Impedance matching optimization of SiCf/Si3N4–SiOC composites for excellent microwave absorption properties

SiC fiber reinforced ceramic matrix composites (SiC_f-CMCs) are considered to be one of the most promising materials in the electromagnetic (EM) stealth of aero-engines, which is expected to achieve strong absorption and broad-band performance. Multiscale structural design was applied to SiC_f/Si₃N₄–SiOC composites by construction of micro/nanoscale heterogeneous interfaces and macro double-layer impedance matching structure. SiC_f/Si₃N₄–SiOC composites were fabricated by using SiC fibers with different conductivities and SiOC–Si₃N₄ matrices with gradient impedance structures to improve impedance matching effectively. Owing to its unique structure, SiC_f/Si₃N₄–SiOC composites (A3-composites) achieved excellent EM wave absorption performance with a minimum reflection coefficient (RC_min) of ?25.1 dB at 2.45 mm and an effective absorption bandwidth (EAB) of 4.0 GHz at 2.85 mm in X-band. Moreover, double-layer SiC_f/Si₃N₄–SiOC with an improved impedance matching structure obtained an RC_min of ?56.9 dB and an EAB of 4.2 GHz at 3.00 mm, which means it can absorb more than 90% of the EM waves in the whole X-band. The RC is less than ?8 dB at 2.6–2.8 mm from RT to 600 °C in the whole X-band, displaying excellent high-temperature absorption performance. The results provide a new design opinion for broad-band EM absorbing SiC_f-CMCs at high temperatures.     

Interfacial microstructure characterization and strength evaluation of Si3N4/Si3N4 joints with Si–Mg composite filler for high-temperature applications

Silicon-nitride (Si₃N₄) components were joined under vacuum at 1100 °C for 10 min using Si–Mg composite fillers with Mg contents (X_Mg) that ranged from 0 at.% to 59 at.%. The Si₃N₄/Si₃N₄ joints were fabricated via Si layer formation at the joint interface; the molten Si–Mg liquid was transformed into a solid Si layer after Mg-evaporation-induced isothermal solidification. The joint tensile strength at room temperature increased considerably when X_Mg exceeded the liquidus composition of 37 at.% because of the enhanced densification/thinning of the Si layer. In these cases, some Mg atoms reacted with Si₃N₄ to form a fine-grained MgSiN₂-based layer, whereas relatively large (>0.1 μm) and smaller MgO precipitates (<10 nm) were observed in the Si layer. At a high X_Mg, the MgO precipitates were arranged in a network-like structure, which improved the fracture strength of the Si layer. The joints with a high strength at room temperature were examined using a three-point bending test at 1200 °C in air and endured a maximum fracture stress of ~200 MPa, which confirmed their potential for use in oxidizing atmospheres at least 100 °C above the bonding temperature.     

Superior high-temperature oxidation resistance of magnetron sputtered Hf–B–Si–C–N film

A hard and optically transparent amorphous Hf₇B₂₃Si₁₇C₄N₄₅ film with a contamination level less than 4 at%, prepared by reactive pulsed dc magnetron sputtering, was subjected to systematic investigation of high-temperature oxidation behavior in air up to 1700 °C. We focus on thermogravimetric analysis of the film in air and on the evolution of the film structure, microstructure and elemental composition with an annealing temperature ranging from 1100 °C to 1700 °C. The film exhibits a superior oxidation resistance up to 1600 °C due to a formation of a nanocomposite protective oxide layer on the surface above 1000 °C. The layer consists of monoclinic and tetragonal (or orthorhombic) HfO₂ nanocrystallites surrounded by a SiO₂-based amorphous matrix, most probably containing boron. The HfO₂ nanocrystallites exhibit a gradient in size with a dense population of small (a couple of nm) crystallites next to the interface and larger but dispersed crystallites close to the surface.     

