Stretchable Thermal Interface Materials by Tailoring the Chain Relaxation at the Filler/Polymer Interface

Polymer-based thermal interface materials integrated with excellent stretchability and simultaneously high thermal conductivity would be of great use in the thermal management of next-generation chips featuring higher power density and a larger packaging size. However, combining thermal conductivity and stretchability in the same material is fundamentally challenging. Herein, in view of the important role of filler/polymer interface, we report a stretchable thermal interface material by tailoring chain relaxation through incorporating macromolecular coupling agent at the aluminum/silicone interface. Thanks to the interfacial relaxation effect, the aluminum/silicone thermal interface material exhibits a large stretchability (117%) and a high thermal conductivity (5.90 W m–1 K–1) at the aluminum weight fraction of 91 wt %. Moreover, these materials show great heat dissipation performance in practical applications, which we demonstrated by rapid heat dissipation in LED and chip. This strategy will provide an avenue to implement interface design for high-performance thermal interface materials for high-performance applications, such as high-performance computing, the Internet of Things, 5G networking, and artificial intelligence computing.