Thermal Transport in Graphene Composites: The Effect of Lateral Dimensions of Graphene Fillers
Sriharsha Sudhindra, Farnia Rashvand, Dylan Wright, Zahra Barani, Aleksey D. Drozdov, Saba Baraghani, Claudia Backes, Fariborz Kargar, Alexander A. Balandin
We report on the investigation of thermal transport in non-cured silicone composites with graphene fillers of different lateral dimensions. Graphene fillers are comprised of few-layer graphene flakes with lateral sizes in the range from 400 nm to 1200 nm and number of atomic planes from one to ~100. The distribution of the lateral dimensions and thicknesses of graphene fillers has been determined via atomic force microscopy statistics. It was found that in the examined range of the lateral dimensions the thermal conductivity of the composites increases with the increasing size of the graphene fillers. The observed difference in thermal properties can be related to the average gray phonon mean free path in graphene, which has been estimated to be around ~800 nm at room temperature. The thermal contact resistance of composites with graphene fillers of 1200-nm lateral dimensions was also smaller than that of composites with graphene fillers of 400-nm lateral dimensions. The effects of the filler loading fraction and the filler size on the thermal conductivity of the composites were rationalized within the Kanari model. The obtained results are important for optimization of graphene fillers for applications in thermal interface materials for heat removal from high-power-density electronics.
Polymer composites were manufactured using biocarbon particles as a reinforcing filler to improve the mechanical and thermal properties. However, a detailed examination of dispersion and agglomeration of filler is essential to correlate the filler matrix and the filler and filler interactions with the mechanical properties of the product. We investigated the variations of mechanical, agglomeration behaviour of fillers, and thermal properties of polypropylene coconut shell biocarbon composites. PP CSB composites were prepared by melt mixing process varying the CSB content using a Brabender mixe…
We report on the thermal and electrical properties of hybrid epoxy composites with graphene and boron nitride fillers. The thicknesses, lateral dimensions, and aspect ratios of each filler material were intentionally selected for geometric similarity to one another, in contrast to prior studies that utilized dissimilar filler geometries to achieve a "synergistic" effect. We demonstrate that the electrically-conductive graphene and electrically-insulating boron nitride fillers allow one to effectively engineer the thermal and electrical conductivities of their resulting composites. By varying t…
The thermal properties of an epoxy-based binary composites comprised of graphene and copper nanoparticles are reported. It is found that the "synergistic" filler effect, revealed as a strong enhancement of the thermal conductivity of composites with the size-dissimilar fillers, has a well-defined filler loading threshold. The thermal conductivity of composites with a moderate graphene concentration of ~15 wt% exhibits an abrupt increase as the loading of copper nanoparticles approaches ~40 wt%, followed by saturation. The effect is attributed to intercalation of spherical copper nanoparticles …
In this article we discuss in detail the effective approaches to enhance the thermal conductivity in polymer composites. It is shown from numerical simulations that maximizing interfacial area between filler and polymer enhances very significantly the effective thermal conductivity in composites. Our study outlines two main facts. (a) Although the nature of the filler's geometry plays an important role in the effective thermal conductivity, we show that among the different geometries thermal conductivity is high for those geometries for which the ratio of surface-area to volume is high. Thus n…
The incorporation of carbon nanotubes (CNTs) within polymer hosts offers a great platform for the development of advanced thermoelectric (TE) composite materials. Over the years, several CNT/polymer composite formulations have been investigated on an effort to maximize the TE performance. Meanwhile, several studies focused on the decay dynamics of the charged excitons within CNTs itself and therefrom derived structures, aiming to investigate the lifetimes and the corresponding recombination processes of free charge carriers. The latter physical phenomena play a crucial role in the performance …
Thermally expanded graphite (EG) polymer composite has high potential in modern thermoelectronic industry due to cost effectiveness, excellent electrical and thermal properties. In this study, we report that expanded graphite polyetherimide(EG/PEID) composite has been fabricated by simple solution mixing technique, reinforcing a low cost EG filler into host polymer matrix, polyetherimide (PEID). This technique enables the inclusion of 3D graphitic filler into polymer matrix retaining the worm structure of expanded graphite, thus developing continuous network throughout the composite. In result…
The paper presents a comprehensive analysis of elastic properties of polystyrene-based nanocomposites filled with different types of inclusions: small spherical particles (SiO2 and Al2O3), alumosilicates (montmorillonite, halloysite natural tubules and Mica) and carbon nanofillers (carbon black and multi-walled carbon nanotubes). Composites were fabricated by melt technology. The analysis of composite melts showed that the introduction of Montmorillonite, Multi-walled carbon nanotubes, and Al2O3 particles provided an increase in melt viscosity by an average of 2 to 5 orders of magnitude over t…