Construction of Si3N4/SiO2/SiC–Y2Si2O7 composite ceramics with gradual impedance matching structure for high-temperature electromagnetic wave absorption

Good impedance matching is vital in upgrading the performance of electromagnetic (EM) wave-absorbing materials. In this study, Si₃N₄/SiO₂/SiC–Y₂Si₂O₇ composite ceramics were synthesized by sintering and chemical vapor infiltration (CVI) technology with gradual impedance matching. The relationship between the microstructure of the as-prepared composite ceramics and EM wave absorption characteristics was thoroughly explored. It was found that the amorphous Si₃N₄, SiO₂, and SiC layers were constructed with a gradual impedance matching structure, which not only improved impedance matching but also increased the number of nano interfaces. More importantly, SiC nanocrystals effectively increased the conduction loss, and the presence of defects and nanoscale heterogeneous interfaces further increased the polarization loss. Consequently, the as-prepared composite ceramics displayed enhanced EM wave absorption properties, with a minimum reflection coefficient (RC_min) value of less than ?20 dB over a temperature range of 25 °C (RT)-300 °C, and an effective absorption bandwidth (EAB) maintained at 4.2 GHz with the thickness range of 3.75–4.75 mm. These results demonstrated the practical significance of high-performance EM wave absorption materials that can be applied in high-temperature and water vapor environments.     

Preparation of SiCf/Si–O–C composites by impregnation pyrolysis of polysiloxane and its electromagnetic wave absorption properties

High-temperature structural electromagnetic wave (EMW) absorption materials are increasing in demand because they can simultaneously possess the functions of mechanical load-bearing, heatproof, and EMW absorption. Herein, SiC_f/Si–O–C composites were prepared by precursor impregnation pyrolysis using continuous SiC fibers needled felt as reinforcement and polysiloxane as a precursor, respectively. The phase composition, microstructure, complex permittivity, and EMW absorption properties of SiC_f/Si–O–C composites after annealing at various temperatures were investigated. The annealing at 1400–1500°C affects positively the EMW absorption performance of the composites, because the β-SiC microcrystals and SiC nanowires were generated by the activation of carbothermal reduction reaction in the composites, and the aspect ratio of SiC nanowires increased with the rise of temperature. The composites exhibit optimal EMW absorption performance, with the effective absorption bandwidth covering the entire X-band and the minimum reflection loss (RL_min) of −32.8 dB at 4.0 mm when the annealing temperature is raised to 1500°C. This is because that the impedance matching is improved as the rising of ε′ and decreasing of ε″ due to the conversion of free carbon in the composite into SiC nanowires.     

Joining of Cf/SiC composites and Si3N4 ceramic with Y2O3–Al2O3–SiO2 glass filler for high-temperature applications

C_f/SiC composites and Si₃N₄ ceramics are candidate materials for applications in thermal protection system. This paper investigated the joining of C_f/SiC and Si₃N₄ using Y₂O₃–Al₂O₃–SiO₂ glass. The reliability of joints was evaluated by thermal shock tests. In this present work, the typical joint structure was C_f/SiC-glass-Si₃N₄. The results demonstrate that Direct bonding has been identified as the interfacial bonding mechanism at the SiC/glass and glass/Si₃N₄ interfaces. The maximum shear strength of the C_f/SiC–Si₃N₄ joint was ~34 MPa, which delivered an effective method to achieve strong, reliable bonding between the dissimilar materials. In addition, after thermal shock for 10 cycles, the residual strength remained ~13 MPa. Bubbles instead of microcracks formed in the glass filler, which was the main factor causing the degradation of the joint performance. It is suggested that improving the high temperature resistance of joining materials is the key to realize the application of this joint structure.     

Production and EDM of Si3 N4–TiB2 ceramic composites

Abstract

Ceramic matrix composites containing TiB₂ as a particulate phase have been produced by hot pressing. The problems of the reactivity of TiB₂ with the Si₃ N₄ matrix and with the sintering environment have been successfully addressed. A novel dual atmosphere sintering profile combined with low temperature hot pressing has been used to successfully produce fully dense materials. The effect of TiB₂ addition on mechanical properties has been investigated. Composites containing TiB₂ show significant improvements in hardness and fracture toughness. The addition of TiB₂ at a level of 40 vol.-% raises the conductivity of the composite to a level where electro-discharge machining (EDM) is possible. A comprehensive study of the application of EDM has been carried out and the optimum machining conditions have been identified. Under these conditions Si₃ N₄–TiB₂ composites have been shaped with relative ease and proved to be ‘robust’ materials under EDM.     

