Thermal Interface Materials with High Adhesion and Enhanced Thermal Conductivity via Optimization of Polydimethylsiloxane Networks and Aluminum Fillers

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.