Thermal Interface\nMaterials with High Adhesion and\nEnhanced Thermal Conductivity via Optimization of Polydimethylsiloxane\nNetworks and Aluminum Fillers

With\nthe rapid growth and widespread adoption of cloud\nservices,\nmachine learning, and artificial intelligence, thermal interface materials\nhave become increasingly vital for efficient thermal management in\nelectronic devices. However, traditional thermal interface materials\noften struggle to strike a delicate balance between adhesion performance\nand thermal conductivity. Here, we report a design of polymer and\nfiller networks to fabricate a thermal interface material consisting\nof polydimethyl­siloxane/aluminum fillers, with high adhesion\nperformance (adhesion strength of 3.30 ± 0.26 MPa, adhesion energy\nof 913.2 ± 152.71 J m<sup>–2</sup>), and enhanced thermal\nconductivity (5.24 ± 0.26 W m<sup>–1</sup> K<sup>–1</sup>). These merit properties stem from the optimization of both the\npolydimethyl­siloxane and aluminum filler networks through adjustments\nin branching point, cross-linking fraction, and filler mass fraction.\nWe envision that the design strategy of optimizing polymer and filler\nnetworks can be adopted in the development of thermal interface materials\nwith desirable multifunctionality.