Enhancement on high-temperature microwave absorption properties of TiB2–MgO composites with multi-interfacial effects

TiB₂–MgO microwave absorbing materials with TiB₂ as the absorber, MgO as the matrix are prepared by spark plasma sintering (SPS). The influences of commercial TiB₂ content and sintering temperature on dielectric and microwave absorption (MA) properties are studied. Besides, to optimize the MA performance, TiB₂–MgO composite containing TiB₂ synthesized by the carbonthermal process is prepared. Meanwhile, its high-temperature dielectric and MA properties are investigated. Indeed, both the commercial TiB₂ content and sintering temperature play key roles in dielectric and MA properties, as they reaching 8 wt% and 1400 °C, the composite presents the optimal MA performance. For composite with synthetic TiB₂ as the absorber, the temperature has a positive effect on dielectric and MA properties. The enhanced high-temperature MA properties with minimum reflection loss (RL_min) of ?52.11 dB at 1.6 mm under 500 °C and effective absorption bandwidth (EAB, RL < ?5 dB) of 4.2 GHz at 1.4–1.6 mm under 800 °C are obtained, which is mainly attributed to the temperature-dependent interfacial polarization compared to the temperature-insensitive conductivity. The excellent mechanical properties (flexural strength = 212.48 MPa), thin absorbing layer (d < 2 mm), enhanced thermal stability and high-temperature MA properties indicate that the TiB₂–MgO composites can be considered as new candidates for high-temperature structure microwave absorbing materials.     

Simultaneous enhancement of mechanical and microwave absorption properties with a novel in-situ synthesis α-Al2O3 fillers for SiCf/SiC composites

The Al and H₃BO₃ mixed powder was introduced into the PCS/Xylene precursor solution as in-situ synthesis α-Al₂O₃ filler by precursor infiltration and pyrolysis (PIP) method. The in-situ synthesis filler can effectively decrease the open porosity of SiC_f/SiC composites and give rise to multiple scattering of microwave and dipolar polarization. Therefore, the mechanical and microwave absorption properties of SiC_f/SiC composites can be simultaneously enhanced. The effects of in-situ synthesis filler on the morphologies, flexure strength and reflection loss values of SiC_f/SiC composites were investigated. With 2 wt% in-situ synthesis filler, the flexure strength of SiC_f/SiC composite was 305 MPa and the maximum reflection loss (RL_m) can reach ? 54.68 dB with the effective absorption band (EAB) of 3.51 GHz in the X band. With 5 wt% in-situ synthesis filler, the flexure strength of SiC_f/SiC composite was 207 MPa and the RL_m was ? 30.91 dB. Due to the inefficient infiltration process, the RL_m of SiC_f/SiC composites with 10 wt% in-situ synthesis filler was only ? 27.36 dB. Nevertheless, the flexure strength of that composite was 259 MPa, owing to the dense matrix. Additionally, the flexure strength of SiC_f/SiC composite without filler was 148 MPa and the RL_m was ? 26.40 dB.     

Thermal shock resistance of Si3N4 and Si3N4–SiC ceramics with rare-earth oxide sintering additives

The influence of various rare-earth oxide additives and the addition of SiC nanoparticles on the thermal shock resistance of the Si₃N₄ based materials was investigated. The location of SiC particles inside the Si₃N₄ grains contributed to a higher level of residual stresses, which caused a failure at the lower temperature difference compared to the composites with a preferential location of the SiC at the grain boundaries. A critical temperature difference increased with an increasing ionic radius of RE³⁺ for both the composites and the monoliths. The critical temperature difference for the composite (580 °C) and the monolith (680 °C) sintered with La₂O₃ was significantly higher compared to the composite and the monolith doped with Lu₂O₃ (430 °C). A good agreement was found between the results of the critical temperature difference estimated by the indentation quench test and that obtained by the strength retention method.     

Synthesis and spark plasma sintering of Si3N4–ZrN self-healing composites

A Si₃N₄–ZrN wear-resistant self-healing composite material was developed. Si₃N₄–ZrN composite ultrafine powders were synthesized at a temperature of 1200 °С via solid-state reactions without milling and densified by spark plasma sintering at 1650 °C to a relative density of 97 ± 0.5%. Balls 13.494 mm in diameter for ball bearings manufactured by spark plasma sintering had a fine-grained structure with a grain size of 200–500 nm, Vickers hardness of 22.5 ± 1.8 GPa, and indentation fracture toughness of 6.2 ± 0.4 MPa. The tribological properties of the composite were investigated under static and dynamic loading. The self-healing capability of the Si₃N₄–ZrN composite was evaluated in the temperature range 500–550 °С. High-temperature three-point bending tests of notched specimens showed a bending strength of 383 ± 21 MPa at room temperature and 413 ± 30 MPa at 500 °С, which confirmed the self-healing of the composite.     

