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1.
    
The barium strontium aluminosilicate and Y2Si2O7‐BSAS‐coated C/SiC composites were corroded in 50%H2O–50%O2 environments at 1250°C, respectively. It was found that the coated composites suddenly lost their strength as the corrosion time was up to 250 and 750 h, respectively. During the water vapor corrosion, a continuous silica scale was formed between the SiC bond coat and environmental barrier coatings, leading to the growth stress. The thickness of silica scale grew with the prolonged corrosion time, accompanied with the accumulation of growth stress in the silica scale. When the growth stress was greater than the bond strength between silica scale and SiC bond coat, the cracks would form and propagate along their interface, resulting in the spallation of EBCs, followed by the failure of the composites.  相似文献   

2.
    
The calcium rare-earth (RE) silicate oxyapatite, Ca2RE8(SiO4)6O2 (RE = Yb, Er, Y, Dy, Nd, Gd, and Sm), powders were synthesized by the solid-state reaction method and characterized by X-ray diffraction (XRD), Raman spectroscopy, and elemental composition analysis. The thermodynamic properties of the oxyapatites have been investigated using high-temperature oxide melt calorimetry in molten 2PbO–B2O3 solvent at 805°C. The energetics of the oxyapatites related to ionic substitution on two crystallographic sites, M(1) and M(2), are discussed. The enthalpy of formation from the oxides becomes more exothermic as the ionic potential decreases or the ionic radius of the REs increases, which indicates increasing energetic stability in this order.  相似文献   

3.
    
Rare earth (RE) disilicates are utilized in environmental barrier coatings to protect Si-based engine components from destructive reactions with water vapor and other combustion species. These coating materials, however, degrade when exposed to molten silicate deposits in the engine. Four RE-disilicates (RE2Si2O7, RE = Er, Dy, Gd, Nd) are analyzed herein in thermochemical interactions with glassy calcium-magnesium-aluminosilicate (CMAS) compositions at 1400°C. Crystalline reaction products included RE2Si2O7, SiO2, and a Ca2+yRE8+x(SiO4)6O2+3x/2+y apatite-type silicate. RE2Si2O7 formation was favored in interactions with CMAS having low CaO:SiO2 ratios. Increased reactivity was observed for higher CaO:SiO2 ratios in CMAS combined with larger RE3+ cation size, resulting in apatite formation of varying stoichiometry and changes in lattice parameters. The crystallization of SiO2 was dependent on both thermodynamic equilibrium at low CaO:SiO2 ratios and sequestration of silicate modifiers at higher CaO:SiO2 ratios, although residual amorphous content after CMAS exposure in both cases was still substantial.  相似文献   

4.
    
Rare earth silicates are promising environmental/thermal barrier coating (E/TBC) materials facing severe CMAS (CaO-MgO-Al2O3-SiO2) corrosion. Previous studies mainly focused on the intrinsic properties of precorrosion coatings, but there were few studies on their CMAS corrosion products that play a crucial role in the performance of coatings in postservice stage. In this work, the mechanical and thermal properties of nine corrosion products between lutetium silicates and CMAS are studied using first-principles calculations. Their differences of elastic stiffness are attributed to the different crystal structures and bonding strength. The T:O ratio is identified as a factor of the crystal structure for silicate products, and it has a good correlation with their elastic stiffness. Moreover, the divergences of thermal conductivity are dominated by three essential factors, that is, atomic vibration intensity, lattice vibrational anharmonicity, and complexity of crystal structure. Compared with rare earth silicates, six products, that is, the α-CaSiO3, β-CaSiO3, Ca2MgSi2O7, Ca2Al2SiO7, CaAl2Si2O8, and Ca2Lu8(SiO4)6O2, showing good damage tolerance and low thermal conductivities, are predicted to be advantageous to E/TBCs. These discoveries reveal the mechanical/thermal properties of corrosion products between lutetium silicates and CMAS and are expected to support the future researches on the performance of E/TBC in the postservice stage.  相似文献   

5.
    
The growth of thermally grown oxide (TGO) layers in thermal barrier coatings (TBCs) due to the oxidation of the bondcoat alloy is a critical factor affecting the durability of TBCs. In the present study, diverse TBC specimens were subjected to long-term oxidation at various temperatures. The TGO growth mechanism was investigated according to cross-sectional images of the oxidized specimens. Impedance spectroscopy (IS) was performed to measure the electrical properties of the integrated TBCs non-destructively. Considering the influence of the TGO composition, the derived TGO electrical capacitance was found to have a good correspondence to the observed TGO thickness over a wide range 0–18.3 μm, regardless of the diverse specimens and oxidation conditions. The error was less than ±2.0 μm. With a certain design of the electrode size, IS is generalized and is recommended as an accurate and practical non-destructive evaluation method for the determination of TGO thickness within a very wide range in TBC systems under real operating conditions.  相似文献   

6.
    
