A Novel Thermal Interface Material Composed of Vertically Aligned Boron Nitride and Graphite Films for Ultrahigh Through-Plane Thermal Conductivity.

The relentless drive toward miniaturization in microelectronic devices has sparked an urgent need for materials that offer both high thermal conductivity (TC) and excellent electrical insulation. Thermal interface materials (TIMs) possessing these dual attributes are highly sought after for modern electronics, but achieving such a combination has proven to be a formidable challenge. In this study, a cutting-edge solution is presented by developing boron nitride (BN) and graphite films layered silicone rubber composites with exceptional TC and electrical insulation properties. Through a carefully devised stacking-cutting method, the high orientation degree of both BN and graphite films is successfully preserved, resulting in an unprecedented through-plane TC of 23.7 Wm-1 K-1 and a remarkably low compressive modulus of 4.85 MPa. Furthermore, the exceptional properties of composites, including low thermal resistance and high resilience rate, make them a reliable and durable option for various applications. Practical tests demonstrate their outstanding heat dissipation performance, significantly reducing CPU temperatures in a computer cooling system. This research work unveils the possible upper limit of TC in BN-based TIMs and paves the way for their large-scale practical implementation, particularly in the thermal management of next-generation electronic devices.

Thermally Conductive and Electrically Insulating Epoxy Composites Filled with Network-like Alumina In Situ Coated Graphene.

With the rapid development of the electronics industry, there is a growing demand for packaging materials that possess both high thermal conductivity (TC) and low electrical conductivity (EC). However, traditional insulating fillers such as boron nitride, aluminum nitride, and alumina (Al2O3) have relatively low intrinsic TC. When graphene, which exhibits both superhigh TC and EC, is used as a filler to fill epoxy resin, the TC of blends can be much higher than that of blends containing more traditional fillers. However, the high EC of graphene limits its application in cases where electrical insulation is required. To address this challenge, a method for coating graphene sheets with an in situ grown Al2O3 layer has been proposed for the fabrication of epoxy-based composites with both high TC and low EC. In the presence of a cationic surfactant, a dense Al2O3 layer with a network structure can be formed on the surface of graphene sheets. When the total content of Al2O3 and graphene mixed filler reached 30 wt%, the TC of the epoxy composite reached 0.97 W m-1 K-1, while the EC remained above 1011 Ω·cm. Finite element simulations accurately predicted TC and EC values in accordance with experimental results. This material, with its combination of high TC and good insulation properties, exhibits excellent potential for microelectronic packaging applications.

Vertical Alignment of Anisotropic Fillers Assisted by Expansion Flow in Polymer Composites.

Orientation control of anisotropic one-dimensional (1D) and two-dimensional (2D) materials in solutions is of great importance in many fields ranging from structural materials design, the thermal management, to energy storage. Achieving fine control of vertical alignment of anisotropic fillers (such as graphene, boron nitride (BN), and carbon fiber) remains challenging. This work presents a universal and scalable method for constructing vertically aligned structures of anisotropic fillers in composites assisted by the expansion flow (using 2D BN platelets as a proof-of-concept). BN platelets in the silicone gel strip are oriented in a curved shape that includes vertical alignment in the central area and horizontal alignment close to strip surfaces. Due to the vertical orientation of BN in the central area of strips, a through-plane thermal conductivity as high as 5.65 W m-1 K-1 was obtained, which can be further improved to 6.54 W m-1 K-1 by combining BN and pitch-based carbon fibers. The expansion-flow-assisted alignment can be extended to the manufacture of a variety of polymer composites filled with 1D and 2D materials, which can find wide applications in batteries, electronics, and energy storage devices.

Highly Anisotropic Thermal Conductivity of Three-Dimensional Printed Boron Nitride-Filled Thermoplastic Polyurethane Composites: Effects of Size, Orientation, Viscosity, and Voids.

Extrusion-based three-dimensional (3D) printing techniques usually exhibit anisotropic thermal, mechanical, and electric properties due to the shearing-induced alignment during extrusion. However, the transformation from the extrusion to stacking process is always neglected and its influence on the final properties remains ambiguous. In this work, we adopt two different sized boron nitride (BN) sheets, namely, small-sized BN (S-BN) and large-sized BN (L-BN), to explore their impact on the orientation degree, morphology, and final anisotropic thermal conductivity (TC) of thermoplastic polyurethane (TPU) composites by fused deposition modeling. The transformation from one-dimensional axial alignment in the extruded filament to two-dimensional alignment (horizontal and vertical alignment) in the stacking filament of BN sheets is observed, and its impact on anisotropic TC in three directions is clarified. It is found that L-BN/TPU composites show a high TC of 6.45 W m-1 K-1 at 60 wt % BN content along the printing direction, while at a lower content (<40 wt %), S-BN/TPU composites exhibit a higher TC than L-BN/TPU composites. Effects of orientation, viscosity, and voids are comprehensively considered to elucidate such differences. Finally, heat dissipation tests demonstrate the great potential of 3D printed BN/TPU composites to be used in thermal management applications.

Highly Thermally Conductive 3D Printed Graphene Filled Polymer Composites for Scalable Thermal Management Applications.

Efficient thermal transportation in a preferred direction is highly favorable for thermal management issues. The combination of 3D printing and two-dimensional (2D) materials such as graphene, BN, and so on enables infinite possibilities for hierarchically aligned structure programming. In this work, we report the formation of the asymmetrically aligned structure of graphene filled thermoplastic polyurethane (TPU) composites during 3D printing process. The as-printed vertically aligned structure demonstrates a through-plane thermal conductivity (TC) up to 12 W m-1 K-1 at 45 wt % graphene content, which is ∼8 times of that of a horizontally printed structure and surpasses many of the traditional particle reinforced polymer composites. The superior TC is mainly attributed to the anisotropic structure design that benefited from the preferable degree of orientation of graphene and the multiscale dense structure realized by finely controlling the printing parameters. Finite element method (FEM) confirms the essential impact of anisotropic TC design for highly thermal conductive composites. This study provides an effective way to develop 3D printed graphene-based polymer composites for scalable thermal-related applications such as battery thermal management, electric packaging, and so on.