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With the continuous advancement of electronic devices, there is an urgent need for advanced thermal interface materials (TIMs) to prevent high-power density electronics from overheating. The orderly arrangement of thermally conductive fillers in TIMs plays a crucial role in enhancing thermal conduction along preferred directions. However, it is challenging to control the orientation of the fillers, especially for two-dimensional fillers. In this study, graphene nanoplates (GNPs) were co-planarly arranged in polyvinyl alcohol (PVA) using a rotating magnetic field, which significantly increased the thermal conductivity of the composites. The coplanar vertically aligned GNPs/PVA (CVGNPs/PVA) exhibited a through-plane thermal conductivity of 11.78 W m−1 K−1, which is about 10 times higher than that of the composites with disorderly distributed GNPs (1.14 W m−1 K−1). The rotating magnetic field facilitated the alignment of GNPs and increased face-to-face contact between adjacent GNPs, which significantly boosted the through-plane thermal conductivity of the composite. The compressive modulus of the CVGNPs/PVA composites was only 1.06 MPa, and it helped to reduce the thermal interface resistance to 49 mm2 K W−1. These results offer a novel approach for preparing excellent TIMs that could be used in various applications. GNPs are oriented more compactly and orderly in PVA by using the rotating magnetic field, resulting in a densified thermal conductive paths and higher thermal conductivity of the composite. [Display omitted] [ABSTRACT FROM AUTHOR]

Efficient thermal interface materials (TIMs) are urgently needed for heat dissipation of high-power density electronics. In this study, vinyl polydimethylsiloxane (PDMS) composites with the spatial alignment of carbon fibers (CFs) bridged by Al 2 O 3 particles were fabricated by the flow field. The through-plane thermal conductivity (TPTC) of the composites with 24 vol% CFs and 47 vol% Al 2 O 3 loading reached 38.0 W m−1 K−1. The oriented CFs bridged by Al 2 O 3 acted as the efficient through-plane thermal conductive network. Furthermore, the effects of shape factor (b/a), spatial angle (γ) of CFs, and CF loading (V f) on the TPTC were quantitatively discussed by steady-state finite element simulation combined with micro-computed tomography and machine learning. The positive contribution of the increased V f to TPTC was in competition with the negative contribution of b/a and γ , both of which increased with the increase of V f. Moreover, b/a exerted more negative effects than γ. The PDMS composites demonstrated excellent thermal stability (T d = 407.5 °C, CTE = −55.3 × 10−6 K−1), low compress modulus (1.71 MPa), and hardness (47 (Shore C)), which made them potential candidates for TIMs. This work offers a feasible method to prepare TIMs on large scale and refreshes the thermal conduction mechanism of TIMs by introducing the influencing factors (b/a and γ). [Display omitted] • Efficient heat conduction paths were constructed by spatial alignment of CFs bridged by Al 2 O 3. • The through-plane thermal conductivity of PDMS composites reached 38 W m−1 K−1. • The effect of spatial orientation angle of CFs on the thermal conduction property was revealed. • The PDMS composites with excellent comprehensive properties can be used as TIMs. [ABSTRACT FROM AUTHOR]

[Display omitted] • Magnetized carbon fibers (MCF) were vertically arranged in silicone rubber (SR) in magnetic field. • The λ of SR composites demonstrated an unusual power-law growth with the increase of MCF. • The o-MCF/SR-9 vol% composite exhibited a high λ of 4.72 W/(m·K) with 2045.5 % enhancement. • A new parameter, "shape factor", was introduced to reveal the heat conduction mechanism. The continual increase in power density and consumption of modern electronic devices calls for high-performance thermal interface materials (TIMs). In this work, silicone rubber composites with vertically oriented magnetic carbon fibers (o-MCF/SR) were successfully prepared via the cast molding and filler orientation upon uniform magnetic field in a vacuum environment. The through-plane thermal conductivity of o-MCF/SR composites showed an unusual power-law growth with increasing MCF loading. At a 9 vol% MCF loading, the o-MCF/SR composite exhibited a maximum through-plane thermal conductivity of 4.72 W/(m·K) with 2045.5 % TCE, about 3.55 W/(m·K) higher than that of SR composites with randomly dispersed MCF (λ = 1.17 W/(m·K), TCE = 431.8 %). To reveal the underlying through-plane heat conduction mechanism of o-MCF/SR composites, finite element simulation combined with classical effective medium theory model and machine learning method was used. A homogeneous unit fiber-filled composite (HUFC) was modelled, and a new parameter influencing the through-plane thermal conductivity, i.e. , shape factor (b / a), was introduced here for the first time. Theoretically, this shape factor was dependent on the filler content and indirectly reflected the assembly of matrix and 1D filler in HUFC fit to a parallel-series hybrid model. Furthermore, a decrease of b / a was practically found with increasing MCF loading, and the dominant series-type assembly gradually transformed to parallel-type assembly of the o-MCF/SR composites. This work not only developed a method to fabricate desirable TIMs that hold great promise for advanced thermal management, but also introduced a new parameter to reveal the underlying mechanism for heat conduction capacity of polymer composites. [ABSTRACT FROM AUTHOR]

