Analytical heat conduction model of particle reinforced tertiary composite materials based on complete spatial randomness of fillers in base matrix and its application in the development of cryosorption pump

In this article, we propose an analytical heat conduction model within a stochastic frame work which estimates the thermal conductivity (TC) value of particle reinforced composite materials comprising of three parent elements i.e. a base matrix along with two different filler element particles randomly distributed in it. The spatial distribution of the filler particles in a sample of specific dimension has been estimated by applying bivariate Poisson distribution. This distribution is then used to arrive at the TC value of the composite. This concept has been applied to predict the TC of the tertiary composite comprised of epoxy as the base matrix, aluminium and zinc particles as filler elements. The TC values obtained from this model for different volume fractions of fillers were extensively compared with experimental results. The model is found to predict the results fairly well with less aberrations up to the total filler volume fraction of ∼20%. The developed model for TC prediction has been used in the design of high efficiency cryosorption pump where the adhesive material used is Epoxy-Aluminium -Zinc composite.     

Enhancement of tensile and thermal properties of epoxy nanocomposites through chemical hybridization of carbon nanotubes and alumina

This paper presents the properties of epoxy nanocomposites, prepared using a synthesized hybrid carbon nanotube–alumina (CNT–Al₂O₃) filler, via chemical vapour deposition and a physically mixed CNT–Al₂O₃ filler, at various filler loadings (i.e., 1–5%). The tensile and thermal properties of both nanocomposites were investigated at different weight percentages of filler loading. The CNT–Al₂O₃ hybrid epoxy composites showed higher tensile and thermal properties than the CNT–Al₂O₃ physically mixed epoxy composites. This increase was associated with the homogenous dispersion of CNT–Al₂O₃ particle filler; as observed under a field emission scanning electron microscope. It was demonstrated that the CNT–Al₂O₃ hybrid epoxy composites are capable of increasing tensile strength by up to 30%, giving a tensile modulus of 39%, thermal conductivity of 20%, and a glass transition temperature value of 25%, when compared to a neat epoxy composite.     

The thermal conductivity of embedded nano-aluminum nitride-doped multi-walled carbon nanotubes in epoxy composites containing micro-aluminum nitride particles

Amino-functionalized nano-aluminum nitride (nano-AlN) particles were doped onto the surfaces of chlorinated multi-walled carbon nanotubes (MWCNTs) to act as fillers in thermally conducting composites. These synthesized materials were embedded in epoxy resin. Then, the untreated micro-aluminum nitride (micro-AlN) particles were added to this resin, whereby the composites filled with nano-AlN-doped MWCNTs (0, 0.5, 1, 1.5, 2 wt%) and micro-AlN (25.2, 44.1, 57.4 vol%) were fabricated. As a result, the thermal diffusivity and conductivity of all composites continuously improved with increasing nano-AlN-doped MWCNT content and micro-AlN filler loading. The thermal conductivity reached its maximum, which was 31.27 times that of the epoxy alone, when 2 wt% nano-AlN-doped MWCNTs and 57.4 vol% micro-AlN were added to the epoxy resin. This result is due to the high aspect ratio of the MWCNTs and the surface polarity of the doped nano-AlN and micro-AlN particles, resulting in the improved thermal properties of the epoxy composite.     

Tensile,dielectric, and thermal properties of epoxy composites filled with silica,mica, and calcium carbonate

The minerals silica, mica, and calcium carbonate (CaCO₃) were used as fillers to produce epoxy thin film composites for capacitor application. The effects of filler loading and type on the morphology, tensile, dielectric, and thermal properties of the epoxy thin film composites were determined. Results showed that epoxy thin films with 20 vol% filler loading showed good dielectric properties, thermal conductivity, and thermal stability. However, the tensile properties of the thin films were reduced as the filler loading was increased due to brittleness. Dielectric constant and dielectric loss of epoxy/inorganic composite films generally increased with increasing mineral filler loading. Meanwhile, the presence of mineral filler improved the thermal stability of the thin film composites. The highest dielectric constant of 5.75 with 20 vol% filler loading at a frequency of 1 MHz was exhibited by the epoxy/CaCO₃ composite, followed by epoxy/mica and epoxy/silica. Therefore, the epoxy/CaCO₃ composite is the most potential candidate for capacitor application. Moreover, precipitated CaCO₃ provided better tensile properties and slightly improved the dielectric properties compared with mineral CaCO₃.     

