Joining of Ti-coated monolithic SiC using a SiCw/Ti3SiC2 filler by electric field-assisted sintering

Monolithic SiC, for the first time, was successfully joined using a SiC whisker-reinforced Ti₃SiC₂ composite (SiC_w/Ti₃SiC₂) filler via electric field-assisted sintering technique. A thin Ti coating layer was formed on the SiC surface to minimize the residual stress at the joint interface by transforming it into a TiC gradient layer. After optimizing process parameters, a joint strength higher than 250 MPa was obtained, which is higher than the other values reported in the literature. Failure occurred at the SiC base rather than the joining interface because of the improved joint strength by the incorporation of SiC_w. The addition up to 15 wt. % SiC_w in the filler layer improved the joint strength by various strengthening mechanisms. On the other hand, the joint strength was lower with 20 wt. % SiC_w addition, indicating the importance of thermal expansion mismatch between SiC_w and Ti₃SiC₂ to obtain a sound SiC joint.     

High-strength SiC joints with a novel in-situ formed SiC/Al4SiC4 joining filler

The in-situ formed SiC/Al₄SiC₄ joining layer was used to join monolithic SiC using an electric field-assisted sintering technique. A multiphase powder of Al₄C₃/SiC/Al₄SiC₄ was used as the initial joining material to obtain the in-situ reaction layer of SiC/Al₄SiC₄ via the appropriate interface reactions. The bending strength as high as 240.5 ± 6.6 MPa was obtained for the sample joined at 1800 °C, which was higher than the strength of the un-joined SiC matrix. Sound joints were obtained when Al₄C₃ was completely transformed to Al₄SiC₄, and a fully dense SiC/Al₄SiC₄ joining layer was consolidated. The integration of the joining layer with the SiC matrix was improved by a high amount of liquid phase formed at the interface. The proposed SiC/Al₄SiC₄ joining layer, with good thermal matching with SiC matrix, shows a great potential to be applied as a joining material for SiC-based ceramic matrix composites.     

Fast seamless joining of SiCw/Ti3SiC2 composite using electric field-assisted sintering technique

A pair of Ti₃SiC₂ reinforced with SiC whiskers (SiC_w/Ti₃SiC₂) composites was successfully joined without any joining materials using electric field-assisted sintering technology at a temperature as low as 1090°C (T_i) and a short time of 30 s. The microstructure and mechanical properties of the obtained SiC_w/Ti₃SiC₂ joints were investigated. The solid-state diffusion was the main joining mechanism, which was facilitated by a relatively high current density (~586 A/cm²) at the joining interface. The shear strength of the sample joined at 1090°C was 51.8 ± 2.9 MPa. The sample joined at 1090°C failed in the matrix rather than at the interface, which confirmed that a sound inter-diffusion bonding was obtained. A rapid and high efficient self-joining process may find application in the case of SiC_w/Ti₃SiC₂ sealing cladding tube and end cap.     

Low temperature seamless joining of SiC using a Ytterbium film

Monolithic SiC, for the first time, was seamless joined at a low temperature of 1200 °C using electric field-assisted sintering technology. A 300 nm Yb coating on SiC was used as the joining filler to form Yb₃Si₂C₂ via an in-situ reaction with the SiC. A liquid phase was formed by an eutectic reaction between Yb₃Si₂C₂ and SiC. Almost completely seamless joints were formed by the precipitated SiC grains, which were fully consolidated with the SiC matrix with the help of in-situ formed liquid phase, followed by its elimination under the uniaxial pressure. The bending strength of the seamless joint joined at 1500 °C for 15 min was as high as 257.2 ± 31.1 MPa, which was comparable to the strength of the SiC matrix. As a result, the failure occurred in the matrix indicated a sound joint was obtained. The proposed low temperature seamless joining could potentially be used for joining of SiC-based composite.     

