温度对高压烧结氮化铝陶瓷热导率的影响

以直接氮化法合成的AlN微米粉为原料,添加3%(质量分数)的CaC2为烧结助剂,在5GPa的压力下烧结30min,考察不同烧结温度对AlN陶瓷热导率的影响。用阿基米德排水法、XRD、SEM等技术手段对AlN烧结体进行性能检测。研究表明,在1500～1800℃范围内,温度的升高能促使AlN陶瓷内部晶粒长大,晶型饱满,尺寸均一,晶界相减少,实现烧结致密化,利于热导率的提高。     

Microstructure and thermal conductivity of spark plasma sintering AlN ceramics

Abstract

Dense aluminium nitride ceramics were prepared by spark plasma sintering at a lower sintering temperature of 1700°C with Y₂O₃, Sm₂O₃ and Dy₂O₃ as sintering additives respectively. The effects of three kinds of sintering additives on the phase composition, microstructure and thermal conductivity of AlN ceramics were investigated. The results showed that those sintering additives not only facilitated the densification via the liquid phase sintering mechanism, but also improved thermal conductivity by decreasing oxygen impurity. Sm₂O₃ could effectively improve thermal conductivity of AlN ceramics compared with Y₂O₃ and Dy₂O₃. Observation by scanning electron microscopy showed that AlN ceramics prepared by spark plasma sintering method manifested quite homogeneous microstructures, but AlN grain sizes and shapes and location of secondary phases varied with the sintering additives. The thermal conductivity of AlN ceramics was mainly affected by the additives through their effects on the growth of AlN grain and the location of secondary phases.     

Study on microstructure and thermal conductivity of Spark Plasma Sintering AlN ceramics

Dense aluminum nitride (AlN) ceramics were prepared by Spark Plasma Sintering with rare-earth oxide and CaF₂ as sintering additives. The effect of sintering additives on the density, phase composition, microstructure and thermal conductivity of AlN ceramics was investigated. The results showed that those sintering additives not only promoted densification through liquid-phase sintering but also improved thermal conductivity by decreasing oxygen impurities. Thermal conductivities of samples sintered with optimum proportion of rare-earth oxide and CaF₂ were higher than those of other samples. During the Spark Plasma Sintering process, the microstructures, especially the content and distribution of secondary phases, played important roles on the thermal conductivity of AlN ceramics.     

Synthesis of neodymium-doped yttrium aluminum garnet (YAG) nanocrystalline powders leading to transparent ceramics

We report on the synthesis of Nd:YAG nanoparticles by the coprecipitation technique and the optimum conditions for the processing of transparent ceramics. The powders prepared by the coprecipitation technique display significantly less agglomeration of crystallites, indicating higher sinterability. The crystallite size dependence on the calcinations temperature suggests the optimum temperature of 1100 °C, at which phase purity of the YAG nanopowder with the highest sinterability can be obtained. We have demonstrated that the optimum temperature for the vacuum-sintering is about 1785 °C for the uniaxially pressed samples to obtain transparent ceramic with uniform particle size of about 5-7 μm, and above this temperature, enormously large grain growth occurs, and facilitates large pores formation in the intergrain region that makes the ceramic fragile at the grain boundary.     

Effect of grain boundary phase on the thermal conductivity of aluminium nitride ceramics

AIN with high thermal conductivity was fabricated by pressureless sintering with Y₂O₃ as the sintering aid. The thermal conductivity was observed to increase with sintering time (up to 8 h) at 1810 °C. The distribution of the sintering aid was identified as one of the major factors influencing the thermal conductivity in AIN. Non-uniform distribution of the grain boundary phase was found to be associated with a significant amount of porosity, resulting in the enhancement of phonon scattering and thereby lowering the thermal conductivity.     

SPS制备AlN/BN复相陶瓷及其性能优化

采用放电等离子烧结技术(SPS),在1750～1850℃烧结制备出兼顾高热导率和优良可加工性能的AlN/BN复相陶瓷.结果表明,通过调节添加剂Y2O3的加入量,能够显著抑制BN对材料热传导性能的劣化作用,BN含量为25%(体积分数)时,热导率仍能达到120W/(m·K),与AlN单相陶瓷相比仅下降18.9%.在SPS制备条件下,添加不同量的Y2O3导致不同组成的Al-Y-O晶界相,随着Y2O3的增加,晶界相在烧结过程中大量挥发,致使Al-Y-O残留量减少,优化了材料的显微组织,有效地提高热传导性能.     