Currently, epoxy-based composites are widely used in thermal management. However, with the development of complex and high power-density electronic devices, the thermal properties of the composites need to be improved. Inspired by the unique galls-leaf structure of Distylium chinense, a graphene-diamond framework (GRDF) is developed by a simple filtration method. A through-plane and in-plane thermal conductivity of 22.7 and 21.8 Wm−1 K−1, respectively, have been achieved by forming epoxy-based composites with the GRDF annealed at 3000 °C. The result is 70% higher than the best-reported value for epoxy-based composites prepared by vacuum filtration under a filler content of 43 wt%. Such high thermal conductivity remains unchanged (within 2%) in a temperature range from 25 to 100 °C. Based on various microscopic characterizations, the diamond particles evenly distribute in a framework formed by graphene sheets, which bridge the gaps in the framework and improve its structural integrity. High-temperature annealing converts most diamond particles to graphite, which further enhances the thermal properties of the composite. The observations provide a feasible way for developing polymer-based composite with high thermal conductivity, which could meet the ever-increasing demands for heat dissipation in high-power electronics. [Display omitted] • The epoxy composite with a through-plane thermal conductivity of 22.7 Wm−1K−1 is achieved under 43.2 wt.% filler filling. • The composites show a high degree of isotropic thermal properties, and a good thermal stability. • The high thermal conductivity of the composite is due to diamond filling and high-temperature graphitization. [ABSTRACT FROM AUTHOR]

A review of carbon-based thermal interface materials: mechanisms, thermal measurements and thermal properties. [Display omitted] • Various carbon-based thermal interface materials were reviewed, ranging from one-dimensional carbon nanotubes, two-dimensional graphene films, to three-dimensional graphene foams, graphene aerogels, vertical graphene and other 3D graphene. • Thermal measurements for bulk and nanoscale materials were discussed to offer a guidance for improving the precision of the results. • The challenges for carbon-based thermal interface materials were discussed, including how to decrease the overall thermal resistance of thermal interface materials, the potential applications from micro to macro devices and the prerequisites for industrial application. With the development of electronic technologies, electronic devices become smaller, while their power density increases dramatically. The resulting excessive heat requires excellent heat dissipation to ensure great performance of the devices. A good thermal interface material (TIM), with excellent bulk thermal conductivity and proper elastic modulus, which can fill the gap between contact surfaces, is of great importance to improve overall performance of thermal management in the electronic devices. Carbon-based materials, such as carbon nanotubes (CNTs) and graphene (Gr), have attracted great attentions, due to their intrinsic high thermal conductivity. In this paper, carbon-based TIMs are reviewed, as well as the thermal conducting mechanisms and techniques to measure thermal properties for materials. The unique three-dimensional network of 3D-Gr provides not only high thermal conductivity, but also excellent mechanical properties, which makes it more competitive as TIM than CNTs and Gr. Furthermore, there is currently no universal characterization techniques, which are suitable to measure thermal properties of all TIMs. Hence, special attention must be paid to select a proper technique based on the measuring principle, in order to obtain accurate results. An outlook of the future challenges of the thermal interface materials is proposed at the end of the paper. [ABSTRACT FROM AUTHOR]