Joining of SiC using CoFeCrNiCuTi high entropy alloy filler by electric current field assisted sintering

SiC ceramics were brazed by electric field-assisted sintering technology using CoFeCrNiCuTi high-entropy alloy as joining filler. The effect on the interface microstructure and bend strength of brazed joints at different brazing temperature was systemically studied. The interfacial reaction was controlled by adjusting the brazing temperature. The main components in the brazing seam are high-entropy alloys FCC (HEAF), C, TiC, CrC, and Cr₂₃C₆ phase. Furthermore, the maximum bending strength of 54 MPa was found when brazed at a lower temperature of 1125℃. In addition, due to the electric field-assisted sintering technology and the high-entropy effect of the CoFeCrNiCuTi filler, the diffusion of elements and the formation of solid solution were accelerated. This suggests that the current field was beneficial to improve the inter-diffusion between the CoFeCrNiCuTi filler and SiC ceramics. Consequently, the low-temperature rapid brazing of SiC ceramics was realized, and this technology provides a new filler system for ceramic brazing.     

Almost seamless joining of SiC using an in-situ reaction transition phase of Y3Si2C2

A new design of seamless joining was proposed to join SiC using electric field-assisted sintering technology. A 500 nm Y coating on SiC was used as the initial joining filler to obtain a desired transition phase of Y₃Si₂C₂ layer via the appropriate interface reactions with the SiC matrix. The phase transformation and decomposition of the transition phase of Y₃Si₂C₂ was designed to achieve almost seamless joining of SiC. The decomposition of the joining layer to SiC, followed up by the inter-diffusion and complete densification with the initial SiC matrix, resulted in the formation of an almost seamless joint at the temperature of 1900 °C. The bending strength of the seamless joint was 134.8 ± 2.1 MPa, which was comparable to the strength of the SiC matrix. The proposed design of seamless joining could potentially be applied for joining of SiC-based ceramic matrix composites with RE₃Si₂C₂ as the joining layer.     

Improved additive manufacturing of silicon carbide parts via pressureless electric field-assisted sintering

High solids loading silicon carbide (SiC)-based aqueous slurries containing only .5 wt. % organic additives were utilized to create specimens of various geometries via an extrusion-based additive manufacturing (AM) technique. Pressureless electric field-assisted sintering was performed to densify each specimen without deformation. The combination of these techniques produced parts with >98% relative density despite containing only 5 wt.% oxide sintering additives. After sintering, specimens contained only the α-SiC and yttrium aluminum perovskite phases. This suggests the evolution of a nonequilibrium yttrium aluminate phase, as well as transformation from β-SiC to α-SiC. The fabrication method presented in this work has advantages over other AM techniques commonly used with SiC, because it does not require significant organic additives nor additional postprocessing steps such as chemical vapor infiltration or polymer impregnation and pyrolysis.     

Joining of C/SiC composites by spark plasma sintering technique

CVD–SiC coated C/SiC composites (C/SiC) were joined by spark plasma sintering (SPS) by direct bonding with and without the aid of joining materials. A calcia-alumina based glass–ceramic (CA), a SiC + 5 wt% B₄C mixture and pure Ti foils were used as joining materials in the non-direct bonding processes. Morphological and compositional analyses were performed on each joined sample. The shear strength of joined C/SiC was measured by a single lap test and found comparable to that of C/SiC.     

Low-temperature Pr3Si2C2-assisted liquid-phase sintering of SiC with improved thermal conductivity

A novel Pr₃Si₂C₂ additive was uniformly coated on SiC particles using a molten-salt method to fabricate a high-density SiC ceramics via liquid-phase spark plasma sintering at a relatively low temperature (1400°C). According to the calculated Pr–Si–C-phase diagram, the liquid phase was formed at ∼1217°C, which effectively improved the sintering rate of SiC by the solution–reprecipitation process. When the sintering temperature increased from 1400 to 1600°C, the thermal conductivity of SiC increased from 84 to 126 W/(m K), as a consequence of the grain growth. However, an increasing amount of the sintering additive increased the interfacial thermal resistance, resulting in a decrease of thermal conductivity of the materials. The highest thermal conductivity of 141 W/(m K) was obtained for the material having the largest SiC grains and an optimized amount of the additive at the grain boundaries and triple junctions. The proposed Pr₃Si₂C₂-assisted liquid-phase sintering of SiC can be potentially used for the fabrication of SiC-based ceramic composites, where a low sintering temperature would inhibit the grain growth of SiC fibers.     

