Microstructure and oxidation of multi-layer MoSi2-CrSi2-Si coatings for SiC coated carbon/carbon composites

Multi-layer MoSi₂-CrSi₂-Si anti-oxidation coatings with different compositional ratios were prepared on the surface of SiC coated carbon/carbon (C/C) composites by a two-step pack cementation method. The microstructure and anti-oxidation performance of the coating were studied. The results show that the multi-layered coatings could protect the C/C composites from oxidation in air at 1773 K for 1000 h or 1873 K for 750 h, respectively. The anti-oxidation performance of the multi-layer MoSi₂-CrSi₂-Si coating is mainly attributed to their dense and microcrack-free structure, appropriate thermal expansion coefficient and the well dispersed MoSi₂ and CrSi₂ in the coating.     

Thermal fatigue behavior of C/C composites modified by SiC-MoSi2-CrSi2 coating

Carbon/carbon (C/C) composites were modified by SiC-MoSi₂-CrSi₂ multiphase coating by pack cementation, and their thermal fatigue behavior under thermal cycling in Ar and air environments was investigated. The modified C/C composites were characterized by scanning electron microscopy and X-ray diffraction. Results of tests show that, after 20-time thermal cycles between 1773 K and room temperature in Ar environment, the flexural strength of modified C/C samples decreased lightly and the percentage of remaining strength was 94.92%. While, after thermal cycling between 1773 K and room temperature in air for 20 times, the weight loss of modified C/C samples was 5.1%, and the flexural strength of the modified C/C samples reduced obviously and the percentage of remaining strength was only 75.22%. The fracture mode of modified C/C samples changed from a brittle behavior to a pseudo-plastic one as the service environment transformed from Ar to air. The decrease of the flexural strength during thermal cycle in air was primarily attributed to the partial oxidation of modified C/C samples.     

A ZrSiO4/SiC oxidation protective coating for carbon/carbon composites

In order to improve the oxidation resistance of carbon/carbon (C/C) composites, a ZrSiO₄ coating on SiC pre-coated C/C composites was prepared by a hydrothermal electrophoretic deposition process. Phase compositions and microstructures of the as-prepared ZrSiO₄/SiC coating were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy dispersive spectrometer (EDS). The anti-oxidation property and failure mechanism of the multi-layer coating were investigated. Results show that hydrothermal electrophoretic deposition is an effective route to prepare crack-free ZrSiO₄ outer coatings. The multi-layer coating obviously exhibits two-layer structure. The inner layer is composed of SiC phase and the outer layer is composed of ZrSiO₄ phase. The bonding strength between the outer layer coatings and C/C–SiC substrate are 30.38 MPa. The ZrSiO₄/SiC coating displays excellent oxidation resistance and can protect C/C composites from oxidation at 1773 K for 332 h with a mass loss rate of only 0.48 × 10^− 4 g/cm²·h. The mechanical properties of the specimens are 84.36 MPa before oxidation and 68.29 MPa after oxidation. The corresponding high temperature oxidation activation energy of the coated C/C composites at 1573–1773 K is calculated to be 119.8 kJ/mol. The oxidation process is predominantly controlled by the diffusion rate of oxygen through the ZrSiO₄/SiC multi-coating. The failure of the coating is due to the formation of penetrative holes between the SiC bonding layer and the C/C matrix at 1773 K.     

SiC nanowire-toughened MoSi2-SiC coating to protect carbon/carbon composites against oxidation

To protect carbon/carbon (C/C) composites against oxidation, a SiC nanowire-toughened MoSi₂-SiC coating was prepared on them using a two-step technique of chemical vapor deposition and pack cementation. SiC nanowires obtained by chemical vapor deposition were distributed random-orientedly on C/C substrates and MoSi₂-SiC was filled in the holes of SiC nanowire layer to form a dense coating. After introduction of SiC nanowires, the size of the cracks in MoSi₂-SiC coating decreased from 18 ± 2.3 to 6 ± 1.7 μm, and the weight loss of the coated C/C samples decreased from 4.53% to 1.78% after oxidation in air at 1500 °C for 110 h.     

