Abstract

Interface thermal resistance has become a crucial barrier to effective thermal management in high-performance electronics and sensors. The growing complexity of operational conditions, such as irregular and dynamic surfaces, demands thermal interface materials (TIMs) to possess high thermal conductivity and soft elasticity. However, developing materials that simultaneously combine soft elasticity and high thermal conductivity remains a challenging task. Herein, we utilize a vertically oriented graphene aerogel (VGA) and rationally design liquid metal (LM) networks to achieve directional and adjustable pathways within the composite. Subsequently, we leverage the advantages of the low elastic modulus and high deformation capabilities of brush-shaped polydimethylsiloxane (BPDMS), together with the bicontinuous thermal conduction path constructed by VGA and LM networks. Ultimately, the designed composite of patterned liquid metal/vertically oriented graphene aerogel/brush-shaped PDMS (LM-VGA/BPDMS) shows a high thermal conductivity (7.11 W m-1 K-1), an ultra-low elastic modulus (10.13 kPa), excellent resilience, and a low interface thermal resistance (14.1 K mm2 W-1). This LM-VGA/BPDMS soft composite showcases a stable heat dissipation capability at dynamically changing interfaces, as well as excellent adaptability to different irregular surfaces. This strategy holds important application prospects in the fields of interface thermal management and thermal sensing in extremely complex environments.

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