Effects of two-step sintering on thermal and mechanical properties of aluminum nitride ceramics by impedance spectroscopy analysis

The effects of two-step sintering on the microstructure, mechanical and thermal properties of aluminum nitride ceramics with Yb₂O₃ and YbF₃ additives were investigated. AlN samples prepared using different sintering methods achieved almost full density with the addition of Yb₂O₃–YbF₃. Compared with the one-step sintering, the grain sizes of AlN ceramics prepared by the two-step sintering were limited, and the higher flexural strength and the larger thermal conductivity were obtained. Moreover, the electrochemical impedance spectroscopy of AlN ceramic was associated with thermal conductivity by analyzing the defects and impurities in AlN ceramics. The fitting grain resistance and the activation energy for the grain revealed the lower concentrations of aluminum vacancy in the two-step sintered AlN ceramics, which resulted in the higher thermal conductivity. Thus, mechanical and thermal properties for AlN ceramics were improved with Yb₂O₃ and YbF₃ additives sintered using two-step regimes.     

Directional properties and microstructures of spark plasma sintered aluminum nitride containing graphene platelets

Graphene platelets (GPLs) containing aluminum nitride (AlN) composites were produced by using both pressureless sintering and spark plasma sintering (SPS). Poor densifications were obtained when composites were pressureless sintered whereas highly dense composites were successfully produced by using SPS. In addition, the applied uniaxial load in the SPS resulted in the orientation of GPLs in the microstructure of composites, indicating that composites would have anisotropic properties. All the mechanical, thermal and electrical properties in the in-plane direction were better than the through-plane direction. Fracture toughness of composites with the addition of 1 wt% GPLs were increased more than 30% compared to AlN matrix. Increased anisotropic effect with increasing amount of GPLs led to even larger differences on the thermal conductivities in through-plane and in-plane directions. AlN also became an electrically conducting material after ∼1 wt% GPLs addition in both through-plane and in-plane directions.     

Tuning electrical conductivity in AlN-based ceramics by incorporating graphene

Aluminum nitride (AlN) is the material of choice for high power modulus substrates. The thermal and electrical conductions can be also fostered by adding CaF₂ and carbon particles, respectively. Moreover, additives (Y₂O₃) have to be used as sintering aids to achieve full densification. In this paper, we report on tuning the electrical conduction within AlN-based composites developed by incorporating graphene nanoplatelets GNP, obtained from graphite exfoliation, in the AlN-based ceramics comprising Y₂O₃ and CaF₂. These composites were prepared by Spark Plasma Sintering through a new configuration called “multiple preparation” with a view to fabricating three samples per cycle, revealing time and energy savings. An increase of the electrical conductivity by 10 orders of magnitude was obtained for these composites compared to the commercial AlN by adjusting the amount of GNP and the way of exfoliation. This work promotes the development of novel multifunctional ceramic composites for Power Electronics applications.     

Mechanical,electrical, and thermal properties of graphene nanosheet/aluminum nitride composites

Graphene nanosheet (GNS)/aluminum nitride (AlN) composites were prepared by hot-pressing and effects of GNSs on their microstructural, mechanical, thermal, and electrical properties were investigated. At 1.49 vol% GNSs content, the fracture toughness (5.09 MPa m^1/2) and flexural strength (441 MPa) of the composite were significantly increased by 30.17% and 17.28%, respectively, compared to monolithic AlN. The electrical conductivity of the composites was effectively enhanced with the addition of GNSs, and showed a typical percolation behavior with a low percolation threshold of 2.50±0.4 vol%. The thermal conductivity of the composites decreased with the addition of GNSs.     