Enhanced thermal conductivity of poly(L-lactide) composites with synergistic effect of aluminum nitride and modified multi-walled carbon nanotubes

Poly (ethylene glycol)-grafted multi-walled carbon nanotubes (PEG-MWNTs) were prepared and added into poly(L-lactide) (PLLA)/aluminum nitride (AlN) composites to obtain PLLA/AlN/PEG-MWNTs nanocomposites. Microstructure and thermal conductivity of the composites were investigated on the basis of the influence of PEG-MWNTs incorporated. The results showed that PEG-MWNTs were well-dispersed in the PLLA matrix and had strong interfacial adhesion with the matrix. The addition of PEG-MWNTs improved the thermal conductivity of PLLA/AlN composites. When 3 wt.% of PEG-MWNTs and 50 wt.% of AlN were both added into the PLLA matrix, the thermal conductivity reached 0.7734 W/mK with enhancement almost by 400% as compared to a neat PLLA. However, the thermal conductivity is 0.3401 W/mK for the PLLA composite with 3 wt.% of PEG-MWNTs and 0.4286 W/mK for the one with 50 wt.% of AlN. The synergistic effect of aggregated AlN particles and well-dispersed MWNTs could form efficient thermal conductive paths for improving the thermal conductivity of PLLA composites greatly.     

Sintering chemical reactions to increase thermal conductivity of aluminium nitride

Chemical reactions to increase thermal conductivity by decreasing oxygen contents during AlN sintering with an Y₂O₃ additive in a reducing nitrogen atmosphere with carbon were investigated. They were: Al₂O₃ + N₂ + 3CO ⇋ 2AlN + 3CO₂, Al₂Y₄O₉ + N₂ + 3CO ⇋ 2AlN + 2Y₂O₃ + 3CO₂ and Y₂O₃ + N₂ + 3CO ⇋ 2YN + 3CO₂. Some of the CO₂ gas reduced to CO gas in the presence of carbon by a chemical reaction: CO₂ + C ⇋ 2CO. These reactions were confirmed by examining oxygen contents, the grain boundary phases of the sintered AlN, and the trapped CO and CO₂ gases in the sintered bodies. These reducing reactions proceed with increasing sintering temperature and periods, and hence the thermal conductivity is increased.     

钛酸钡-氮化硼/聚间苯二甲酰间苯二胺复合电介质的制备与导热性能

选用聚多巴胺(PDA)和十八烷基异氰酸酯分别改性钛酸钡纳米线(BTW)和氮化硼纳米片(BNNSs)来构筑D@BTW-fBNNSs高介电导热填料.研究了D@BTW-fBNNSs高介电导热填料对芳香族聚酰胺(PMIA)基复合电介质介电性能、击穿强度和导热性能的影响.结果表明:随着复合电介质中D@BTW-fBNNSs含量的增...     

The influence of microstructure on the thermal conductivity of aluminium nitride

Starting from three different commercial powders, AIN materials were densified by pressureless sintering under various temperature and time values in order to investigate the influence of microstructure on thermal conductivity. The influence of the sintering aids (3 wt% Y₂O₃ and 2 wt% CaC₂) and of the forming processes (cold isostatic pressing and thermocompression of tape cast pieces) were also been evaluated. Thermal conductivity increased with the purity level of the starting powder and with an increasing the sintering temperature and soaking time. The highest thermal conductivity values (196 Wm^–1 K^–1) were obtained with the purest powder and high temperature (1800 °C) sintering over long periods (6 h). No influence on thermal conductivity was detected from the forming technique.     

Effect of grain-boundary stabilization on the strength, thermal conductivity, and dielectric properties of aluminum nitride

The thermal conductivity, dielectric properties, and strength of A1N ceramics were studied. The ceramics were prepared by semidry pressing and sintering. Increasing the sintering time was found to increase the thermal conductivity of the ceramics up to 200 W/(m K). A nonequilibrium-phonon-propagation method was used to analyze the effect of grain boundaries and processing conditions on the thermal conductivity of the ceramics.     

The response of yttrium aluminum garnet (YAG) grains and grain boundaries to nanoindentation

A systematic investigation on the mechanical response of the interior grain and grain boundary of yttrium aluminum garnet is carried out using nanoindentation and microstructure characterization. The nano-hardness is calculated, while the residual indent is analyzed in terms of surface profiles, plastic deformation and elastic recovery. The results show that the nano-hardness at the center of grain is higher than that in the grain boundary region. All indents display an anisotropic elastic recovery, mainly occurring in the loading direction. The grain boundary has a better plasticity than the center of grain, which is probably due to a weaker inter-atomic bonding force at the grain boundary rather than the formation of glassy phase at intergranular region. In addition, indentation size effect in the center of grain and at grain boundary region are determined by the analysis of nano-hardness using Meyer’s law. A weaker indentation size effect in the grain boundary region is observed due to a smaller elastic recovery.     