Rare earth silicate environmental barrier coatings (EBCs) are state of the art for protecting SiC ceramic matrix composites (CMCs) against corrosive media. The interaction of four pure rare earth silicate EBC materials Yb2SiO5, Yb2Si2O7, Y2SiO5, Y2Si2O7 and three ytterbium silicate mixtures with molten calcium-magnesium-aluminosilicate (CMAS) were studied at high temperature (1400°C). The samples were characterized by SEM and XRD in order to evaluate the recession of the different materials after a reaction time of 8 hours. Additionally, the coefficient of thermal expansion (CTE) was determined to evaluate the suitability of Yb silicate mixtures as EBC materials for SiC CMCs. Results show that monosilicates exhibit a lower recession in contact with CMAS than their disilicate counterparts. The recession of the ytterbium silicates is far lower than the recession of the yttrium silicates under CMAS attack. Investigation of the ytterbium silicate mixtures exposes their superior resistance to CMAS, which is even higher than the resistance of the pure monosilicate. Also their decreased CTE suggests they will display better performance than the pure monosilicate.  相似文献   

7.
Calcia-magnesia-aluminosilicate (CMAS) corrosion behaviors of hot-pressed (Y1-xYbx)2SiO5 ceramics at 1673 K and 1773 K have been investigated. The main corrosion product of nonstoichiometric Ca-RE-Si-O apatite phase evolves with increasing temperature or prolonging corrosion time. The growth of apatite layer at 1673 K follows approximately a linear rate law, however it follows a proximately parabolic rate law at 1773 K. The growth rate of the apatite layer at 1773 K is lower than that at 1673 K in the process of interaction between CMAS and rare-earth monosilicates. Yb-doping mediates the CMAS corrosion resistance of Y2SiO5 effectively by changing the growth rate of apatite layer and the composition of formed apatite phase. This work provides new insights on compositional regulation of (Y1-xYbx)2SiO5 EBCs materials to resist CMAS corrosion.  相似文献   

8.
    
The oxygen permeability of ytterbium disilicate (YbDS) topcoat (TC) and silicon dioxide (SiO2) thermally grown oxide (TGO) is evaluated. The primary goal is to elucidate the oxidation mechanisms in environmental barrier coatings (EBCs). For this purpose, oxidant diffusion is investigated using physics-based and numerical modeling. The oxygen permeability constants are systematically evaluated and quantified in terms of thermodynamics using defect reactions and the parabolic rate constant (kp), respectively. Dry oxygen and wet oxygen conditions as well as different temperatures, partial pressures, and topcoat modifiers are investigated. The results offer evidence that the oxygen permeability constant for the YbDS topcoat is an order of magnitude higher than for the TGO. As such, the TGO hinders the oxidant diffusion stronger, proving to be the diffusion rate-controlling layer. Moreover, water vapor strongly increases the oxidant permeation with defect reactions playing a key role. It is suggested that the mass transfer through the topcoat is primarily by outward ytterbium ion diffusion and inward oxygen ion movement, with the latter being dominant, particularly in wet environments. The effect of topcoat modifiers on oxidant permeation is composition sensitive and seems to be related to their interaction with oxygen ions and their mobility.  相似文献   

9.
    
《Ceramics International》2022,48(7):9313-9323
Thermal environmental barrier coatings (TEBCs) are capable of protecting ceramic matrix composites (CMCs) from hot gas and steam. In this paper, a tri-layer TEBC consisting of 16 mol% YO1.5 stabilized HfO2 (YSH16) as thermal barrier coating, ytterbium monosilicate (YbMS) as environmental barrier coating, and silicon as the bond coating was designed. Microstructure evolution, interface stability, and oxidation behavior of the tri-layer TEBC at 1300 °C were studied. The as-sprayed YSH16 coating was mainly comprised of cubic phase and ~3.4 vol% of monoclinic (M) phase. After 100 h of heat exposure, the volume fraction of the M phase increased to ~27%. The YSH16/YbMS interface was proved to be very stable because only slight diffusion of Yb to YSH16 was observed even after thermal exposure at 1300 °C for 100 h. At the YbMS/Si interface, a reaction zone including a Yb2Si2O7 layer and a SiO2 layer was generated. The SiO2 grew at a rate of ~0.039 μm2/h in the first 10 h and a reduced rate of 0.014 μm2/h in the subsequent exposure.  相似文献   

10.
    
