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.     

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.     

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.     

Microstructure and mechanical properties of SiC-SiC joints joined by spark plasma sintering

The development of reliable joining technology is of great importance for the full use of SiC. Ti₃SiC₂, which is used as a filler material for SiC joining, can meet the demands of neutron environment applications and can alleviate residual stress during the joining process. In this work, SiC was joined using different powders (Ti₃SiC₂ and 3Ti/1.2Si/2C/0.2Al) as filler materials and spark plasma sintering (SPS). The influence of the joining temperature on the flexural strength of the SiC joints at room temperature and at high temperatures was investigated. Based on X-ray diffraction and scanning electron microscopy analyses, SiC joints with 3Ti/1.2Si/2C/0.2Al powder as the filler material possess high flexural strengths of 133 MPa and 119 MPa at room temperature and at 1200 °C, respectively. The superior flexural strength of the SiC joint at 1200 °C is attributed to the phase transformation of TiO₂ from anatase to rutile.     

Improved shear strength of SiC-coated 3D C/SiC composite joints with a tailored Ti-Si-C interlayer

SiC-coated 3D C/SiC composites were successfully joined using SPS technology with a Ti-Si-C interlayer. The interface morphologies, phase composition, and mechanical properties of the joints were investigated in detail. By adjusting the joining temperature, the interlayer transitioned, in situ, from Ti-Si-C compounds to Ti₃SiC₂ grains without decomposition. Because of the plastic deformation behavior of Ti₃SiC₂ grains, the ability of the interlayer to inhibit crack propagation increased. For joints with different interlayer thickness, the distribution of thermal residual stress was calculated using finite element analysis, and the distribution was associated with the evolution of interlayer morphologies, which was eventually used to establish fracture models. Optimized bonding was achieved without erosion of carbon fibers and also without interfacial defects. Finally, a reliable joint with shear strength of 51 ± 3.0 MPa was obtained by precisely controlling the interlayer reaction and optimizing thermal residual stress.     

Microstructural evolution and growth kinetics of interfacial reaction layers in SUS430/Ti3SiC2 diffusion bonded joints using a Ni interlayer

Ti₃SiC₂ ceramic and SUS430 stainless steel (SS) were successfully joined by a solid diffusion bonding technique using Ni interlayers. Diffusion bonding was performed in the temperature range of 850 °C–1100 °C under vacuum. The interfacial reaction phase, morphology evolution, growth kinetics and tensile strength were systematically investigated. In all cases, the inter-diffusion and reaction between Ti₃SiC₂ and SS can be effectively prevented by Ni foil, and the good transition in the joint benefit to the sound joining. The interface in the joints adjacent to SS matrix was composed of γ solid solution and a small amount of σ intermetallic compound. The compounds in the Ni/Ti₃SiC₂ interface was Ni/Ni(Si)/Ni₃₁Si₁₂ + Ni₁₆Ti₆Si₇ + Ti₃SiC₂ + TiC_x/Ti₂Ni + Ti₃SiC₂ + TiC_x/Ti₃SiC₂, which formed by the inter-diffusion and chemical reactions between Si and Ni atoms. The diffusion mechanism and reaction mechanism were interrelated, and decided the width of each reaction zones. Furthermore, the diffusion activation energy was 113 kJ/mol. The tensile strength increases with increasing the bonding temperature. The minimum and maximum strength of 32.3 MPa and 88.8 MPa were obtained from SUS430/Ni/Ti₃SiC₂ joints, which bonding experiments were carried out at 850 °C and 1100 °C, respectively.     

Improving thermal stability of SiC whiskers via nanoscale Ti3SiC2 coatings

Effects of SiC whiskers (SiC_w) on the mechanical properties of composites largely depend on their thermal stability at high temperature. In this study, pure SiC_w and Ti₃SiC₂ coated SiC_w were thermal treated at 1600–1800°C for 1 h. Their phase assemblage, morphology, and structural evolution were investigated. Oxygen partial pressures in the graphite furnace resulted in the breakdown of SiC_w into particles at 1600°C, and the degradation became more pronounced with temperature increasing. The thermal stability of SiC whiskers at 1600–1700°C was significantly improved by a thin Ti₃SiC₂ coating on them, as both thermodynamic calculations and experimental observations suggest Ti₃SiC₂ coating could be preferentially oxidized/decomposed, prior to the active oxidation of SiC. At 1800°C, the protective role of the coating on the whiskers became weakened. SiC was converted into gaseous SiO and CO, with the remaining of interconnected TiC micro-rods and amorphous carbon.     

