Resilient Thermal Interface Materials with Low Thermal Contact Resistance and High Modulus via Hybrid Cross-Linking Strategy

Thermal interface materials (TIMs) are crucial for achieving efficient thermal management of electronic devices. Traditional TIMs require extreme compliance for low thermal contact resistance (Rc), resulting in the challenge of achieving both a high modulus and a low Rc. Here, we report a resilient (>96%) thermally conductive elastomer with a high elastic modulus (12.3 MPa) and a low Rc (12.3 K mm2 W–1) based on a dynamic/nondynamic hybrid cross-linking network strategy. The nondynamic cross-linking network serves as the backbone of the elastomer, providing elasticity and robustness, while the dynamic cross-linking network with dynamic features offers partial solid-state plasticity to reduce the Rc between the elastomer and the rigid substrate. Use of the thermally conductive elastomer as the TIM in chip cooling demonstrated superior heat dissipation capability, resulting in an 11 °C reduction in the chip temperature compared with that obtained with the commercial TIM. This work provides an effective strategy for balancing the Rc and modulus, broadening the application range of TIMs.