Tailoring of thermal and dielectric properties of LDPE-matrix composites by the volume fraction,density, and surface modification of hollow glass microsphere filler

Hollow glass microsphere (HGM) filled low-density polyethylene (LDPE) composites were prepared, and the effects of density, content, and surface modification of HGM on the thermal and dielectric properties of the composites were investigated. It is found that the thermal conductivity of the composites decreases with increasing HGM content or decreasing HGM density. At the same HGM content and density, the composites filled with suitable amount of silane coupling agent (KH570) modified HGM exhibit higher thermal conductivity than unmodified-HGM filled composites. The dielectric constant at 1 MHz of the composites also decreases with increasing HGM content or decreasing HGM density, but their dielectric loss increases with increasing HGM content or increasing HGM density. By modifying the surface of HGM with suitable amount of KH570, the dielectric constant and loss at 1 MHz of the composites can be decreased at the same time. The results of microwave dielectric properties of the composites indicate that the dielectric constant decreases with increasing HGM content or decreasing HGM density, the quality factor (Q × f) decreases with increasing HGM content or increasing HGM density, but both dielectric constant and quality factor are slightly affected by the surface modification of HGM. Due to lower intrinsic thermal conductivity and dielectric constant but higher dielectric loss of HGM than LDPE, the thermal conductivity and dielectric properties of the composites can be controlled with adding HGM and varying its volume fraction. The surface modification of HGM improves the interface contact between HGM and LDPE in the composites, which is confirmed by the SEM observation, and thus the heat conduction and dielectric properties at low frequency are improved. Based on calculated thermal conductivity and dielectric constant of HGM, the experimental trends of thermal conductivity and dielectric constant at 1 MHz of the composites are analyzed by using different models, including typical models for particles-filled composites and special models developed for hollow microsphere filled composites. The results from suitable models show close correlation with the experimental values.     

Thermal conductivity and dielectric properties of Al/PVDF composites

Polymeric composites with relatively high thermal conductivity, high dielectric permittivity, and a low dissipation factor are obtained in the present study. Three types of core-shell-structured aluminum (Al) particles are incorporated in poly(vinylidene fluoride) (PVDF) by melt-mixing and hot-pressing processes. The morphological, thermal, and dielectric properties of the composites are characterized using thermal analysis, a scanning electron microscope, and a dielectric analyzer. The results indicate that the Al particles decrease the degree of crystallinity of PVDF, and that the particle size and shape of the filler affect the thermal conductivity and dielectric properties of Al/PVDF. No variation in the dissipation factor is observed up to 60 wt.% Al. Thermal conductivity and dielectric permittivity values as high as 1.65 W/m K and 230, respectively, as well as a low dissipation factor of 0.25 at 0.1 Hz, are realized for the composites with 80 wt.% spherical Al.     

Influence of glass microspheres on selected properties of polylactide composites

Comparison of some changes occurring in polylactide (PLA) due to its modification by glass filler being in the form of microspheres (GM) was the objective of the present study. Mechanical and thermal properties, density, mass flow rate, and were determined. In addition, there were examined surface free energy and changes in the surface geometrical structure of sample fractures. It was found that PLA as modified with GM exhibited the enhanced longitudinal modulus of elasticity, flexural modulus, and mass flow rate. The impact strength and flexural strength did not change. The tensile strength and tensile strain at break decreased. The used glass filler did not affect essentially the thermal properties of PLA. The prepared composites exhibited uniform distribution of the dispersed phase in the polymer matrix and adequate adhesion at the interface between the two components. Substantial changes in the properties of the surface layer were observed, mainly in surface free energy.     

Dielectric properties and thermal conductivity of PVDF reinforced with three types of Zn particles

In this study, three types of Zinc (Zn) particles, i.e., the spherical Zn (s-Zn), flaky Zn (f-Zn), and metal–semiconductor Zn@ZnO core–shell structure, are incorporated in poly(vinylidene fluoride) (PVDF) to obtain high dielectric permittivity polymer. The morphological, dielectric properties and thermal conductivity of the composites are characterized. The results indicate that compared with the s-Zn/PVDF the Zn@ZnO/PVDF at lower filler loading exhibited obviously higher dielectric permittivity due to the duplex interfacial polarizations, and that the f-Zn/PVDF showed larger dielectric permittivity and thermal conductivity owing to f-Zn’s high aspect ratio facilitating the formation of bridges between themselves. Furthermore, the dissipation factors of the s-Zn/PVDF and Zn@ZnO/PVDF were still at low level owing to the presence of self-passivation layer or ZnO shell between Zn core and PVDF, leading to a high critical filler concentration, whereas, a noticeable variation in the dissipation factor for the f-Zn/PVDF is observed up to 12 vol.% f-Zn.     