Microstructure and mechanical property of SiC whisker coating modified C/C composite/Ti2AlNb alloy dissimilar joints prepared by transient liquid phase diffusion bonding

SiC whisker coating was prepared on the surface of C/C composite successfully by CVD, and transient liquid phase (TLP) diffusion bonding was employed to realize the joining of SiC whisker coating modified C/C composite and Ti₂AlNb alloy using Ti–Ni–Nb foils as interlayer. The microstructure, shear strength and fracture behavior were investigated by scanning electron microscopy (SEM) with energy dispersive X-ray spectrometer (EDS), X-ray diffraction (XRD) and universal testing machine. The results show that SiC has good compatibility with C/C composite, and gradient interface formed between SiC-modified C/C composite and Ti₂AlNb alloy. When the bonding experiment was carried out under bonding temperature of 1040 °C and holding time of 30min with 5 MPa pressure in vacuum, the joints formed well and no obvious defects can be observed. The typical microstructure of joints is C/C composite/SiC + TiC/Ti–Ni compounds + Ti–Ni–Nb solid solutions/residual Nb/diffusion reaction layer/Ti₂AlNb alloy. With the increasing of bonding temperature, the thickness of joining area increased due to sufficient element diffusion. However, when bonding temperature is elevated to 1060 °C, some defects such as cracks and slag inclusions exist in the interface layer between interlayer and Ti₂AlNb. The joints with maximum average shear strength of 32.06 MPa are bonded at 1040 °C for 30min. C, SiC and TiC can be found on the fracture surface of joints bonded at 1040 °C which indicated that fracture occurred at the interface layer adjacent SiC layer.     

Ti3SiC2 interphase coating in SiCf/SiC composites: Effect of the coating fabrication atmosphere and temperature

The SiC fibers were coated with Ti₃SiC₂ interphase by dip-coating. The Ti₃SiC₂ coated fibers were heat-treated from 900 °C to 1100 °C in vacuum and argon atmospheres to comparatively analyze the effect of temperature and atmosphere on the microstructural evolution and mechanical strength of the fibers. The results show that the surface morphology of Ti₃SiC₂ coating is rough in vacuum and Ti₃SiC₂ is decomposed at 1100 °C. However, in argon atmosphere, the surface morphology is smooth and Ti₃SiC₂ is oxidized at 1000 °C and 1100 °C. At 1100 °C, Ti₃SiC₂ oxidized to form a thin layer of amorphous SiO₂ embedded with TiO₂ grains. Meanwhile, defects and pores appeared in the interphase scale. As a result, the fiber strength treated in the argon was lower than that treated in vacuum. The porous Ti₃SiC₂ interphase fabricated under vacuum was then employed to prepare the SiC_f/SiC mini composite by chemical vapor infiltration (CVI) combined with precursor infiltration pyrolysis (PIP), and can effectively improve the toughness of SiC_f/SiC mini composite. The propagating cracks can be deflected within the porous interphase layer, which promotes fiber pull-outs under the tensile strength.     

Wetting behavior and brazing of titanium-coated SiC ceramics using Sn0.3Ag0.7Cu filler

By coating active titanium, Sn0.3Ag0.7Cu (SAC) filler wetted SiC effectively, as the contact angle decreased significantly from ~145° to ~10°. Ti₃SiC₂ and TiO_x (x ≤ 1) reaction layers were formed at the droplet/SiC interface, leading to the reduction of contact angle. Reliable brazing of SiC was achieved using titanium deposition at 900°C for 10 minutes, and the typical interfacial microstructure of Ti-coated SiC/SAC was SiC/TiO_x + Ti₃SiC₂/Sn(s,s). Comparing to direct brazing, Ti–Sn compounds in the brazing seam were effectively reduced and the mechanical property of joints was dramatically improved by titanium coating. The optimal average shear strength of SiC joints reached 25.3 MPa using titanium coating- assisted brazing, which was ∼62% higher than that of SiC brazed joints using SAC-Ti filler directly.     

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.     

Joining of SiCf/SiC using polycarbosilane and polysilazane preceramic mixtures

Polycarbosilane (PCS)/polysilazane (PSZ) preceramic mixtures with weight ratios of 100/0, 75/25, 50/50, 25/75, and 0/100 were used as a filler for the joining of SiC_f/SiC to obtain high purity SiC at the joining region. SiC_f/SiC was fabricated by the electrophoretic infiltration of a SiC-based matrix phase into Tyranno SA3 SiC fabrics followed by hot-pressing at 1750?°C under 20?MPa for 2?h in an Ar atmosphere. Microstructural analysis confirmed a sound join without cracks after joining at 1750?°C for 2?h under a pressure of 10?MPa. SiC was the only phase remaining at the joint when PCS was used, while a small amount of Si₃N₄ along with the main SiC were observed in the join using PSZ. The flexural strengths of the butt-joint SiC_f/SiC were 120 and 137?MPa for the samples joined using a pure PCS and PSZ at 1750?°C, respectively, whereas those joined using the mixture fillers showed relatively lower strength.     