Prerequisite for maximizing thermal conductivity of epoxy laminate using filler

Boron nitride-filled epoxy laminate with excellent thermal conductivity was prepared. Its thermal conductivity was enhanced through sliane surface treatment prior to mixing the epoxy. The lamination enhanced thermal conductivity of the boron nitride filled epoxy by 20 % by reducing the voids in the structure. The heat conduction mechanism in laminated board, i.e. BN, glass fabric and epoxy, is not the same as a simpler BN-epoxy system, even though thermal conductivity of epoxy laminate is mainly affected by filler size and contents, as in the case of BN-epoxy composite. This study provides evidence of the importance of temperature and pressure after surface engineering of boron nitride for fabricating high thermal conductivity laminates, establishing the prerequisites for maximizing thermal conductivity of BN-epoxy laminate. The infrared thermogram showed that the BN-laminate can effectively lower the temperature of a surface mounted LED by 12.5 °C compared to the traditional FR4. According to the IESNA LM 80 lifetime testing method, this reduction in LED temperature is equivalent to increasing the LED’s lifetime by 21,000 h.     

Thermal conductivity of liquid crystalline epoxy/BN filler composites having ordered network structure

BN filler was added to a liquid crystalline (LC) epoxy resin to obtain a high thermal conductive material. The LC epoxy/BN composites, which were cured at different temperatures, formed an isotropic or LC polydomain phase structure. The relationship between the network orientation containing mesogenic groups and the dispersibility of the BN filler was discussed. As a result, the thermal conductivity of the LC polydomain system was drastically enhanced even at a relatively low volume fraction of BN (30 vol%), regardless of the fact that both the LC and isotropic phase systems consisted of the same resin and filler content combination. This result is due to the formation of thermal conductive paths by the BN filler by exclusion of the BN filler from the LC domain formed during the curing process in the composite having the LC polydomain matrix.     

氧化锌晶须/环氧树脂导热绝缘复合材料的制备与性能

以环氧树脂(E-44)为聚合物基体,四针状氧化锌晶须(ZnOw)为填充材料,制备了氧化锌晶须/环氧树脂导热绝缘复合材料,研究了ZnOw含量对复合材料的导热性能、电性能的影响,并用扫描电子显微镜对断口形貌进行了观察。结果表明,较少量ZnOw的加入(体积分数<10%),复合材料的导热性能得到有效改善,但仍维持了聚合物材料所具有的电绝缘和低介电常数、低介电损耗的特点。其中当ZnOw体积分数为10%时,ZnOw/EP复合材料的热导率达到0.68W/(m·K),相比纯环氧树脂提高了3倍。     

BN表面改性对BN/环氧树脂复合材料导热性能的影响

采用十八烷基三甲基溴化铵（OTAB）阳离子表面活性剂对BN微米片进行有机化改性,研究了BN表面改性对BN/环氧树脂复合材料导热性能的影响。当OTAB浓度为0.6 g · L^-1时,BN表面的OTAB吸附量接近饱和。BN表面改性提高了环氧树脂对BN的浸润性,降低了BN的导热系数。SEM观察及黏度测试结果表明：BN表面改性改善了BN/环氧树脂复合材料的界面性能及体系相容性。由于界面热阻的降低,改性BN/环氧树脂复合材料的导热系数高于未改性BN/环氧树脂复合材料,当BN填充量为30%（填料与树脂基体的质量比）时,改性BN/环氧树脂复合材料的导热系数为1.03 W （m · K）^-1,是未改性BN/环氧树脂导热系数（0.48 W （m · K）^-1）的2.15倍。     

Fabrication, thermal, and dielectric properties of self-passivated Al/epoxy nanocomposites

The current paper reports the effects of an epoxide-functionalized, silane surface-treated, self-passivated aluminum (Al) nanoparticles on the glass transition, morphology, thermal conductivity, dielectric properties of an epoxy composite. The surface modification of the Al nanoparticles improved the dispersion of the filler, as well as the glass transition temperature, thermal conductivity, and dielectric properties of the epoxy composites. The epoxy/Al nanocomposites showed a dielectric constant transition concentration. The dielectric constant and dissipation factor increased when the Al particle loading exceeded the critical content but gradually decreased with the frequency. The epoxy nanocomposites containing 15 % by weight Al nanoparticles have a high thermal conductivity and a high dielectric constant but a low dissipation factor. The enhancements in the thermal and dielectric properties of the epoxy nanocomposites show potential for future engineering applications.     

Carbon black/graphite nanoplatelet/rubbery epoxy hybrid composites for thermal interface applications

Hybrid composites were developed by dispersing carbon black (CB) nanoparticles and graphite nanoplatelets (GNPs) at 4–6 and 12–14 wt%, respectively, into rubbery epoxy resin. SEM analysis showed that CB particles improved the dispersion of GNPs in the hybrid composite. The thermal conductivity of 4 wt% CB/14 wt% GNP-15/rubbery epoxy hybrid composite, 0.81 W/m K, is ca. four times higher than that of rubbery epoxy. When silane-functionalised, the fillers reduced the viscosity of the hybrid dispersion and made the hybrid composite highly electrically insulating. Nevertheless, filler functionalisation decreased the composite’s thermal conductivity by only 16.6%. Compression testing showed that the hybrid fillers increased the compressive modulus and strength of rubbery epoxy by nearly two and three times, respectively. Overall, the hybrid composites with their thermal paste-type morphology, low viscosity, high compliance, improved thermal conductivity and, when fillers are functionalised, low electrical conductivity makes them promising materials as thermal interface adhesives.     