Molding compounds (MCs) have been used extensively as an encapsulation material for integrated circuits, however, MCs are susceptible to moisture and charge spreading over time. The increase in dissipation factor due to the increase of parasitic electrical conductivity (σ) and the decrease in dielectric strength (E_MC^Crit) restrict their applications. Thus, a fundamental understanding of moisture transport will suggest strategies to suppress moisture diffusion and broaden their applications. In this paper, we 1) propose a generalized effective medium and solubility (GEMS) Langmuir model to qu…
We describe a method for scalable synthesis of epoxy composites with graphene and few-layer graphene fillers, and report on the electromagnetic interference (EMI) shielding and thermal properties of such composites at elevated temperatures. The tested materials reveal excellent total EMI shielding of ~65 dB (~105 dB) at a thickness of 1 mm(~2 mm) in the X-band frequency range of f=8.2 GHz - 12.4 GHz. The room-temperature cross-plane thermal conductivity of the composite with ~19.5 vol.% of fillers was determined to be ~11.2 W/mK, which is a factor of x41 larger than that of the pristine epoxy.…
We report on the synthesis and characterization of the epoxy-based composites with the few-layer graphene fillers, which are capable of the duel functional applications. It was found that composites with the certain types of few-layer graphene fillers reveal an efficient total electromagnetic interference shielding, SE~45 dB, in the important X-band frequency range, f=8.2 GHz - 12.4 GHz, while simultaneously providing the high thermal conductivity, K = 8 W/mK, which is a factor of x35 larger than that of the base matrix material. The efficiency of the dual functional application depends on the…
We report on the synthesis of the epoxy-based composites with graphene fillers and testing their electromagnetic shielding efficiency by the quasi-optic free-space method in the extremely high frequency (EHF) band (220 - 325 GHz). The curing adhesive composites were produced by a scalable technique with a mixture of single-layer and few-layer graphene layers of a few-micron lateral dimensions. It was found that the electromagnetic transmission, T, is low even at small concentrations of graphene fillers: T<1% at frequency of 300 GHz for a composite with only 1 wt% of graphene. The main shieldin…
The global increase in materials consumption calls for innovative materials, with tailored performance and multi-functionality, that are environmentally sustainable. Composites from renewable resources offer solutions to fulfil these demands but have so far been dominated by hybrid petrochemicals-based matrixes reinforced by natural fillers. Here, we present biological matrix composites with properties comparable to wood and commercial polymers. The biocomposites are obtained from cultured, undifferentiated plant cells, dehydrated and compressed under controlled conditions, forming a lamellar …
We demonstrate the large scale exfoliation of bulk black phosphorus into few-layers black phosphorus. We use wet-jet mill (WJM) as an industrially scalable exfoliation technique. In order to avoid the degradation by oxidation of the exfoliated flakes, the few-layers black phosphorus is protected by functionalisation (with 4-bromobenzene-diazonium tetrafluoroborate) during the exfoliation process. We used the exfoliated and functionalised flakes as fillers in a polymethyl methacrylate matrix to test the mechanical endurance, obtaining an improvement in the Young modulus of 106% compared to the …
Correlations between electrical and thermal conduction in polymer composites are blurred due to the complex contribution of charge and heat carriers at the nanoscale junctions of filler particles. Conflicting reports on the lack or existence of thermal percolation in polymer composites have made it the subject of great controversy for decades. Here, we develop a generalized percolation framework that describes both electrical and thermal conductivity within a remarkably wide range of filler-to-matrix conductivity ratios (Y_f/Y_m), covering 20 orders of magnitude. Our unified theory provides a …
As one of the most promising next-generation energy storage device, lithium metal batteries have been extensively investigated. However, the poor safety issue and undesired lithium dendrites growth hinder the development of lithium metal batteries. The application of solid state electrolytes has attracted increasing attention as they can solve the safety issue and partly inhibit the growth of lithium dendrites. Polyethylene oxide (PEO)-based electrolytes are very promising due to their enhanced safety and excellent flexibility. However, PEO-based electrolytes suffer from low ionic conductivity…
Graphene is considered an ideal filler for the production of multifunctional nanocomposites; as a result, considerable efforts have been focused on the evaluation and modeling of its reinforcement characteristics. In this work, we modelled successfully the mechanical percolation phenomenon, observed on a thermoplastic elastomer (TPE) reinforced by graphene nanoplatelets (GNPs), by designing a new set of equations for filler contents below and above the percolation threshold volume fraction (Vp). The proposed micromechanical model is based on a combination of the well-established shear-lag theo…
