Balancing Interfacial Toughness and Intrinsic Dissipation for High Adhesion and Thermal Conductivity of Polymer-Based Thermal Interface Materials

In recent years, adhesive thermal interface materials have attracted much attention because of their reliable adhesion properties on most substrates, preventing moisture, vibration impact, or chemical corrosion damage to components and equipment, as well as solving the heat dissipation problem. However, thermal interface materials have a huge contradiction between strong adhesion and high thermal conductivity. Here, we report a polymer-based thermal interface material consisting of polydimethylsiloxane/spherical aluminum fillers, which possesses both adhesion properties (adhesion strength of 3.59 MPa and adhesion toughness of 1673 J m^–2 and enhanced thermal conductivity of 3.90 W m^–1 K^–1). These excellent properties are attributed to the modified chain structure by introducing acrylate accelerators into the polydimethylsiloxane network, thereby striking a balance between interfacial toughness and intrinsic dissipation. The addition of thermally conductive aluminum fillers not only increases the thermal conductivity but also improves the bulk energy dissipation of the thermal interface material. This work provides a novel strategy for designing a novel thermal interface material, leading to new ideas in long-term applications in high-power electronics.