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.
With the rapid growth and widespread adoption of cloud services, machine learning, and artificial intelligence, thermal interface materials have become increasingly vital for efficient thermal management in electronic devices. However, traditional thermal interface materials often struggle to strike a delicate balance between adhesion performance and thermal conductivity. Here, we report a design of polymer and filler networks to fabricate a thermal interface material consisting of polydimethylsiloxane/aluminum fillers, with high adhesion performance (adhesion strength of 3.30 ± 0.26 MPa, adhesion energy of 913.2 ± 152.71 J m–2), and enhanced thermal conductivity (5.24 ± 0.26 W m–1 K–1). These merit properties stem from the optimization of both the polydimethylsiloxane and aluminum filler networks through adjustments in branching point, cross-linking fraction, and filler mass fraction. We envision that the design strategy of optimizing polymer and filler networks can be adopted in the development of thermal interface materials with desirable multifunctionality.
With heat-flux density of electronics drastically increase polymer-based thermal interface materials play a critical role in the performance of electronics. Although surface energy of fillers has been recognized as a crucial parameter, the exploitation of the filler surface energy-dependent properties is still unclear. Herein, we report on unveiling the effect of the surface energy of aluminum on thermal and mechanical properties in thermal interface materials consisted of polydimethylsiloxane and modified aluminum with silane-coupling agents containing varied chain lengths. The results show that reducing the surface energy of aluminum is beneficial to improve the aluminum fillers dispersibility in polydimethylsiloxane, leading to improved macroscopic properties, including rheology, mechanical properties, and thermal properties. Furthermore, based on the thermodynamic prediction, a winding hypothesis was proposed to explain the interaction between the modified aluminum and polydimethylsiloxane. This work provides valuable guidance for rationally designing the surface energy of fillers in thermal interface materials.
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