Study on thermal properties of graphene foam/graphene sheets filled polymer composites

The polymer composites composed of graphene foam (GF), graphene sheets (GSs) and pliable polydimethylsiloxane (PDMS) were fabricated and their thermal properties were investigated. Due to the unique interconnected structure of GF, the thermal conductivity of GF/PDMS composite reaches 0.56 W m⁻¹ K⁻¹, which is about 300% that of pure PDMS, and 20% higher than that of GS/PDMS composite with the same graphene loading of 0.7 wt%. Its coefficient of thermal expansion is (80–137) × 10⁻⁶/K within 25–150 °C, much lower than those of GS/PDMS composite and pure PDMS. In addition, it also shows superior thermal and dimensional stability. All above results demonstrate that the GF/PDMS composite is a good candidate for thermal interface materials, which could be applied in the thermal management of electronic devices, etc.     

Effect of surface treatment on thermal stability of the hemp-PLA composites: Correlation of activation energy with thermal degradation

The thermal behavior of hemp-poly lactic acid composites with both untreated and chemically surface modified hemp fiber was characterized by means of activation energy of thermal degradation. Three chemical surface modification employed were; alkali, silane and acetic anhydride. Model-free isoconversion Flynn–Wall–Ozawa method was chosen to evaluate the activation energy of composites. The results indicated that composites prepared with acetic anhydride modified hemp had 10–13% higher activation energy compared to other composites. Further, among the three surface modifications, acetic anhydride resulted in higher activation energy (159–163 kJ/mol). Fourier transform infrared spectroscopy supported the findings of thermogravimetric analysis results, wherein surface functionalization changes were observed as a result of surface modification of hemp fiber. It was concluded that, higher bond energy results in higher activation energy, which improves thermal stability. The activation energy data can aid in better understanding of the thermal degradation behavior of composites as a function of composite processing.     

Synergistic effect of boron nitride flakes and tetrapod-shaped ZnO whiskers on the thermal conductivity of electrically insulating phenol formaldehyde composites

Tetrapod-shaped zinc oxide (T-ZnO) whiskers and boron nitride (BN) flakes were employed to improve the thermal conductivity of phenolic formaldehyde resin (PF). A striking synergistic effect on thermal conductivity of PF was achieved. The in-plane thermal conductivity of the PF composite is as high as 1.96 W m⁻¹ K⁻¹ with 30 wt.% BN and 30 wt.% T-ZnO, which is 6.8 times higher than that of neat PF, while its electrical insulation is maintained. With 30 wt.% BN and 30 wt.% T-ZnO, the flexural strength of the composite is 312.9% higher than that of neat PF, and 56.2% higher that of the PF composite with 60 wt.% BN. The elongation at break is also improved by 51.8% in comparison with that of the composite with 60 wt.% BN. Such a synergistic effect results from the bridging of T-ZnO whiskers between BN flakes facilitating the formation of effective thermal conductance network within PF matrix.     

The effect of interfacial state on the thermal conductivity of functionalized Al2O3 filled glass fibers reinforced polymer composites

Rapidly increasing packaging density of electronic devices puts forward higher requirements for thermal conductivity of glass fibers reinforced polymer (GFRP) composites, which are commonly used as substrates in printed circuit board. Interface between fillers and polymer matrix has long been playing an important role in affecting thermal conductivity. In this paper, the effect of interfacial state on the thermal conductivity of functionalized Al₂O₃ filled GFRP composites was evaluated. The results indicated that amino groups-Al₂O₃ was demonstrated to be effective filler to fabricate thermally conductive GFPR composite (1.07 W/m K), compared with epoxy group and graphene oxide functionalized Al₂O₃. It was determined that the strong adhesion at the interface and homogeneous dispersion of filler particles were the key factors. Moreover, the effect of interfacial state on dielectric and thermomechanical properties of GFRP composites was also discussed. This research provides an efficient way to develop high-performance GFRP composites with high thermal conductivity for integrated circuit packaging applications.     