Microstructure,thermophysical properties and oxidation resistance of SiCf/SiC–YSi2–Si composite fabricated through reactive melt infiltration

As an ideal component material for advanced aeroengines, SiC composite faces severe challenges of high temperatures and oxidation. Here, a high-densification SiC_f/SiC–YSi₂–Si composite was prepared through combining PIP with RMI of Si–13 at% Y alloy to achieve enhanced performance at high temperatures. Based on the analysis of the microstructure and thermophysical properties, it found that the introduction of the highly crystalline Si–Y alloy can improve the high-temperature thermal conductivity of the composite through phonon and electron conduction. In addition, Y migrates to the surface and forms yttrium silicate with increasing oxidation temperature, which facilitates the excellent long-term oxidation resistance of the composite at 1200–1300 °C. Thus, the composite retained its high strength (89.15% and 86.84%) after oxidation at 1200 °C and 1300 °C for 100 h. The experimental results clearly demonstrate that the introduction of the Si–Y alloy is an effective way of preparing high-performance SiC composites.     

Influence of rare-earth oxide additives on the oxidation resistance of Si3N4–SiC nanocomposites

The influence of different rare earth oxide additives (La₂O₃, Nd₂O₃, Sm₂O₃, Y₂O₃, Yb₂O₃ and Lu₂O₃) on the oxidation behaviour of carbon derived Si₃N₄–SiC micro-nanocomposites has been investigated. All investigated composites exhibited predominately parabolic oxidation behaviour indicated diffusion as the rate limiting mechanism. Except the Si₃N₄–SiC composite sintered with Lu₂O₃ the rate-limiting oxidation mechanism for all other materials was an outward diffusion of the additive cations along the grain boundary towards the surface. Such diffusion of cation has been strongly suppressed in the Lu-doped composite because of the beneficial effect of stable grain boundary phase and the presence of the SiC particles predominately located at the grain boundaries of Si₃N₄. Nanoparticles at the grain boundaries act as the obstacles for migration of cations of the additives resulting in superior oxidation resistance of Si₃N₄–SiC–Lu₂O₃ where the rate-limiting step is inward diffusion of oxygen through the oxide layer to the bulk ceramics.     

Microstructure and oxidation resistance of C-AlPO4–mullite coating prepared by hydrothermal electrophoretic deposition for SiC-C/C composites

Oxidation resistant C-AlPO₄–mullite coating for SiC pre-coated carbon/carbon composites (SiC-C/C) was prepared by a novel hydrothermal electrophoretic deposition process. The phase composition, surface and cross-section microstructure of the as-prepared multi-layer coatings were characterized by X-ray Diffraction (XRD), scanning electron microscopy (SEM) and energy dispersive spectroscopy (EDS). The influence of deposition voltage on phase composition, microstructure and oxidation resistance of the as-prepared coatings was particularly investigated. Results show that the outer layer coating mainly composed of C-AlPO₄ and mullite phase can be achieved after the hydrothermal electrophoretic deposition. The thickness, density and anti-oxidation property of the C-AlPO₄–mullite coating was improved with the increase of deposition voltage from 160 V to 200 V. The multi-layer coating prepared at a voltage of 200 V exhibit excellent anti-oxidation property, which can effectively protect C/C composites from oxidation in air at 1773 K for 324 h with a weight loss of 1.01%. The failure of the multi-layer coatings is due to the generation of cross-holes in the coating, which cannot be self-cured by the metaphosphate and silicate glass layer after long time oxidation at 1773 K.     

High-strength and wave-transmitting Si3N4–Si2N2O-BN composites prepared using selective laser sintering

In this study, high-strength and wave-transmission silicon nitride (Si₃N₄) composites were successfully developed via selective laser sintering (SLS) with cold isostatic pressing (CIP) after debinding and before final sintering, and the optimal moulding process parameters for the SLS Si₃N₄ ceramics were determined. The effects of the sintering aids and secondary CIP on the bulk density, porosity, flexural strength, fracture toughness, and wave-transmitting properties of the Si₃N₄ composites were studied. The results showed that the increased CIP pressure was beneficial to the densification of SLS Si₃N₄ ceramics and improved their mechanical properties. However, the wave-transmitting performance decreased as the CIP pressure increased. The Si₃N₄ ceramics prepared by the moulding of sample S₁₁ were more in line with the performance requirements of the radomes. To obtain good comprehensive performance, an additional 3% of interparticle Y₂O₃ was added to the pre-printed mixed powder of granulated Si₃N₄ particles and resin and the secondary CIP pressure was adjusted to 280 MPa. After sintering, the bending strength, fracture toughness, and dielectric constant of the Si₃N₄ ceramics were 651 MPa, 6.0 MPa m^1/2, and 3.48 respectively. This study provides an important method for preparing of Si₃N₄ composite radomes using SLS process.     

