Tetris-Style Stacking Process to Tailor the Orientation of Carbon Fiber Scaffolds for Efficient Heat Dissipation

As the miniaturization of electronic devices and complication of electronic packaging, there are growing demands for thermal interfacial materials with enhanced thermal conductivity and the capability to direct the heat toward heat sink for highly efficient heat dissipation. Pitch-based carbon fiber (CF) with ultrahigh axial thermal conductivity and aspect ratios exhibits great potential for developing thermally conductive composites as TIMs. However, it is still hard to fabricate composites with aligned carbon fiber in a general approach to fully utilize its excellent axial thermal conductivity in specific direction. Here, three types of CF scaffolds with different oriented structure were developed via magnetic field-assisted Tetris-style stacking and carbonization process. By regulating the magnetic field direction and initial stacking density, the self-supporting CF scaffolds with horizontally aligned (HCS), diagonally aligned and vertically aligned (VCS) fibers were constructed. After embedding the polydimethylsiloxane (PDMS), the three composites exhibited unique heat transfer properties, and the HCS/PDMS and VCS/PDMS composites presented a high thermal conductivity of 42.18 and 45.01 W m(−1) K(−1) in fiber alignment direction, respectively, which were about 209 and 224 times higher than that of PDMS. The excellent thermal conductivity is mainly ascribed that the oriented CF scaffolds construct effective phonon transport pathway in the matrix. In addition, fishbone-shaped CF scaffold was also produced by multiple stacking and carbonization process, and the prepared composites exhibited a controlled heat transfer path, which can allow more versatility in the design of thermal management system. [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-023-01119-0.