We review the current state of the art of graphene-enhanced thermal interface materials for the management of heat the next generation of electronics. Increased integration densities, speed, and power of electronic and optoelectronic devices require thermal interface materials with substantially higher thermal conductivity, improved reliability, and lower cost. Graphene has emerged as a promising filler material that can meet the demands of future high-speed and high-powered electronics. This review describes the use of graphene as a filler in curing and non-curing polymer matrices. Special at…
Probing optical and acoustic phonons in heated nano-Si/epoxy composites
Nazarbayev University（纳扎尔巴耶夫大学）；Taras Shevchenko National University of Kyiv（基辅塔拉斯舍甫琴科国立大学）；Al-Farabi Kazakh National University（阿尔法拉比哈萨克国立大学）；INSA de Lyon（里昂国立应用科学学院）；Claude Bernard University of Lyon（里昂第一大学（克洛德·贝尔纳大学））；National Laboratory Astana（阿斯塔纳国家实验室）
The implementation of processed magnetic materials onto thermoplastics can be an approach for practical application of brittle intermetallic materials with the advantage of enlarging the range of applications. In the present work, we evaluate the effect of blending magnetocaloric Gd$_5$Si$_{2.4}$Ge$_{1.6}$ micrometric particles with 3.4 $μ$m in different weight fractions onto a flexible, transparent and non-magnetic poly(methyl methacrylate) (PMMA). A close to homogeneous grain distribution along the polymer surface were achiever by using a simple solvent casting method for evaluation of their…
This work summarizes recent progress on the thermal transport properties of three-dimensional (3D) nanostructures, with an emphasis on experimental results. Depending on the applications, different 3D nanostructures can be prepared or designed to either achieve a low thermal conductivity for thermal insulation or thermoelectric devices, or a high thermal conductivity for thermal interface materials used in the continuing miniaturization of electronics. A broad range of 3D nanostructures have been discussed, ranging from colloidal crystals/assemblies, array structures, holey structures, hierarc…
The use of graphene in a form of discontinuous flakes in polymer composites limits the full exploitation of the unique properties of graphene, thus requiring high filler loadings for achieving - for example - satisfactory electrical and mechanical properties. Herein centimetre-scale CVD graphene/polymer nanolaminates have been produced by using an iterative 'lift-off/float-on' process and have been found to outperform, for the same graphene content, state-of-the-art flake-based graphene polymer composites in terms of mechanical reinforcement and electrical properties. Most importantly these th…
Polymer composites with thermally conductive nanoscale filler particles, such as graphene and hexagonal boron nitride (h-BN), are promising for certain heat transfer applications. While graphene-polymer composites have been extensively investigated, studies on h-BN-polymer composites has been relatively rare. In this paper, we use molecular dynamics (MD) simulations to study the interfacial thermal conductance (ITC) involved in the h-BN-polymer composites. We first compare the ITC across h-BN/hexane (C6H14) interfaces to that of graphene/hexane interfaces, where we found that the electrostatic…
Materials for electronics that function as electrical and/or thermal conductors are often rigid, expensive, difficult to be sourced and sometimes toxic. An electrically and thermally conductive nanocomposite that is lightweight, flexible and eco-friendly could improve the environmental friendliness of the electronics sector and enable new applications. Considering this, we have fabricated electrically and thermally conductive flexible materials by functionalizing paper with nanocarbon conductive inks. Carnauba wax is emulsified in isopropyl alcohol and mixed with graphene nanoplatelets (GNPs) …
Composite materials where magnetic micrometer-sized particles are embedded into a compliant polymer matrix are known as magnetorheological or magnetoactive elastomers (MAEs). They are distinguished by huge variations of their physical properties in a magnetic field, which is commonly attributed to the restructuring of the filler. The process of the magnetic-field-induced restructuring in a magnetorheological elastomer is interpreted as progression towards percolation. Such a physical model was previously used to explain the dependence of the magnetic permeability and dielectric permittivity of…
Different types of graphene-related materials (GRM) are industrially available and have been exploited for thermal conductivity enhancement in polymers. These include materials with very different features, in terms of thickness, lateral size and composition, especially concerning the oxygen to carbon ratio and the possible presence of surface functionalization. Due to the variability of GRM properties, the differences in polymer nanocomposites preparation methods and the microstructures obtained, a large scatter of thermal conductivity performance is found in literature. However, detailed cor…
Two-dimensional (2D) materials have many promising applications, but their scalable production remains challenging. Herein, we develop a glue-assisted grinding exfoliation (GAGE) method in which the adhesive polymer acts as a glue to massively produce 2D materials with large lateral sizes, high quality, and high yield. Density functional theory simulation shows that the exfoliation mechanism involves the competition between the binding energy of selected polymers and the 2D materials which is larger than the exfoliation energy of the layered materials. Taking h-BN as an example, the GAGE produ…