Fabrication and contact resistivity of W–Si3N4/TiB2–Si3N4/p–SiGe thermoelectric joints

The design and fabrication of silicon germanium (SiGe) thermoelectric elements, typically including the selection of electrode and intermediate materials, the process of joining electrode and intermediate layer onto thermoelectric materials, are the major challenge for SiGe thermoelectric device technology. In this study, W–Si₃N₄ and TiB₂–Si₃N₄ composites are designed as the electrode and intermediate layer, respectively, and the W–i₃N₄/TiB₂–Si₃N₄/p–Si₈₀Ge₂₀B_0.6 joints are fabricated by a one-step spark plasma sintering process. The influences of the composition of TiB₂–Si₃N₄ intermediate layer on the interfacial structure, contact resistivity and interfacial thermal stability are investigated. The interfacial thermal stability is improved with increasing Si₃N₄ content in TiB₂–Si₃N₄ intermediate layer due to the reduced mismatch of coefficients of thermal expansion between the intermediate layer and SiGe. On the other hand, the contact resistivity increases with the rising of Si₃N₄ content due to the weakened TiB₂/SiGe ohmic contact, which degrades the device efficiency. As the balanced point, the intermediate layer with the composition of 80 vol% TiB₂+20 vol% Si₃N₄ provides good interfacial thermal stability and moderately small contact resistivity (~75 μΩ cm² after aging at 1000 °C for 120 h) simultaneously, which is an optimized intermediate layer composition for W–Si₃N₄/TiB₂–Si₃N₄/p–Si₈₀Ge₂₀B_0.6 thermoelectric element. The TiB₂–Si₃N₄ intermediate layer has excellent chemical stability to both W–Si₃N₄ electrode and SiGe thermoelectric material at high temperatures, which contributes to the sharp interface of the joint and effectively prevents the inter-diffusion between the electrode and the SiGe.     

Fabrication of Si3N4–SiC/SiO2 composites using 3D printing and infiltration processing

Si₃N₄–SiC/SiO₂ composites were prepared by employing three-dimensional (3D) printing using selective laser sintering (SLS) and infiltration processing. The process was based on the infiltration of silica sol into porous SLS parts, and silicon carbide and silicon nitride particles were bonded by melted nano-sized silica particles. To optimize the manufacturing process, the phase compositions, microstructures, porosities, and flexural strengths of the Si₃N₄–SiC/SiO₂ composites prepared at different heat-treatment temperatures and infiltration times were compared. Furthermore, the effects of the SiC mass fraction and the addition of Al₂O₃ and mullite fibers on the properties of the Si₃N₄–SiC/SiO₂ composites were investigated. After repeated infiltration and heat treatment, the flexural strength of the 3D-printed Si₃N₄–SiC/SiO₂ composite increased significantly to 76.48 MPa. Thus, a Si₃N₄–SiC/SiO₂ composite part with a complex structure was successfully manufactured by SLS and infiltration processes.     

TaB2–SiC–Si multiphase oxidation protective coating for SiC-coated carbon/carbon composites

To improve the oxidation resistance of the carbon/carbon (C/C) composites, a TaB₂–SiC–Si multiphase oxidation protective ceramic coating was prepared on the surface of SiC coated C/C composites by pack cementation. Results showed that the outer multiphase coating was mainly composed of TaB₂, SiC and Si. The multilayer coating is about 200 μm in thickness, which has no penetration crack or big hole. The coating could protect C/C from oxidation for 300 h with only 0.26 × 10^?2 g²/cm² mass loss at 1773 K in air. The formed silicate glass layer containing SiO₂ and tantalum oxides can not only seal the defects in the coating, but also reduce oxygen diffusion rates, thus improving the oxidation resistance.