Thermal conductivity of epoxy composites with a binary-particle system of aluminum oxide and aluminum nitride fillers

Aluminum oxide and aluminum nitride with different sizes were used alone or in combination to prepare thermally conductive polymer composites. The composites were categorized into two systems, one including composites filled with large-sized aluminum nitride and small-sized aluminum oxide particles, and the other including composites filled with large-sized aluminum oxide and small-sized aluminum nitride. The use of these hybrid fillers was found to be effective for increasing the thermal conductivity of the composite, which was probably due to the enhanced connectivity offered by the structuring filler. At a total filler content of 58.4 vol.%, the maximum values of both thermal conductivities in the two systems were 3.402 W/mK and 2.842 W/mK, respectively, when the volume ratio of large particles to small particles was 7:3. This result was represented when the composite was filled with the maximum packing density and the minimum surface area at the same volume content. As such, the proposed thermal model predicted thermal conductivity in good agreement with experimental values.     

Preparation and properties of hollow glass microsphere-filled epoxy-matrix composites

Hollow glass microsphere (HGM)–filled epoxy composites, with filler content ranging from 0 to 51.3 vol.%, were prepared in order to modify the dielectric properties of the epoxy. The results showed that the dielectric constant (D_k) and dielectric loss (D_f) of the composites decreased simultaneously with increasing HGM content, which was critical for the provision of superior high-frequency device performance. Other properties of the composite, such as the coefficient of thermal expansion (CTE) and the glass transition temperature (T_g), were also improved. The improvement in these properties was related to strong interaction between the HGM and epoxy, which was indicated by the formation of an interphase between the HGM and epoxy-matrix. It was unsatisfactory in this study that the thermal conductivity of the composites also decreased with HGM content. In order to obtain relatively high thermal conductivity and a low dielectric constant simultaneously, this paper suggests further adding other filler.     

Estimation of thermal conductivity for polypropylene/hollow glass bead composites

The thermal conductivity of hollow glass bead (HGB)-filled polypropylene (PP) composites was estimated using the thermal conductivity equation of inorganic hollow microsphere-filled polymer composites published in the previous paper. The estimations were compared with the measured data of the PP composites filled with two kinds of HGB with different size (the mean diameter was respectively 35 μm and 70 μm). The results showed that the predictions of the thermal conductivity were in good agreement with the measured data except to individual data points. Furthermore, both the estimated and measured thermal conductivity decreased roughly linearly with increasing the HGB volume fraction when the HGB volume fraction was less than 20%; the influence of the particle diameter on the thermal conductivity was insignificant.     

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.     

Electrical properties of polyvinylidene fluoride (PVDF)/multi-walled carbon nanotube (MWCNT) semi-transparent composites: Modelling of DC conductivity

Transparent conductive composites can be achieved from PVDF–MWCNT at very low concentration of MWCNT. These composites show different degree of UV–Visible radiation absorption depending on MWCNT concentration in composites. The composition dependent dielectric properties and AC conductivity were also measured for these composites. Properties like AC conductivity, dielectric constant and loss are increasing with filler concentration. The variations of DC conductivity against composition and temperature are also reported. The electrical hysteresis and electrical set are observed for PVDF–MWCNT composites when subjected to heating–cooling cycle. The validity of different theoretical models depicting percolation threshold with respect to DC conductivity was tested for these composites.     

Effects of aluminium nitride inclusions on thermal and electrical properties of epoxy and polypropylene: An experimental investigation

Thermal and dielectric properties of polymers reinforced with micro-sized aluminium nitride (AlN) particles have been studied. A set of epoxy–AlN composites, with filler content ranging from 0 to 25 vol% is prepared by hand lay-up technique. With similar filler loading, polypropylene -AlN composites are fabricated by compression molding technique. Density (ρ_c), effective thermal conductivity (k_eff), glass transition temperature (T_g), coefficient of thermal expansion (CTE) and dielectric constant (ε_c) of these composites are measured experimentally. The various experimental data were interpreted using appropriate theoretical models. Incorporation of AlN in both the resin increases the k_eff and T_g whereas CTE of composite decreases favourably. The dielectric constant of the composite also found to get modified with filler content. With improved thermal and modified dielectric characteristics, these AlN filled polymer composites can possibly be used for microelectronics applications.     

Engineering the coefficient of thermal expansion and thermal conductivity of polymers filled with high aspect ratio silica nanofibers

The thermomechanical properties of epoxy filled with two different types of silica nanofillers: spherical nanoparticles and nanofibers were investigated as a function of silica nanofiller aspect ratio and concentration. Results indicated that at room temperature and at 8.74% silica nanofiber concentration (by volume) the thermal conductivity of epoxy increased twofold and coefficient of thermal expansion (CET) decreased by ∼40%. Silica nanofiber filled epoxy showed 1.4 times greater CET and 1.5 times greater thermal conductivity compared to spherical nanoparticle filled epoxy. The significant changes observed in thermomechanical properties of silica nanofiber filled epoxy were attributed to its high aspect ratio by constraining the polymer matrix as well as reducing the phonon scattering due to the formation of a continuous fiber network within the matrix. In addition to being electrically insulating, the improved properties of silica nanofiber filled epoxy make it an extremely attractive material as underfill and encapsulant in advanced electronic packaging industry.     

