Vitrimeric phase change material facilitating 3D-structured boron nitride network for reliable thermal conductive interface materials

Phase change materials (PCMs) shows great promise as thermal interface materials (TIMs) due to their compliance and thermal management properties from solid-liquid phase transition characteristics. However, the significantly reduced thermal conductivity resulting from that randomly dispersed thermal conductive fillers susceptible to localized volume change by solid-liquid phase transition deteriorates the reliable heat transfer of TIM but is often overlooked. In this work, 3D-structured network of boron nitride (BN) fillers is created in vitrimeric PCM (vPCM) consisting of dynamic covalent crosslinking polyolefin elastomer (POE)/paraffin wax (PW) blends. The resulted composites with interconnected BN network show a through-plane thermal conductivity (κ⊥) of 3.08 W m−1 K−1 at 29.8 vol% BN. Significantly, the composites can keep the BN network continuous when heated, and remain κ⊥ of about 1.4 W m−1 K−1 after the solid-liquid phase transition of PW, which ensures reliable heat transfer when achieving thermal management by melting endotherm of PW. Moreover, the composites conform to the surface topography of sandwiching surfaces through solid plasticity under low stress when the crosslinked network rearranges via the exchange of dynamic covalent bonds activated by the melting of POE, reducing the thermal contact resistance. When the composites are used as TIM through thermally triggered reconfigurable package procedures at 80 °C and 50 kPa, the heat dissipation is better than a commercial thermal pad with κ⊥ of 3.86 W m−1 K−1. Vitrimeric PCM facilitates reliable 3D-structured BN network and thermally triggered conformability, paving a promising way for high-performance TIM with excellent heat dissipation.