High-strength SiC joints fabricated at a low-temperature of 1400°C using a novel low activation filler of Praseodymium

High-strength SiC joints were successfully obtained by electric current field-assisted sintering technique at a low temperature of 1400°C using a Pr coating (100 nm) as the initial joining filler. A Pr₃Si₂C₂ transient phase was formed in situ by the interfacial reaction, while the eutectic reaction between Pr₃Si₂C₂ and SiC at ∼1150°C resulted in the formation of a liquid phase. The liquid phase promoted the atomic diffusion at the interface and improved consolidation of the newly precipitated nano-sized SiC with the SiC matrix. This led to the formation of partially seamless joints of SiC. When the thickness of the joining layer decreased from 1 to 100 nm, the content of the residual Pr-O phase at the interface decreased, while the bending strength of the joints increased. A sound SiC joint with a bending strength of 227 ± 12 MPa was obtained at such a low temperature as 1400°C when a 100 nm Pr coating was applied.     

Ultrafast low-temperature near-seamless joining of Cf/SiC using a sacrificial Pr3Si2C2 filler via electric current field-assisted sintering technique

A novel layered structure material, Pr₃Si₂C₂, was synthesized at a low temperature of 850 °C using a molten salt approach for the first time, and subsequently used as the joining filler for carbon fibers reinforced SiC composites (C_f/SiC). A robust near-seamless C_f/SiC joint was successfully obtained at 1509 °C (T_i) for 30 s, while an ultrafast heating rate of 6000 °C/min was applied via electric field-assisted sintering technology. The near-seamless joining process was attributed to the newly precipitated SiC grains, which were densified well with the C_f/SiC matrix by liquid-assisted sintering. The liquid phase was in-situ formed by the eutectic reaction between Pr₃Si₂C₂ and SiC. The shear strength of the near-seamless joint obtained at 1509 °C for 30 s was 17.6 ± 3.0 MPa. The failure occurred in the C_f/SiC matrix. The formation of near-seamless C_f/SiC joints dismisses the issues related to thermal mismatch between C_f/SiC matrices and traditional joining fillers.     

The effects of preparation temperature on the SiCf/SiC 3D4d woven composite

Continuous silicon carbide fiber reinforced silicon carbide matrix (SiC_f/SiC) composites have promising applications in aero-engine due to their unique advantages, such as low density, high modulus and strength, outstanding high temperature resistance and oxidation resistance. As SiC fibers are main reinforcements in SiC_f/SiC composites, the crystallization rate and initial damage degree of SiC fibers are seriously influenced by preparation temperatures of SiC_f/SiC composites, namely mechanical properties of SiC fibers and SiC_f/SiC composites are influenced by preparation temperatures. In this paper, KD-II SiC fibers were woven into 3D4d preforms and SiC matrix was fabricated by PIP process at 1100 °C, 1200 °C, 1400 °C and 1600 °C. Digital image correlation (DIC) method was adopted to measure the uniaxial tensile properties of these SiC_f/SiC composites. In addition, finite element method (FEM) based on representative volume element (RVE) was adopted to predict the mechanical properties of SiC_f/SiC composites. The good agreements between numerical results and experimental results of uniaxial tensile tests verified the validity of the RVE. In last, the transverse tensile, transverse shear, uniaxial shear properties were predicted by this method. The predicted results illustrated that axial tensile, transverse tensile and axial shear properties were greatly influenced by the preparation temperatures of SiC_f/SiC composites while transverse shear properties were not significantly various. And the mechanical properties of SiC_f/SiC composites peaked at 1200 °C among these four temperatures while their values reached their lowest points at 1600 °C because of thermal damage and brittle failure of SiC_f/SiC composites.     

In-situ formation of Ti3SiC2 interphase in SiCf/SiC composites by molten salt synthesis

Titanium silicon carbide (Ti₃SiC₂) film was synthesized by molten salt synthesis route of titanium and silicon powder based on polymer-derived SiC fibre substrate. The pre-deposited pyrolytic carbon (PyC) coating on the fibre was utilized as the template and a reactant for Ti₃SiC₂ film. The morphology, microstructure and composition of the film product were characterized. Two Ti₃SiC₂ layers form the whole film, where the Ti₃SiC₂ grains have different features. The synthesis mechanism has been discussed from the thickness of PyC and the batching ratio of mixed powder respectively. Finally, the obtained Ti₃SiC₂ film was utilized as interphase to prepare the SiC fibre reinforced SiC matrix composites (SiC_f/Ti₃SiC₂/SiC composites). The flexural strength (σ_F) and fracture toughness (K_IC) of the SiC_f/Ti₃SiC₂/SiC composite is 460 ± 20 MPa and 16.8 ± 2.4 MPa?m^1/2 respectively.     