真空烧结Nd:YAG透明陶瓷的研究

以高纯Al2O3、Y2O3和Nd2O3粉体为原料,少量MgO和SiO2为添加剂,采用真空烧结方法制备了不同掺杂浓度的NdYAG(Y3Al5O12)透明陶瓷,并且对烧成的NdYAG陶瓷的显微结构和光学性能进行了研究.结果发现,真空烧结有利于气孔的排出,从而达到几乎完全致密化;适量烧结助剂的添加,有利于提高陶瓷的烧结活性和透光性;NdYAG陶瓷能够实现高浓度掺杂,但是透过率随着Nd掺杂量的增加有所降低,光吸收随着掺杂量的增加而增加;掺杂浓度升高,发射谱峰出现展宽,并且出现红移现象,当Nd3+的掺杂浓度大于3.0%(原子分数)时,发射强度急剧降低.     

The thermal conductivity of polycrystalline corundum in the range from 90 to 1100°K

We describe a method for the measurement of the thermal conductivity of a dielectric ceramic at low temperatures. We present the results from the measurements carried out on polycrystalline A1₂O₃ in the range from 90 to 1100°K, and we discuss the nature of the temperature relationship to thermal conductivity.     

Influence of deposition conditions on optical properties of aluminum nitride (AlN) thin films prepared by DC-reactive magnetron sputtering

Aluminum nitride (AlN) films have been prepared by DC-reactive magnetron sputtering technique. The optical properties of the films have been studied by optical spectroscopy with an incoherent light source. For the first time, it is demonstrated that for certain deposition conditions, the film may behave as a metallic thin film. In this case, there are strongly enhanced reflection peaks in the optical spectrum and the peaks may red-shift according to the degree of the metallization. The microscopic structures of the films have also been studied with scanning electron microscopy (SEM) and X-ray diffraction (XRD). It turns out that the orientation of the crystallites in the film determines whether the film remains dielectric or becomes metallic. It is found that the degree of the metallization depends on the proportion of (1000) preferred orientation in the film. In the deposition process, various deposition parameters have been experimented and a close relation between the deposition parameters and the status of the films is established. The most influential deposition conditions are as follows: the substrate temperature in a range from 200 to 700 °C, the gas composition ratio of Ar/N₂ from 20/80 to 60/40 and the plasma current from 0.2 to 0.45 A.     

Fabrication and characterization of aluminum nitride polymer matrix composites with high thermal conductivity and low dielectric constant for electronic packaging

Polymethyl methacrylate (PMMA) composites filled with Aluminum Nitride (AlN) were prepared by powder processing technique. The microstructures of the composites were investigated by scanning electron microscopy techniques. The effect of AlN filler content (0.1–0.7 volume fraction (vf)) on the thermal conductivity, relative permittivity, and dielectric loss were investigated. As the vf of AlN filler increased, the thermal conductivity of the specimens increased. The thermal conductivity and relative permittivity of AlN/PMMA composites with 0.7 vf AlN filler were improved to 1.87 W/(m K) and 4.4 (at 1 MHz), respectively. The experimental thermal conductivity and relative permittivity were compared with that from simulation model.     

Sol-gel processing and sintering of yttrium aluminum garnet (YAG) powders

Gels of yttrium aluminum garnet (YAG) with the stoichiometric composition 3Y₂O₃·5AI₂O₃, were prepared by a sol-gel technique and dried by supercritical extraction with CO₂. Powders were produced by lightly grinding the dried gels. Crystallization of the powder occurred at 900°C and within the limits of detection, the X-ray diffraction pattern of the crystallized material was identical to that of the stoichiometric composition. Powder compacts with a green density of 0.50 of the theoretical were sintered to nearly full density in O₂ during constant heating rate sintering at 5 °C min^–1 to 1600 °C. This is better than the density obtained with powders from a similar gel dried conventionally (by evaporation of the liquid) and considerably better than that obtained with powders prepared by solid state reaction. The room temperature flexural strength and fracture toughness of the material fabricated from the supercritically dried gels were 190 MPa and 2.2 MPa.m^1/2, respectively. These strength and fracture toughness values are higher than those reported in other studies for YAG produced by the sintering route.     

The thermal conductivity of liquid 1,1,1,2-tetrafluoroethane (HFC 134a)

The thermal conductivity of HFC 134a was measured in the liquid phase with the polarized transient hot-wire technique. The experiments were performed at temperatures from 213 to 293 K at pressures up to 20 MPa. The data were analyzed to obtain correlations in terms of density and pressure. This study is part of an international project coordinated by the Subcommittee on Transport Properties of Commission 1.2 of IUPAC, conducted to investigate the large discrepancies between the results reported by various authors for the transport properties of HFC 134a, using samples of different origin. Two samples of HFC 134a from different sources have been used. The thermal conductivity of the first sample was measured along the saturation line as a function of temperature and the data were presented earlier. The thermal conductivity of the second one, the round-robin sample was measured as a function of pressure and temperature. These data were extrapolated to the saturation line and compared with the data obtained, previously in order to demonstrate the importance of the sample origin and their real purity. The accuracy of the measurements is estimated to be 0.5%. Finally, the results are compared with the existing literature data.