Effect of hot-pressing sintering on thermal and electrical properties of AlN ceramics with impedance spectroscopy and dielectric relaxations analysis

The effects of hot-pressing sintering on the phase composition, microstructure, thermal and electrical properties of AlN ceramics with CeO₂–CeF₃ additives were studied. During hot-pressing sintering, high pressure reduced the grain boundary phase CeAlO₃ and decreased the concentration of oxygen in AlN ceramics. The hot-pressing sintered AlN samples had a much higher thermal conductivity of 191.9 W/m·K than pressureless sintered ones because of the great reduction of grain boundary phases and oxygen impurities in AlN ceramic. As the carbon content in hot-pressing sintered sample was very high, carbon contamination led to the decrease in electrical resistivity and changes in polarization mechanisms for AlN ceramics. The relaxation peak in the dielectric temperature spectrum with an activation energy of 0.64 eV for hot-pressing sintered samples was caused by electrons from free carbon at low temperature. Overall, hot-pressing sintering can effectively increase the thermal conductivity and change the electrical properties of AlN ceramics.     

The quantitative investigation of the lattice oxygen and grain edge oxygen on the thermal conductivity of aluminum nitride ceramics

The good thermal conductivity of AlN is essential for insulation and high heat dissipation applications. However, the influence of oxygen impurities at various locations (the lattice oxygen and grain edge oxygen) on the thermal resistivity of AlN ceramics is unclear. In this study, AlN ceramics with various oxygen distributions are prepared by different methods, and the oxygen contents of different regions are distinguished. The results indicate that the lattice oxygen is the main factor affecting thermal resistivity. Meanwhile, high-temperature annealing and pre-sintering processes can lower the lattice oxygen content from 0.061 wt% to 0.038 wt% and 0.036 wt%, respectively. Additionally, when grain edge phase volume is less than 4 vol%, it does not contribute significantly to thermal resistivity. The main formation of thermal resistance changes from phonon-defect scattering to phonon-phonon scattering with increasing temperature. These results may be informative for the microstructure design of AlN ceramics with high thermal conductivity.     

The effect of boron nitride nanosheets on the mechanical and thermal properties of aluminum nitride ceramics

The boron nitride nanosheets (BNNSs)/aluminum nitride (AlN) composites were prepared by hot press sintering at 1600°C. The microstructure, mechanical properties, and thermal conductivity of the samples were measured, and the effect of adding BNNSs to AlN ceramics on the properties was studied. It is found that the addition of BNNSs can effectively improve the mechanical properties of AlN. When the additional amount is 1 wt%, the bending strength of the sample reaches the maximum value of 456.6 MPa, which is 23.1% higher than that of the AlN sample without BNNSs. The fracture toughness of the sample is 4.47 MPa m^1/2, a 68.7% improvement over the sample without BNNSs. The composites obtained in the experiment have brilliant mechanical properties.     

Improved crack resistance and thermal conductivity of cubic zirconia containing graphene nanoplatelets

Composites of 8 mol.% yttria-stabilized zirconia (8YSZ) with graphene nanoplatelets (GNP) have been pointed as alternative interconnectors in SOFC due to their mixed ionic-electronic conduction. Here we show that GNP addition provides rising crack-resistance behavior, with long crack toughness up to 78% higher than that of 8YSZ, also improving its thermal conductivity (up to 6 times for the in-plane direction). Toughness versus crack length is measured for 7 and 11 vol.% of GNP using single edge V-notched beam technique and ultrashort pulsed laser notching; and thermal behavior is analyzed by the laser flash method. Materials also have highly anisotropic coefficient of thermal expansion. These properties contribute to enhance their performance under the harsh operating conditions of SOFC, as thermal residual stresses could be reduced while significantly improving the system mechanical stability. Moreover, the heat transfer may be enhanced especially along the interface direction which would increase the system efficiency.     

Enhancement of electrical and thermal conductivity of Su-8 photocrosslinked coatings containing graphene

Graphene platelets were dispersed into photocurable SU-8 resin. A strong increase of the T_g value as a function of the graphene content was observed and attributed to a mobility hindering effect on the polymeric chains caused by the graphene filler. A significant increase of electrical conductivity is achieved for composites containing functionalized graphene sheets (FGS) between 3 and 4 wt%. The thermal diffusivity of the polymer was observed to increase as a function of filler content in the nanocomposites confirming the conducting nature of the polymeric coating with incorporation of graphene.     

