect with each other more compact, thus a thermal conduction networks with reduced phonon scattering were formed.

In this work, a multi‐contact Al2O3@AgNPs hybrid thermal conductive filler was synthesized by in‐situ growth method to fill high thermal conductivity polydimethylsiloxane (PDMS)‐based composites to prepare TIMs. And the thermal conductivity, electrical conductivity, and mechanical properties of the composite materials were studied. During the synthesis process of the multi‐contact hybrid filler, different concentrations of silver ions were reduced to generate silver nanoparticles and attached to the surface of Al2O3. Al2O3@AgNPs/PDMS thermally conductive composites were prepared by changing the filler addition. Using SEM, XPS, and XRD is used to characterize the morphology and chemical composition of Al2O3@AgNPs hybrid filler. The thermal conductivity of PDMS‐based composites with different AgNPs content under 70 wt% filler loading was studied. The results show that the thermal conductivity of PDMS‐based composites filled with 7owt%Al2O3@3AgNPs/PDMS multi‐contact hybrid filler is 0.67 W/m·K, which is 3.72 times that of pure PDMS, and is higher than that of unmodified Al2O3 with the same addition amount. /PDMS composite material has a high thermal conductivity of 24%. This work provides a new idea for the design and manufacture of high thermal conductivity hybrid fillers for TIMs.