Development and characterization of the composites based on mesoporous MCM-41 and polyethylene glycol and their properties

Novel MCM-41/polyethylene glycol composites have been synthesized using different ratios of MCM-41. The structure of the different composites was confirmed by using various characterization tools, including: thermal analyses (TGA and DTA), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), and field emission scanning electron microscopy (FE-SEM). The XRD and FT-IR results indicated that PEG interacts with MCM-41 via the formation of hydrogen bonds where no new phase was detected. The TGA analysis results demonstrated that the presence of MCM-41 practically affects the temperature of the main step of degradation. The DTA analysis demonstrated that an increase in the MCM-41 content up to 30 wt.% is accompanied by a continuous decrease in the melting point of PEG.     

Effect of silica coating thickness on the thermal conductivity of polyurethane/SiO2 coated multiwalled carbon nanotube composites

Silica coated multiwalled carbon nanotubes (SiO₂@MWCNTs) with different coating thicknesses of ∼4 nm, 30–50 nm, and 70–90 nm were synthesized by a sol–gel method and compounded with polyurethane (PU). The effects of SiO₂@MWCNTs on the electrical properties and thermal conductivity of the resulting PU/SiO₂@MWCNT composites were investigated. The SiO₂ coating maintained the high electrical resistivity of pure PU. Meanwhile, incorporating 0.5, 0.75 and 1.0 wt% SiO₂@MWCNT (70–90 nm) into PU, produced thermal conductivity values of 0.287, 0.289 and 0.310 W/mK, respectively, representing increases of 62.1%, 63.3% and 75.1%. The thermal conductivity of PU/SiO₂@MWCNT composites was also increased by increasing the thickness of the SiO₂ coating.     

Enhanced thermal resistance of phenolic resin composites at low loading of graphene oxide

By incorporating graphene oxide (GO) into phenolic resin (PR), GO/PR composites were prepared, and the effects of the content and reduction degree of GO on thermal resistance of GO/PR composites were studied. The peak degradation temperature of the PR was increased by about 14 °C with GO which was heat treated. The char yield of GO/PR composite at a GO weight fraction of 0.5% was about 11% greater than that of PR. The interactions such as covalent bonds and π–π stacking between GO and PR were regarded as the main reason for the enhancement. Located at the GO–PR interface, GO effectively anchored and structured PR molecular near the surfaces of GO sheets, and thus facilitated the formation of char. The superiority of GO/PR composites over PR in terms of thermal properties enhancement should also be related to the promoting graphitization by the addition of GO.     

Facile preparation of graphene nanoribbon filled silicone rubber nanocomposite with improved thermal and mechanical properties

In the present study, graphene nanoribbon was prepared through unzipping the multi walled carbon nanotubes, and its reinforcing effect as a filler to the silicone rubber was further investigated. The results showed that carbon nanotubes could be unzipped to graphene nanoribbon using strong oxidants like potassium permanganate and sulfuric acid. The prepared graphene nanoribbon could homogeneously disperse within silicone rubber matrix using a simple solution mixing approach. It was also found from the thermogravimetric analysis curves that the thermal stability of the graphene nanoribbon filled silicone rubber nanocomposites improved compared to the pristine silicone rubber. Besides, with the incorporation of the nanofiller, the mechanical properties of the resulting nanocomposites were significantly enhanced, in which both the tensile stress and Young’s modulus increased by 67% and 93% respectively when the mass content of the graphene nanoribbon was 2.0 wt%. Thus it could be expected that graphene nanoribbon had large potentials to be applied as the reinforcing filler to fabricate polymers with increased the thermal and mechanical properties.     

Investigation of the electrical conductivity of HDPE composites filled with bundle-like MWNTs

Bundle-like multi-walled carbon nanotubes (MWNTs) were melting-mixed with high-density polyethylene (HDPE). MWNTs are distributed in the matrix mostly isolated. Agglomerates are observed at higher concentrations. The electric conductivity of the composites follows the theory of a percolation system, and the charge transport shows different models. The temperature dependence of the electrical conductivity for the composites shows that both positive (PTC) and negative (NTC) temperature coefficients appear near the melting temperature of matrix. The NTC behaviors within the temperature range below the melting point depend on the MWNTs concentration and the NTC intensity increases with the increasing MWNTs concentration.