Structural,thermal and mechanical properties of aluminum nitride ceramics with CeO2 as a sintering aid

AlN ceramics have been prepared with CeO₂ as a sintering aid at a sintering temperature of 1900 °C. The effect of CeO₂ contents on the microstructure, density, thermal conductivity and hardness was investigated. Addition of CeO₂ exerted a significant effect on the densification of AlN ceramics and hence on the microstructure. Thermal conductivity of AlN ceramics increased with CeO₂ content and was greater than that of Y₂O₃-doped AlN ceramics at a similar sintering temperature. The resulting AlN ceramics with 1.50 wt% of CeO₂ had the highest relative density of 99.94%, thermal conductivity of 156 W m⁻¹ K⁻¹ and hardness of 72.46 kg/mm².     

Investigation of thermal conductivity and rheological properties of nanofluids containing graphene nanoplatelets

In the present study, stable homogeneous graphene nanoplatelet (GNP) nanofluids were prepared without any surfactant by high-power ultrasonic (probe) dispersion of GNPs in distilled water. The concentrations of nanofluids were maintained at 0.025, 0.05, 0.075, and 0.1 wt.% for three different specific surface areas of 300, 500, and 750 m²/g. Transmission electron microscopy image shows that the suspensions are homogeneous and most of the materials have been well dispersed. The stability of nanofluid was investigated using a UV-visible spectrophotometer in a time span of 600 h, and zeta potential after dispersion had been investigated to elucidate its role on dispersion characteristics. The rheological properties of GNP nanofluids approach Newtonian and non-Newtonian behaviors where viscosity decreases linearly with the rise of temperature. The thermal conductivity results show that the dispersed nanoparticles can always enhance the thermal conductivity of the base fluid, and the highest enhancement was obtained to be 27.64% in the concentration of 0.1 wt.% of GNPs with a specific surface area of 750 m²/g. Electrical conductivity of the GNP nanofluids shows a significant enhancement by dispersion of GNPs in distilled water. This novel type of nanofluids shows outstanding potential for replacements as advanced heat transfer fluids in medium temperature applications including solar collectors and heat exchanger systems.     

Novel in-situ constructing approach for vertically aligned AlN skeleton and its thermal conductivity enhancement effect on epoxy

As one of the key components of electronic devices, thermal management materials (TMMs) with high thermal conductivity are essential to ensure their safety and long service life. For polymer-based TMMs, AlN is one of the preferred fillers, but it has some drawbacks such as high cost and easy hydrolysis. Herein, a controllable and continuously oriented three-dimensional AlN skeleton (3D-AlNNS) was in-situ transformed from a low-cost 3D Al-containing skeleton (3D-AlNS) by combining the ice-templating and nitriding reaction sintering. Subsequently, AlN/epoxy composites were obtained by a vacuum infiltration. The composite containing 39.69 vol% AlN had the highest thermal conductivity of 4.29 W m^?1·K^?1, which was 21.45 times higher than that of pure epoxy. The composite substrates showed excellent heat dissipation performance in practical applications due to their high thermal conductivity. The continuous directional alignment of AlN powders in the 3D skeleton and intersection of AlN whiskers between the skeleton walls produced in-situ contributed to the formation of effective multichannel heat transferring paths and improvement in thermal conductivity. This novel approach has the advantages of low-cost, short processing time, simple operation and repeatability, and provides a new idea for developing heat-conducting polymer composites, which can also be extended to the preparation of similar TMMs.     

Tailoring the properties of spark plasma sintered SiAlON containing graphene nanoplatelets by using different exfoliation and size reduction techniques: Anisotropic electrical properties

Insulating SiAlON ceramics can be machined into complex shapes if the electrical conductivities can be increased with additives. Therefore, the microfluidization technique was used as an alternative to traditional sonication for exfoliation and homogenization of GNPs to investigate the effects of different exfoliation, size reduction and homogenization techniques on the microstructure, electrical conductivity and percolation threshold values of GNPs-SiAlON composites. 2.85, 5.70 and 11.40?vol. % sonicated and sonicated?+?microfluidized GNPs added into SiAlON matrix and were densified by using SPS technique. Due to their thinner and smaller platelet size, microfluidized GNPs dispersed more homogeneously compared to the sonicated GNPs in the SiAlON matrix. Electrical conductivities of the microfluidized GNPs-SiAlON composites were ～70–200% higher than sonicated GNPs-SiAlON in the both measured directions. Lower percolation thresholds were achieved when sonicated?+?microfluidized GNPs used in comparison to sonicated GNPs containing composites. Electrical conductivities in the in-plane direction were also higher than through-plane direction.     