Seamless joining of silicon carbide ceramics through an sacrificial interlayer of Dy3Si2C2

A ternary carbide Dy₃Si₂C₂ coating was fabricated on the surface of SiC through a molten salt technique. Using the Dy₃Si₂C₂ coating as the joining interlayer, seamless joining of SiC ceramic was achieved at temperature as low as 1500 °C. Phase diagram calculation indicates that seamless joining was achieved by the formation of liquid phase at the interface between Dy₃Si₂C₂ and SiC, which was squeezed out under pressure and continuously consumed by the joining interlayer. This work implies the great potential of the family of ternary rare-earth metal carbide Re₃Si₂C₂ (Re = Y, La-Nd) as the sacrificial interlayer for high-quality SiC joining.     

Solid-state joining of SiC using a thin Ti3AlC2, TiC,or Ti filler

SiC monoliths containing 5 wt.% Al₂O₃-Y₂O₃ additive were joined using a thin Ti₃AlC_2, TiC, or Ti filler. After joining at 1900 °C for 5 h under 3.5 MPa, the joint properties were compared in terms of the microstructure, phase evolution, joining strength, and possible elimination of the joining layer. Although all samples showed a sound joint, the microstructure differed according to the filler. SiC joined with Ti₃AlC₂ filler showed an indistinguishable joining interface due to the filler decomposition followed by solid-state diffusion into the SiC base, whereas TiC filler remained at the interface without showing decomposition or diffusion. In contrast, the Ti filler showed a possible elimination of the joining layer because of the diffusion of Ti and the formation of TiC. The mean joining strengths for the Ti₃AlC₂, TiC, and Ti fillers were 300, 234, and 248 MPa, respectively, which were comparable to that of the base SiC material (250 MPa).     

Microstructure and mechanical properties of Cf/SiC composite joints joined using AlCoCrFeNi2.1 eutectic high-entropy alloy filler via spark plasma sintering

C_f/SiC composites were joined by spark plasma sintering technology using AlCoCrFeNi_2.1 eutectic high-entropy alloy as the joining filler. The typical structure of the joint could be described as C_f/SiC/CrSi₂ + HEAF + Al₄C₃ + C-rich phase/HEAF/CrSi₂ + HEAF + Al₄C₃ + C-rich phase/C_f/SiC. Under the pressure of 30 MPa and at 1450 ℃ for 10 min, the shear strength of the joint was 9.85 MPa at room temperature. However, when a 50 µm thick Ti foil was added to obtain Ti foil/AlCoCrFeNi_2.1/Ti foil composite filler, the joint strength was remarkably increased to 21.15 MPa at room temperature. The formation of TiC phase relieved the thermal stress at the joining interface. Due to the high entropy effect of AlCoCrFeNi_2.1 filler, the central zone of the joint still contained the FCC structure of high-entropy alloy. The existence of the pulsed electric field was beneficial to element diffusion and microstructure homogenization, which improved the mechanical properties of the joint while shortening the joining cycle.     

Joining of SiCf/SiC using a layered Ti3SiC2-SiCw and TiC gradient filler

A layered filler consisting of Ti₃SiC₂-SiC whiskers and TiC transition layer was used to join SiC_f/SiC. The effects of SiC_w reinforcement in Ti₃SiC₂ filler were examined after joining at 1400 or 1500 °C in terms of the microstructural evolution, joining strength, and oxidation/chemical resistances. The TiC transition layer formed by an in-situ reaction of Ti coating resulted in a decrease in thermal expansion mismatch between SiC_f/SiC and Ti₃SiC₂, revealing a sound joint without cracks formation. However, SiC_f/SiC joint without TiC layer showed formation of cracks and low joining strength. The incorporation of SiC_w in Ti₃SiC₂ filler showed an increase in joining strength, oxidation, and chemical etching resistance due to the strengthening effect. The Ti₃SiC₂ filler containing 10 wt.% SiC_w along with the formation of TiC was the optimal condition for joining of SiC_f/SiC at 1400 °C, showing the highest joining strength of 198 MPa as well as improved oxidation and chemical resistance.     