Si-W-Mo coating for SiC coated carbon/carbon composites against oxidation

In order to prevent carbon/carbon (C/C) composites from oxidation at 1773 K, a Si-W-Mo coating was prepared on the surface of SiC coated C/C composites by a simple pack cementation technique. The microstructures and phase composition of the as-received multi-coating were examined by SEM, XRD and EDS. It was seen that the compact multi-coating was composed of α-SiC, Si and (W_xMo_1 − x)Si_2. Oxidation behaviour of the SiC/Si-W-Mo coated C/C composites was also studied. After 315 h oxidation in air at 1773 K and thermal cycling between 1773 K and room temperature for 17times, no weight loss of the as-coated C/C composites was measured. The excellent anti-oxidation ability of the multi-coating is attributed to its dense structure and the formation of the stable glassy SiO₂ film on the coating surface during oxidation.     

A MoSi2/SiC oxidation protective coating for carbon/carbon composites

To protect carbon/carbon (C/C) composites against oxidation, a MoSi₂ outer coating was prepared on pack-cementation SiC coated C/C composites by a hydrothermal electrophoretic deposition. The phase composition, microstructure and oxidation resistance of the prepared MoSi₂/SiC coatings were investigated. Results show that hydrothermal electrophoretic deposition is an effective route to achieve crack-free MoSi₂ outer coatings. The MoSi₂/SiC coating can protect C/C composites from oxidation at 1773 K for 346 h with a weight loss of 2.49 mg cm⁻² and at 1903 K for 88 h with a weight loss of 5.68 mg cm⁻².     

Microstructure and anti-oxidation property of Si-W-Cr coating for SiC coated carbon-carbon composites

To protect carbon/carbon (C/C) composites from oxidation at high temperature, a Si-W-Cr coating was prepared on the surface of SiC coated C/C composites by a simple pack cementation technique. The microstructure and phase composition of the as-received multi-coating were examined by SEM, XRD and EDS. The coating obtained by first step pack cementation was porous α-SiC structure. New phases of WSi₂ and CrSi₂ together with α-SiC deposited on the porous SiC inner layer. Oxidation test shows that the weight loss of single SiC coated C/C is up to 8.21% after 9 h in air at 1773 K, while the weight loss of Si-W-Cr/SiC coated C/C composites is only 2.26% after 51 h. After thermal cycling between 1773 K and room temperature for 40 times, the weight loss is only 3.36%. The weight loss of coated C/C composites was primarily due to the reaction of C/C matrix and oxygen diffusing through the penetrable cracks in the coating.     

A MoSi2-SiC-Si oxidation protective coating for carbon/carbon composites

To protect carbon/carbon (C/C) composites from oxidation, a dense coating has been produced by a two-step pack cementation technique. XRD and SEM analysis shows that the as-obtained coating was composed of MoSi₂, SiC and Si with a thickness of 80-100 μm. The MoSi₂-SiC-Si coating has excellent anti-oxidation property, which can protect C/C composites from oxidation at 1773 K in air for 200 h and the corresponding weight loss is only 1.04%. The weight loss of the coated C/C composites is primarily due to the reaction of C/C substrate and oxygen diffusing through the penetration cracks in the coating.     

C/SiC/MoSi2–Si multilayer coatings for carbon/carbon composites for protection against oxidation

To improve the oxidation resistance of carbon/carbon (C/C) composites, a C/SiC/MoSi₂–Si multilayer oxidation protective coating was prepared by slurry and pack cementation. The microstructure of the as-prepared coating was characterized by scanning electron microscopy, X-ray diffraction and energy dispersive spectroscopy. The isothermal oxidation and erosion resistance of the coating was investigated in electrical furnace and high temperature wind tunnel. The results showed that the multilayer coating could effectively protect C/C composites from oxidation in air for 300 h at 1773 K and 103 h at 1873 K, and the coated samples was fractured after erosion for 27 h at 1873 K h in wind tunnel. The weight loss of the coated specimens was considered to be caused by the formation of penetration cracks in the coating. The fracture of the coated C/C composites might result from the excessive local stress in the coating.     

Multilayer oxidation protective coating for C/C composites from room temperature to 1500 °C

To prevent carbon/carbon (C/C) composites from oxidation, a multilayer oxidation resistant coating was prepared. The inner SiC coating was prepared by pack cementation, and the outer SiC-MoSi₂ three-layer coating was obtained by slurry coating using silicon-sol as the caking agent. X-ray diffraction, scanning electron microscopy and energy dispersive X-ray spectroscopy were used to analyze the phase, microstructure and element distribution of the as-prepared coating. The results show that, the as-received multilayer coating has a crack-free structure with the thickness of about 300 μm. It is provided with excellent oxidation resistance from room temperature to 1500 °C in air and can protect C/C composites from oxidation for more than 120 h at 900 °C and more than 110 h at 1500 °C in air. The weight loss of the coated samples during oxidation tests mainly resulted from the oxidation of Mo₅Si₃ and the volatilization of SiO₂ in the coating.     