Effects of SmF3 addition on aluminum nitride ceramics via pressureless sintering

Aluminum nitride (AlN) ceramics with dense structure, high thermal conductivity, and exceptional mechanical properties were fabricated by pressureless sintering with a novel non-oxide sintering additive, samarium fluoride (SmF₃). The results showed that the use of a moderate amount of SmF₃ promoted significant densification of AlN and removed the oxygen impurity. This led to the formation of fine and isolated secondary phase that cleaned the grain boundaries and increased the contact between AlN grains, remarkably enhancing thermal conductivity. Furthermore, SmF₃ also exhibited grain refinement and grain boundary strengthening effects similar to traditional sintering additive, samarium oxide (Sm₂O₃), leading to high mechanical properties in SmF₃-doped AlN samples. The most optimal characteristics (thermal conductivity of 190.67 W·m⁻¹·K⁻¹, flexural strength of 403.86 ± 18.27 MPa, and fracture toughness of 3.71 ± 0.19 MPa·m^1/2) were achieved in the AlN ceramic with 5 wt% SmF₃.     

Fabrication and characterization of aluminum nitride thick film coated on aluminum substrate for heat dissipation

For effective heat dissipation in high-power LED applications, aluminum nitride (AlN) thick films as thermally conductive dielectric layers were developed, which were deposited on an Al substrate by aerosol deposition (AD). The aerosol-deposited AlN thick films on Al substrates have advantages over conventional polymer-based dielectric substrates or ceramic substrate mounted heatsink systems including an epoxy adhesive, such as excellent heat dissipation capacity and low thermal resistance. AD is an effective method to fabricate high-quality AlN thick film without the Al₂O₃ phase because the film is formed at room temperature. Highly dense and well-adhered, pure AlN thick films with thicknesses up to 30 µm were deposited on an Al substrate. AlN-Al₂O₃ and AlN-polyvinylidene fluoride (PVDF) composite films were also deposited on an Al substrate in order to investigate the effect of Al₂O₃ and polymer on the microstructure and thermal properties. Among the films, pure AlN thick film exhibited the highest dielectric strength, the highest thermal conductivity, and the lowest thermal resistance. Therefore, it can be expected that the aerosol-deposited AlN thick film on Al substrate could be used as a powerful heatsink.     

Effect of MgF2 addition on mechanical properties and thermal conductivity of silicon nitride ceramics

Dense silicon nitride (Si₃N₄) ceramics were prepared using Y₂O₃ and MgF₂ as sintering aids by spark plasma sintering (SPS) at 1650 °C for 5 min and post-sintering annealing at 1900 °C for 4 h. Effects of MgF₂ contents on densification, phase transformation, microstructure, mechanical properties, and thermal conductivity of the Si₃N₄ ceramics before and after heat treatment were investigated. Results indicated that the initial temperature of liquid phase was effectively decreased, whereas phase transformation was improved as increasing the content of MgF₂. For optimized mechanical properties and thermal conductivity of Si₃N₄, optimum value for MgF₂ content existed. Sample with 3 mol.% Y₂O₃ and 2 mol.% MgF₂ obtained optimum flexural strength, fracture toughness and thermal conductivity (857 MPa, 7.4 MPa m^1/2 and 76 W m⁻¹ K⁻¹, respectively). It was observed that excessive MgF₂ reduced the performance of the ceramic, which was caused by the presence of excessive volatiles.     

