Thermal stress resulting from excessive temperatures is a major cause of electronic device failure. In this work, with easy installation and good interface adaptability, Phase Change Thermal Interface Materials (PCTIMs) which possess high thermal conductivity were prepared. By incorporating phase change material stearic acid (SA) into the thermal interface material, the instantaneous heat absorption during the solid-liquid phase transition of SA effectively alleviates the problem of instantaneous high heat flux impacting electronic devices. Additionally, the solid-liquid transition reduces the modulus of TIMs, thereby minimizing the contact thermal resistance between the heat source and the heat sink during mechanical installation. To further enhance performance, the thermal interface material utilizes a dynamically cross-linked polyolefin elastomer (POE) with borate bonds, which effectively restricts the flow of SA even at its phase change point due to the three-dimensional cross-linked framework. By constructing a thermal conductive network using carbon fibers and aluminum nitride of different dimensions, the thermal conductivity of the thermal interface material reached 1.82 W∙m−1K−1 with a filler content of only 30 vol % . At 70 °C, with a force of 50 N applied to a sample area of 400 mm², the contact thermal resistance was only 2.39×10−4 K∙m2W−1. Furthermore, the PCTIMs exhibits excellent self-healing ability under thermal conditions, assuring the permanent encapsulation of small electronic devices.
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