Abstract

Thermal interface materials with high thermal conductivity (TC) and mechanical compliance were essential for electronic devices. In this work, a highly thermal conductive and compliant composite with strong interfacial strength was fabricated by multilayer-stacking partially vulcanized silicone rubber (SR)/graphite (Gr) composites (Heter-SR/Gr) with high and low Gr contents, and then fully cured by further hot pressing. The multi-step vulcanization endowed great orientation of Gr and covalent bond between layers, thus heightened TC, maintained the mechanical compliance and enhanced the interfacial strength, respectively. The out-plane TC reached 25.45 W/(m·K) with an overall Gr content of 60.94 wt%, the TC value of the homogeneous structured composite was only 11.15 W/(m·K); these were consistent to the FEA simulation results. Moreover, the stress of Heter-SR/Gr reached 2.24 MPa at 25% compressive strain, which was 35.82% lower than that of homogeneous composite (3.49 MPa). This facile strategy is expected to be promoted in the further applications.

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