Improvement in fracture strength in electrically conductive AlN ceramics with high thermal conductivity

It is possible to impart electrical conductivity to insulating aluminum nitride (AlN) ceramics by precipitating a yttrium oxycarbide grain boundary phase with electrical conductivity. However, previously, sintering at high temperature was required to increase the electrical conductivity through the transformation of the grain boundary phase from yttrium aluminum oxide (Al₂Y₄O₉) to rare-earth oxycarbide. As a result, the increase in electrical conductivity was accompanied with a considerable decrease in the fracture strength due to grain growth of AlN. In this study, sintering temperature and additive compositions were investigated to maintain the high strength of electrically conductive AlN without losing the high thermal conductivity.     

Synergistic enhancement of thermal conductivity by addition of graphene nanoplatelets to three-dimensional boron nitride scaffolds for polyamide 6 composites

Three-dimensional boron nitride/graphene nanoplatelets (3D-BN-GNP) scaffolds were fabricated using an ice-templating method and polyamide 6 (PA6)-based composites were prepared by vacuum impregnation of caprolactam monomers into the scaffolds, followed by polymerization. The BN sheets in the PA6/3D-BN and PA6/3D-BN-GNP composites display a predominant parallel alignment along the ice-crystal formation constructing thermally conductive paths. The addition of few GNPs assists the dispersion of BN sheets in the PA6/3D-BN-GNP composites and repair the broken thermal paths caused by local agglomeration of the BN sheets. Consequently, GNPs play a morphology-promoted synergistic role in the enhancement of the thermal conductivity of the PA6/3D-BN-GNP composites. The PA6/3D-BN-GNP composite prepared with 23.40 wt% BN sheets and 2.60 wt% GNPs exhibits the highest thermal conductivity of 2.80 W m⁻¹ K⁻¹, which is 833% and 33% higher than the values recorded for the pure PA6 and the PA6/3D-BN composite at BN loading of 26.18 wt%, respectively. Infrared imaging analysis revealed that the surface of the PA6/3D-BN-GNP composite has a fast response to heating and cooling, suggesting the potential of the composites in thermal management applications.     

The manufacturing and properties of a nano-laminate derived from graphene powder

The work presents a method of consolidation of graphene flakes (platelets) into a bulk material showing high anisotropy of thermal, electrical and mechanical properties. Such materials can be used as directional high-temperature thermal insulators similar to graphite foils, but due to much finer microstructure they may exhibit different, possibly enhanced properties. The graphene flakes were consolidated by a filter pressing of propanol suspension followed by a hot-pressing of produced green bodies at 2200 °C under 25 MPa in a protective atmosphere.The hot-pressing step was necessary to force orientation of the flakes and to densify the material. Microstructural observations, mechanical strength and elastic properties assessment, as well as thermal and electrical properties analysis were performed. Scanning electron microscopy revealed that microstructure of the material consisted of highly-oriented layers of the graphene flakes. It resulted in a distinct anisotropy of thermal conductivity (360 vs. 3 W/mK), coefficient of thermal expansion (25·10⁻⁶ vs. −1·10⁻⁶ 1/K) and electrical resistivity (60·10⁻⁶ vs. 850·10⁻⁶ Ω m) of the material in the in-plane and through plane direction, respectively. The material showed brittle behavior, but it could be machined.     

Graphene platelets/aluminium nitride metacomposites with double percolation property of thermal and electrical conductivity

Graphene platelets/aluminium nitride (GPLs/AlN) metacomposites with double percolation property of thermal and electrical conductivity were successfully fabricated by spark plasma sintering. Microstructures and phase composition of the GPLs/AlN metacomposites were investigated by field emission scanning electron microscopy, X-ray diffraction and Raman spectroscopy. With increase of the GPLs contents, the double percolation property of thermal (19.27?wt% GPL) and electrical conductivity (19.03?wt% GPL) was found. Moreover, the negative permittivity behavior was also observed when the GPLs content reached 19.50?wt%, which was attributed to the formation of continuous GPLs networks. Finally, the equivalent circuit models were used to analyze the negative permittivity behavior. As the reactance (Z′′) converted from negative to positive, the inductors were introduced into the equivalent circuit models, and the GPLs/AlN metacomposites went through the capacitive-inductive transition with the increasing GPLs content, corresponding to the negative permittivity behavior.