Synergetic effect of hybrid boron nitride and multi-walled carbon nanotubes on the thermal conductivity of epoxy composites

This study investigates the synergistic effect of combining multi-walled carbon nanotubes (MWCNTs) and boron nitride (BN) flakes on thermally conductive epoxy composite. The surface of the two fillers was functionalized to form covalent bonds between the epoxy and filler, thereby reducing thermal interfacial resistance. The hybrid filler provided significant enhancement of thermal conductivity, adding 30 vol% modified BN and 1 vol% functionalized MWCNTs achieving a 743% increase in thermal conductivity (1.913 W mK⁻¹, compared to 0.2267 W mK⁻¹ of neat epoxy).     

A Study on Microsized Titanium Oxide-Filled Epoxy with Enhanced Heat Conductivity for Microelectronic Applications

This article presents a study on the thermal conductivity characterization of microsized TiO₂-filled epoxy composites. Titanium oxide (TiO₂) particles of about 100 µm mean size are embedded in epoxy resin to develop composites by hand layup technique. Effective thermal conductivity values of these samples are measured using Unitherm Model 2022 in accordance with ASTM-E 1530 standards. The measured values are then compared with those obtained from a mathematical correlation deduced basing upon a one-dimensional heat conduction model developed by the authors previously. This study reveals that there is a significant improvement in thermal conductivity of the composites with increase in TiO₂ content. With addition of 25 vol% of TiO_2, the thermal conductivity of epoxy composite improves by about 223%. On comparing the measured conductivity values with those obtained from the theoretical model, it has been observed that the measured values are in very good agreement with the theoretical values for low filler concentrations (0–17.5 vol%). It is further seen that TiO₂ particles show percolation behavior in epoxy matrix at about 17.5 vol% of filler content at which a sudden jump in the conductivity value is noticed.     

电器封装用高效导热/阻燃环氧复合材料的制备

目的为了提高电器封装材料的安全性,制备出一种具有高效导热/阻燃的环氧复合材料。方法通过原位聚合法,采用三聚氰胺-甲醛树脂预聚体(MF)修饰石墨烯(G)/磷烯(BP)合成纳米填料,辅以环氧树脂(E51)制备高导热/阻燃的环氧复合材料。通过TGA、热线法和锥形量热法分别测试复合材料的热稳定性、导热性和阻燃性。结果研究结果表明,当MF@BP/G的质量分数为3%时,环氧复合材料的残碳量高达22.19%,相较于纯的环氧复合材料提升了76.77%;导热系数提升至0.257 W/(m∙K),提升率为27.86%;峰值热释放率、总的热释放量、峰值烟雾释放率和总的烟雾释放量分别下降了43.76%,27.72%,46.81%和28.83%。结论以MF@BP/G为功能填料,可以有效提高环氧复合材料的导热性和阻燃性,有利于提升环氧复合材料的使用安全性。     

Thermal conductivity of ceramic particle filled polymer composites and theoretical predictions

Models and theories for predicting the thermal conductivity of polymer composites were discussed. Effective Medium Theory (EMT), Agari model and Nielsen model respectively are introduced and are applied as predictions for the thermal conductivity of ceramic particle filled polymer composites. Thermal conductivity of experimentally prepared Si₃N₄/epoxy composite and some data cited from the literature are discussed using the above theories. Feasibility of the three methods as a prediction in the whole volume fraction region of the filler from 0 to 1 was evaluated for a comparison. As a conclusion: both EMT and Nielsen model can give a well prediction for the thermal conductivity at a low volume fraction of the filler; Agari model give a better prediction in the whole range, but with larger error percentage.     

Effect of the addition of milled carbon fiber as a secondary filler on the electrical conductivity of graphite/epoxy composites for electrical conductive material

In this work, carbon composite bipolar plates consisting of synthetic graphite and milled carbon fibers as a conductive filler and epoxy as a polymer matrix developed using compression molding is described. The highest electrical conductivity obtained from the described material is 69.8 S/cm for the in-plane conductivity and 50.34 S/cm for the through-plane conductivity for the composite containing 2 wt.% carbon fiber (CF) with 80 wt.% filler loading. This value is 30% greater than the electrical conductivity of a typical graphite/epoxy composite with 80 wt.% filler loading, which is 53 S/cm for the in-plane conductivity and 40 S/cm for the through-plane conductivity. The flexural strength is increased to 36.28 MPa compared to a single filler system, which is approximately 25.22 MPa. This study also found that the General Effective Media (GEM) model was able to predict the in-plane and through-plane electrical conductivities for single filler and multiple filler composites.     