Rapidly achieving a reliable full-ceramic interface of ZrC-SiC composite using Ti interlayer via pulsed electric current joining

A reliable full-ceramic interface of ZrC-SiC composite was achieved rapidly at low temperature via pulsed electric current joining. Using a Ti foil as joining interlayer, the Zr and Si atoms reacted with Ti to form Ti₃Zr₃Si₃, while the dissolved C precipitated in form of TiC. The current delivering during joining promoted the atomic diffusion and caused the preferential growth of TiC, rapidly achieving a full-ceramic interface at 1300 ℃. Evaluating the reliability by Weibull distribution, the full-ceramic interface exhibited a considerable characteristic strength of 178 MPa, and its reliability was better than the raw ZrC-SiC composite. The in-situ formed ceramic interface toughened the joint via the mechanism of multi-cracking, crack deflection and termination. The proposed method provides a practical technology for the rapid joining of ultra-high temperature composites or the construction of layered composites with high toughness at low temperature.     

Fast interdiffusion and Kirkendall effects of SiC-coated C/SiC composites joined by a Ti-Nb-Ti interlayer via spark plasma sintering

SiC-coated 3D C/SiC composites were successfully joined with a Ti-Nb-Ti interlayer by SPS. When joined at 1200 °C, the apparent shear strength of the samples was as high as 61 ± 6 MPa as a result of an appropriate interface diffusion reaction. However, higher joining temperature (1600 °C) resulted in significantly lower shear strengths, and this was associated with the observed depletion of Si atoms and Kirkendall voids at the joining interface. Subsequently, a detailed characterization was performed by FIB/TEM/STEM. The interdiffusion mechanism of the samples during the joining process was revealed by thermodynamics and diffusion kinetics, and different interdiffusion mechanisms were associated with the evolution of the phase composition. The micro voids formed via Kirkendall effect were observed to grow rapidly with the joining temperature, resulting in catastrophic joint failure. Finally, these results were used to propose a failure model for the joints.     

Flash joining of CVD-SiC coated Cf/SiC composites with a Ti interlayer

Flash joining of CVD-SiC coated C_f/SiC samples with a Ti interlayer was achieved using a Spark Plasma Sintering machine. The influence of different heating powers and discharge times were investigated. The sample flash joined at a maximum heating power of 2.2 kW (peak electric current of 370 A) within 7 s showed the highest apparent shear strength of 31.4 MPa, which corresponds to the interlaminar shear strength of the composites. A maximum joining temperature of ∼1237 °C was reached during the flash joining. An extremely rapid heating rate of 9600 °C/min combined with a very short processing time hindered any reaction between the CVD-SiC coating and the Ti interlayer. The formation of a metallic joint (Ti based) in the absence of any detectable reaction phase is proposed as a new joining mechanism. For a conventionally joined SPS sample, the formation of titanium silicide phases inhibited the formation of a bond.     

Two-step pulsed electric current sintering of transparent Al2O3 ceramics

Abstract

Fully densified Al₂O₃ ceramics with fine grain size were obtained by pulsed electric current sintering through a two-step heating profile (referred to as TS-PECS). Highly transparent Al₂O₃ polycrystals with fine grain size (400 nm) were successfully fabricated by the TS-PECS process, namely, sintering at 1000°C for 1 h and followed at 1200°C for 20 min under uniaxial pressure of 100 MPa. Effects of the first step temperature and heating rate were discussed for bulk density, grain size and transparency. The temperature in the first step strongly affects densification and grain growth of Al₂O₃. On the other hand, heating rate, even of 100 K min^?1, in TS-PECS does not give significant influences on densification and grain growth of Al₂O₃. Inline transmittance at 640 nm in wavelength normalised to 1 mm in thickness is increased by decreasing heating rate even in TS-PECS.     

