Ultrahigh Thermally Conductive Graphene-Based Thermal Interface Material with Low Compressive Modulus

The current trend toward high power density and high integration of electronic devices is challenging thermal interface materials (TIMs). Graphene is a potential candidate for fabricating high performance TIMs, due to its excellent thermal conductivity (TC). However, the preparation of graphene-based TIMs with high thermal conductivity and high compressibility remains a significant challenge. In this study, an innovative strategy for high performance TIMs is proposed by constructing vertically aligned elastic graphene arrays and filling acrylate emulsion. The graphene-based TIMs reach an ultrahigh vertical TC (⊥TC) up to 90.5 W m–1 K–1 and a low compressive modulus of 1.89 MPa at a graphene content of 30.07 wt %. Notably, the TIMs are applied in the heat dissipation of a commercial computer, allowing the CPU temperature to be cooled 4.6 °C lower than the commercial thermal pad (⊥TC ≈ 10 W m–1 K–1), which demonstrates superior heat transfer in practical thermal management applications. This research provides an efficient and convenient method to produce TIMs with high ⊥TC and low compressive modulus, which is expected to stand out in the competition of thermal management materials.