Thermal,mechanical, and conductivity properties of cyanate ester composites

Cyanate ester resins have been widely proposed as replacements for epoxy resins in high temperature applications. One such application, semiconductor encapsulation, uses a large amount of inorganic filler, typically 65 wt%. The effect of filler incorporation, on the properties of cyanate ester composites, was assessed incrementally in this work.It was found that, as is the case with epoxy based encapsulants, silica filler increased cyanate ester composite thermal conductivity, Young's modulus, and dielectric constant (slightly), and decreased encapsulant thermal expansion. It was also found that silica addition resulted in a marginal decrease in strength. This indicated a high degree of interfacial adhesion between the untreated silica filler and the cyanate ester matrix, a conclusion supported by work by Possart et al. [1].     

Facile orientation of unmodified BN nanosheets in polysiloxane/BN composite films using a high magnetic field

Composite films consisting of highly oriented boron nitride (BN) nanosheets in polysiloxane were fabricated without modifying the BN surface by applying a high magnetic field generated by a superconducting magnet. The hexagonal BN nanosheets were dispersed by sonication in a prepolymer mixture of polysiloxane. The homogeneous suspension was then cast on a polyamide spacer of microscale thickness and a magnetic field was applied before the mixture became crosslinked. The BN nanosheets in the polysiloxane were aligned with high anisotropy either parallel or perpendicular to the composite film plane depending on the magnetic flux direction. The fabricated composite films exhibited enhanced thermal conductivity by controlling the anisotropy of the BN nanosheets in the film. The mechanisms for rotation of BN nanosheets and heat diffusion across the composite film are discussed.     

三维网状石墨烯/环氧树脂热界面复合材料的制备和热性能

三维网状石墨烯/环氧树脂热界面复合材料由于具有良好的热导性能和力学性能,而被广泛应用于微电子器件领域。但是通过化学剥离-还原法制备石墨烯,在填加石墨烯质量分数相同的条件下,石墨烯/环氧树脂热界面复合材料的热导率差别仍然很大。研究发现这主要是由于石墨烯表面官能团含量不同所导致的,因此很难建立统一的标准评估石墨烯作为导热填料的作用效果。为了避免表面官能团对石墨烯/环氧树脂复合物热导率的影响,本研究小组采用化学气相沉积法制备的三维网状石墨烯作为导热填料,对环氧树脂进行修饰,制备了一系列石墨烯/环氧树脂材料。通过研究三维网状石墨烯含量对石墨烯/环氧树脂材料热导率、力学性能及热导率在高温条件下稳定性的影响,有助于完善石墨烯修饰的环氧树脂热界面复合材料的研究,并建立石墨烯作为导热填料的评价体系。     

Influence of the Kapitza resistance on the thermal conductivity of filled epoxies

The thermal conductivity of epoxy resins filled with copper powder was measured as a function of grain size and filler concentration between 1.5 and 20 K. In addition, the thermal boundary layer resistance (Kapitza resistance) between epoxy resin and copper was measured. As a consequence of this resistance the thermal conductivity is strongly dependent on grain size in the lower temperature range. Below a characteristic temperature dependent on grain size, thermal conductivity is reduced by adding filler. A simple formula is presented for calculation of the thermal conductivity of filled resins.     

Magnetically-functionalized self-aligning graphene fillers for high-efficiency thermal management applications

We report on heat conduction properties of thermal interface materials with self-aligning “magnetic graphene” fillers. Graphene enhanced nano-composites were synthesized by an inexpensive and scalable technique based on liquid-phase exfoliation. Functionalization of graphene and few-layer-graphene flakes with Fe₃O₄ nanoparticles allowed us to align the fillers in an external magnetic field during dispersion of the thermal paste to the connecting surfaces. The filler alignment results in a strong increase of the apparent thermal conductivity and thermal diffusivity through the layer of nano-composite inserted between two metallic surfaces. The self-aligning “magnetic graphene” fillers improve heat conduction in composites with both curing and non-curing matrix materials. The thermal conductivity enhancement with the oriented fillers is a factor of two larger than that with the random fillers even at the low ~ 1 wt.% of graphene loading. The real-life testing with computer chips demonstrated the temperature rise decrease by as much as 10 °C with use of the non-curing thermal interface material with ~ 1 wt.% of the oriented fillers. Our proof-of-concept experiments suggest that the thermal interface materials with functionalized graphene and few-layer-graphene fillers, which can be oriented during the composite application to the surfaces, can lead to a new method of thermal management of advanced electronics.