Fabrication and properties of Si2N2O-Si3N4 ceramics via direct ink writing and low-temperature sintering

Direct ink writing (DIW) and low-temperature sintering methods were applied to prepare Si₂N₂O-Si₃N₄ ceramics for radome materials. Lattices of Si-SiO₂ green body were printed by DIW with 78 wt % solid portion of water-based Si-SiO₂ slurry, in which silicon particles and silica fume were used as the solid portion and Methylcellulose (HPMC) was used as the dispersant. Effects of HPMC addition on stability and silica fume content on rheological properties of the slurry were studied, respectively. The pseudoplastic mechanism of the slurry was analyzed. The Si-SiO₂ green bodies were sintered at 1250 °C–1400 °C in nitrogen. The effect of temperature on phase composition, microstructure, mechanical and dielectric properties of samples was investigated. With the HPMC addition of 0.12 wt% and the silica fume proportion of 30 wt% in solid portion, a stable and pseudoplastic slurry with the yield stress of 110.9 Pa was obtained, which is suitable for DIW. With the decrease of initial holding temperature, more N₂ enters the sample and reacts with silicon and silica fume, promoting the generation of Si₂N₂O and Si₃N₄. The optimal condition yields Si₂N₂O-Si₃N₄ ceramics with apparent porosity of 42.73%, compressive strength of 24.7 MPa, dielectric constant of 4.89 and loss tangent of 0.0054. It is found that columnar Si₃N₄ comes from a direct reaction between silicon and N₂, and fibrous Si₂N₂O is mainly generated by the reaction between silicon, SiO(g), and N₂ through the chemical vapor deposition mechanism. Good dielectric properties are achieved due to high porosity, high proportion of Si₂N₂O phase and no residual silicon.     

Fabrication of highly dense Si3N4 via record low-content additive system for low-temperature pressureless sintering

Dense Si₃N₄ ceramics were fabricated by pressureless sintering at a low temperature of 1650°C with a short holding period of 1 h under a nitrogen atmosphere. The role of ternary oxide additives (Y₂O₃–MgO–Al₂O₃, Y₂O₃–MgO–SiO₂, Y₂O₃–MgO–ZrO₂) on the phase, microstructure, and mechanical properties of Si₃N₄ was examined. Only 5 wt.% of Y₂O₃–MgO–Al₂O₃ additive was sufficient to achieve >98% of theoretical density with remarkably high biaxial strength (∼1200 MPa) and prominent hardness (∼15.5 GPa). Among the three additives used, Y₂O₃–MgO–Al₂O₃ displayed the finest grain diameter (0.54 μm), whereas Y₂O₃–MgO–ZrO₂ produced the largest average grain diameter (∼0.95 μm); the influence was seen on their mechanical properties. The low additive content Si₃N₄ system is expected to have superior high-temperature properties compared to the system with high additive content. This study shows a cost-effective fabrication of highly dense Si₃N₄ with excellent mechanical properties.     

Pulsed electric current sintering of transparent Cr-doped Al2O3

Pulsed electric current sintering (PECS) was applied to obtain transparent ruby polycrystals. Al₂O₃-Cr₂O₃ powder mixture was prepared by drying an aqueous slurry consisting of Al₂O₃ and Cr(NO₃)₃ followed by PECS consolidation in vacuum at a sintering temperatures ranging from 1100 to 1300 °C with various heating rates between 2 and 100 °C/min and under an applied pressures from 40 to 100 MPa. Slow heating rate and high-pressure lead to highly densified and transparent Cr-doped Al₂O₃ polycrystals at sintering temperature of 1200 °C.