Thermal Interface Engineering in a 3D-Structured Carbon Framework for a Phase-Change Composite with High Thermal Conductivity

Phase-change materials (PCMs) are promising thermal storage medium for thermal management due to their efficient thermal energy harvesting capabilities. However, the low thermal conductivity (TC) and poor shape stability of PCMs have hindered their practical applications. Construction of an interconnected three-dimensional (3D) heat-conductive structure is an effective way to build phonon conduits and provide PCM confinement. Phonon scattering at the interface is an unavoidable effect that undermines the TC improvement in the PCM composite and necessitates careful engineering. This study focuses on creating a highly thermally conductive 3D carbon-bonded graphite fiber (CBGF) network to enhance the TC of the PCM, with attention especially on thermal interface engineering considering both filler–matrix (F–M) and filler–filler (F–F) interfaces. The composite with an optimized proportion of F–M and F–F interface area achieves the highest TC of 45.48 W·m –1 ·K –1, which is 188.5 times higher than that of the pure PCM, and a high TC enhancement per volume fraction of the filler (TCEF) of 831% per 1 vol % loading. This also results in an enhanced spatial construction for PCM confinement during the phase change. The results emphasize the significance of interface engineering in creating high-TC and form-stable phase-change composites, providing insightful guidance for rational structural design.