Synthesis of Ti3SiC2 coatings onto SiC monoliths from molten salts

Coatings with composition close to Ti₃SiC₂ were obtained on SiC substrates from Ti and Si powders with the molten NaCl method. In this work, the growth of coatings by reaction in the salt between monolithic SiC substrates and titanium powder is obtained between 1000 and 1200 °C. At 1000 °C, a coating of 8 µm thickness is formed in 10 h whereas a thin coating of 0.5 µm has been grown in 2 h. A lack in silicon was first found in the coatings prepared at 1100 and 1200 °C. For these temperatures, the addition of silicon powder in the melt had a favorable effect on the final composition, which is found very close to the composition of Ti₃SiC₂. The reaction mechanism implies the formation of TiC_x layers in direct contact with the SiC substrate and the presence of more or less important quantities of Ti₃SiC₂ and Ti₅Si₃C_x in the upper layers.     

Compressive creep of SiC whisker/Ti3SiC2 composites at high temperature in air

The compressive creep of a SiC whisker (SiC_w) reinforced Ti₃SiC₂ MAX phase-based ceramic matrix composites (CMCs) was studied in the temperature range 1100-1300°C in air for a stress range 20-120 MPa. Ti₃SiC₂ containing 0, 10, and 20 vol% of SiC_w was sintered by spark plasma sintering (SPS) for subsequent creep tests. The creep rate of Ti₃SiC₂ decreased by around two orders of magnitude with every additional 10 vol% of SiC_w. The main creep mechanisms of monolithic Ti₃SiC₂ and the 10% CMCs appeared to be the same, whereas for the 20% material, a different mechanism is indicated by changes in stress exponents. The creep rates of 20% composites tend to converge to that of 10% at higher stress. Viscoplastic and viscoelastic creep is believed to be the deformation mechanism for the CMCs, whereas monolithic Ti₃SiC₂ might have undergone only dislocation-based deformation. The rate controlling creep is believed to be dislocation based for all the materials which is also supported by similar activation energies in the range 650-700 kJ/mol.     

The thermal,electrical and mechanical properties of porous α-SiC ceramics bonded with Ti3SiC2 and β-SiC via low temperature in-situ reaction sintering

Porous SiC ceramics have recently attracted wide attention for their applications in the electrically heatable filter. Further improvement of the thermal and electrical conductivity without sacrificing permeability is a critical parameter for such applications. In the present work, porous SiC/Ti₃SiC₂ ceramic composites with Ti₃SiC₂ and micro/nano SiC have been prepared from TiC/Si/α-SiC mixtures at a low sintering temperature (1400 °C). Nano-laminated Ti₃SiC₂ enhanced the electrical conductivity, while the good thermal conductivity was achieved through in-situ formed nano β-SiC and raw coarse α-SiC in the porous ceramics. Along with the increase of initial α-SiC particle size from 0.76 to 16.13 μm, the permeability, thermal and electrical conductivity improved due to the decreased porosity and increased pore size in porous SiC/Ti₃SiC₂ ceramics. The results suggested that the decoupling of the electrical conductivity from the thermal conductivity could be tuned by adjusting the initial α-SiC particle size.     

Improvement for Ti3SiC2/Cu joint brazed using composite fillers with abnormal expansion ceramic particulates

Reducing the residual stresses and improving the mechanical strength of large-scale ceramic/metal brazing joints is an important problem that must be solved for its practical engineering application. Using composite filler with solid-state phase transformation ceramic particulates, it is theoretically feasible to relieve the residual stress and improve the mechanical properties of ceramic/metal brazed joints. In this study, Cu mesh, Ag–28Cu–2Ti (wt.%), and yttria-stabilized zirconia (0.6 mol.% YSZ solid-state phase transformation ceramic particulates) composite power fillers were used in the brazing of Ti₃SiC₂ ceramic and pure copper. The microstructure of joints and YSZ particulates in the interface was investigated and confirmed by scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), scanning transmission electron microscopy (STEM), and transmission electron microscopy (TEM). In addition, the effect of YSZ particulates content on the mechanical properties of joints was investigated and evaluated by the shear strength. The results show that the interfacial phases were mainly Ti₅Si₃, TiC, Ti_xCu, Ag (s, s), Cu (s, s), and YSZ particulates. Moreover, most of YSZ particulates undergo the solid-state phase transformation from tetragonal zirconia (t-ZrO₂) to monoclinic zirconia (m-ZrO₂) during the cooling process of brazing. The abnormal volume expansion of the solid-state phase transformation reduced the thermal mismatch between Ti₃SiC₂ ceramic and filler, thereby reducing the residual stress in the interface of joint. When using composite filler with 6 wt.% YSZ particulates, the shear strength of Ti₃SiC₂/Cu joint reached the maximum. The maximum average shear strength of the joints was 80.2 MPa, which was about 103.6% more than the joint without YSZ particulates.