SiC/SiC–YAG–YSZ oxidation protective coatings for carbon/carbon composites

SiC/SiC–YAG–YSZ coatings were prepared by pack cementation, chemical vapor deposition and slurry painting on carbon/carbon (C/C) composites. The microstructures and oxidation behavior of coatings were investigated. The results show that the coatings displayed good oxidation and thermal shock resistance due to a dense glassy layer with silicates formed on the coating of SiC–YAG–YSZ. The weight gain rate of coated C/C composites was 1.77% after oxidation for 150 h at 1773 K. SiC in outer coating can promote the formation of oxygen diffusion barrier and lead to the optimum oxidation resistance for the coatings, compared with YSZ and YAG.     

ZrO2–SiO2 gradient multilayer oxidation protective coating for SiC coated carbon/carbon composites

In order to eliminate the mismatch of thermal expansion coefficient between the ZrO₂ outer layer and the internal bonding SiC layer, ZrO₂–SiO₂ composition-gradient transition layers were prepared by a sol–gel technique using tetraethoxysilane (TEOS) and zirconyl chloride as source materials. Energy dispersive spectroscopy (EDS) analysis displays that the gradient composition ZrO₂–SiO₂ outer coating could be obtained by immersing the SiC precoated carbon/carbon (C/C) composites into the gradient composition zirconia-silica sols (ZS sol) in turn. Oxidation test shows that, after 10 h oxidation in air at 1773 K, the weight loss of the gradient ZrO₂–SiO₂ coating coated SiC-C/C is only 1.97%.     

B2O3 modified SiC–MoSi2 oxidation resistant coating for carbon/carbon composites by a two-step pack cementation

To protect carbon/carbon (C/C) composites against oxidation, a B₂O₃ modified SiC–MoSi₂ coating was prepared by a two-step pack cementation. The microstructure and the oxidation resistant property of the coating were studied. The results show that, the as-received coating is a dense structure, and is composed of α-SiC, β-SiC and MoSi₂. The B₂O₃ modified SiC–MoSi₂ coating has excellent oxidation resistant property, and can protect C/C composites from oxidation at 1773 K in air for more than 242 h. The failure of the coating was considered to arise from the existence of the penetration cracks in the coating during the slow cooling from 1873 to 673 K.     

Anti-oxidation properties of ZrB2 modified silicon-based multilayer coating for carbon/carbon composites at high temperatures

To improve the anti-oxidation ability of silicon-based coating for carbon/carbon (C/C) composites at high temperatures, a ZrB₂ modified silicon-based multilayer oxidation protective coating was prepared by pack cementation. The phase composition, microstructure and oxidation resistance at 1773, 1873 and 1953 K in air were investigated. The prepared coating exhibits dense structure and good oxidation protective ability. Due to the formation of stable ZrSiO₄–SiO₂ compound, the coating can effectively protect C/C composites from oxidation at 1773 K for more than 550 h. The anti-oxidation performance decreases with the increase of oxidation temperature. The mass loss of coated sample is 2.44% after oxidation at 1953 K for 50 h, which is attributed to the decomposition of ZrSiO₄ and the volatilization of SiO₂ protection layer.     

ZrSiO4 Oxidation Protective Coating for SiC-Coated Carbon/Carbon Composites Prepared by Supersonic Plasma Spraying

To protect carbon/carbon (C/C) composites against oxidation, ZrSiO₄ oxidation protective coating was prepared on SiC-coated C/C composites by supersonic plasma spraying. X-ray diffraction and scanning electron microscopy were used to analyze the phase and microstructure of the coating. The results show that the as-prepared ZrSiO₄ coating is continuous and well bonded with the SiC inner layer without penetrating crack, which exhibits good oxidation-resistant properties. After oxidation at 1773 K in air for 97 h and nine thermal shock cycles between 1773 K and room temperature, the weight loss of the coated C/C composites was only 0.08%. The excellent oxidation-resistant properties of the coating were attributed to its dense structure and the formation of the stable ZrO₂-SiO₂ glassy mixture on the surface of ZrSiO₄ coating.     

Preparation and oxidation protection of CVD SiC/a-BC/SiC coatings for 3D C/SiC composites

An amorphous boron carbide (a-BC) coating was prepared by LPCVD process from BCl₃-CH₄-H₂-Ar system. XPS result showed that the boron concentration was 15.0 at.%, and carbon was 82.0 at.%. One third of boron was distributed to a bonding with carbon and 37.0 at.% was dissolved in graphite lattice. A multiple-layered structure of CVD SiC/a-BC/SiC was coated on 3D C/SiC composites. Oxidation tests were conducted at 700, 1000, and 1200 °C in 14 vol.% H₂O/8 vol.% O₂/78 vol.% Ar atmosphere up to 100 h. The 3D C/SiC composites with the modified coating system had a good oxidation resistance. This resulted in the high strength retained ratio of the composites even after the oxidation.     

Mullite-gadolinium silicate environmental barrier coatings for melt infiltrated SiC/SiC composites

Slurry based mullite/gadolinium silicate (Gd₂SiO₅) environmental barrier coatings (EBCs) were developed for melt infiltrated (MI) SiC/SiC composites. The coating chemically adhered well on the substrates. Thermal cycling of uncoated MI-SiC/SiC composites conducted between 1350 °C and 90 °C (one hour hot and 15 min cold) in a 96.5% H₂O-3.5% O₂ environment caused severe oxidation damage after 100 cycles resulting in the formation of dense silica layer of about 25 μm maximum thickness. Mullite/Gd₂SiO₅ EBCs provided excellent protection to MI-SiC/SiC against moisture damage with significantly less oxidation of the substrate; only about a 2 μm thick oxide layer formed even after 400 similar thermal cycles. The hair-line cracks formed at the coating/substrate interface after 400 cycles causing partial coating de-lamination.     

The oxidation behavior and mechanical properties of MoSi2–CrSi2–SiC–Si coated carbon/carbon composites in high-temperature oxidizing atmosphere

A MoSi₂–CrSi₂–SiC–Si multi-component coating was prepared on the surface of carbon/carbon (C/C) composites by a two-step pack cementation method. The microstructure, oxidation behavior and mechanical properties of the coating were studied. These results show that the multi-component coating could protect the C/C composites from oxidation in air at 1873 K for 300 h and withstand 30 thermal cycles between 1873 K and room temperature, respectively. The mass loss and mechanical property loss of the coated C/C composites are considered due to the worse fluidity of SiO₂ at intermediate temperatures and the thermal mismatch between the coating and C/C composites.     

HfB2/SiC as a protective coating for 2D Cf/SiC composites: Effect of high temperature oxidation on mechanical properties

In the field of thermal shielding for aerospace applications C_f/SiC composites are raising great interest, provided that they are protected from oxidation by suitable coatings. Conversely, ultra high temperature ceramics, and in particular HfB₂, are among the best oxidation resistant materials known. A coating made of a HfB₂/SiC composite (20% weight SiC) was tested as an oxidation protection on a C_f/SiC composite. The composite was produced by Polymer Impregnation Pyrolysis (PIP), which is a simple and low cost method; the coating was applied by painting a slurry on the surface of the composite and by heat treating. The thermal behaviour was studied by thermo-gravimetric analysis, and mechanical tests were conducted before and after oxidation. The HfB₂/SiC composite seems to effectively protect the underlying C_f/SiC composite, with a mechanical strength reduction of only 20% after 30 min at 1600 °C, even if some weight loss due to partial carbon fibre damage is observed. A first analysis of thermal cycling in oxidizing environment suggested that the HfB₂/SiC coating reduces continual damage thanks to the sealing effect of the glassy surface layer.     

Investigation on the Electrical Properties of Vacuum Cold Sprayed SiC-MoSi2 Coatings at Elevated Temperatures

SiC-MoSi₂ composite powders was prepared by wet milling with MoSi₂ powders and SiC loose grinding ball in alcohol solution. Vacuum cold spray (VCS) process was used to deposit SiC-MoSi₂ electric conducting composite coatings. The microstructure of the VCS SiC-MoSi₂ composite coatings were characterized by scanning electron microscopy. The electrical resistance of the coatings was measured using a four-point probe method. The effects of the deposition parameters on the electrical resistivity of the composite coatings were investigated. The electrical properties of the coatings at elevated temperatures in air and Ar gas atmospheres were also explored. The results show that the electrical resistivity of SiC-MoSi₂ coatings decreases with increasing He gas flow rates ranged from 3 to 6 L/min. The electrical resistivity increases with the increase in heat treatment temperature due to “pesting” behavior of MoSi_2. The electric conductive property of the VCS SiC-MoSi₂ coating is significantly improved after heat treatment at 1000 °C for 3 h in Ar protective atmosphere without oxidation. A minimum resistivity of the heat treated coating is 0.16 Ω · cm.