Suspensions of ytterbium disilicate in isopropanol were prepared using iodine dispersant. Their zeta potential, electrical conductivity, and pH dependence with iodine concentration is detailed. Electrophoretic deposition was performed on silicon substrates at various voltages (100-200 V) and times (until 10 minutes) and the growth dynamic was investigated. It was observed that the deposited mass reaches a maximum value for [I2] = 0.2 g/L, and the coating microstructure becomes porous at higher iodine concentrations. Current density and voltage measurements allowed to correlate this behavior to the increase of free protons concentration in the suspension. In these conditions, it was proved that porosity increases with the increase in applied voltage, and a compaction occurs as the deposition time increases. This has been related to the coating resistance increase and subsequent decrease in effective voltage in the suspension. The denser coatings (20% of porosity) were obtained in the case of suspension without iodine, at the minimum applied voltage and for the longest deposition times.  相似文献   

11.
  总被引:1,自引:0,他引:1  
《Ceramics International》2020,46(2):1532-1544
The failure of plasma-sprayed thermal barrier coating (TBC) is often caused by the coating spallation due to crack propagation. In this study, a new model with stacking lamellae is developed based on the cross-section micrograph to explore crack propagation behavior within the ceramic top coat (TC) during isothermal cycling. The dynamic growth process of thermally grown oxide (TGO) is simulated via material properties change step by step. The stress profiles in the lamellar model are first evaluated, and the pore and lamellar interface crack effects on the stress state are further explored. Then, the successive crack growth, linkage, and ultimate coating spallation process is simulated. The results show that the stress intensity in TC enhances with thermal cycling. Large stress concentration always occurs near the pore and lamellar interface crack, which can result in the incipient crack growth. Moreover, the lamellar interface crack also changes the stress distribution within the TC and at the TC/bond coat interface. The multiple crack propagation upon temperature cycling is explored, and the possible coalescence mechanism is proposed. The lamellar crack steadily propagates at the early stage. The crack length sharply increases before the occurrence of coating spallation. The simulated coat spalling path is in line with the experimental result. Therefore, the new lamellar model developed in this work is beneficial to further reveal coating failure mechanism and predict coating lifetime.  相似文献   

12.
13.
    
The current generation of multilayer Si/Yb2Si2O7 environmental barrier coatings (EBCs) are temperature limited by the melting point of Si, 1414°C. To investigate higher temperature EBCs, the cyclic steam oxidation of EBCs comprised of a single layer of ytterbium disilicate (YbDS) was compared to multilayered Si/YbDS EBCs, both deposited on SiC substrates using atmospheric plasma spray. After 500 1-h cycles at 1300°C in 90 vol%H2O-10 vol%air with a gas velocity of 1.5 cm/s, both multilayer Si/YbDS and single layer YbDS grew thinner silica scales than bare SiC, with the single layer YbDS forming the thinnest scale. Both coatings remained fully adherent and showed no signs of delamination. Silica scales formed on the single layer coating were significantly more homogeneous and possessed a markedly lower degree of cracking compared to the multilayered EBC. The single layer EBC also was exposed at 1425°C in steam with a gas velocity of 14 cm/s in an alumina reaction tube. The EBC reduced specimen mass loss compared to bare SiC but formed an extensive 2nd phase aluminosilicate reaction product. A similar reaction product was observed to form on some regions of the bare SiC specimen and appeared to partially inhibit silica volatilization. The 1425°C steam exposures were repeated with a SiC reaction tube and no 2nd phase reaction product was observed to form on the single layer EBC or bare SiC.  相似文献   

14.
    
A primary failure mode for environmental barrier coatings (EBCs) on SiC ceramic matrix composites (CMCs) is the oxidation of the intermediate Si-bond coating, where the formation of SiO2 at the bond coating–EBC interface results in debonding and spallation. This work compares the microstructure evolution and steam oxidation kinetics of the Si-bond coating beneath yttrium/ytterbium disilicate ((Y/Yb)DS) and ytterbium disilicate/monosilicate (YbDS/YbMS) EBCs to better understand the impact of EBC composition on oxidation kinetics. After 500 1-h cycles at 1350°C, (Y/Yb)DS displayed a decreasing concentration of the monosilicate minor phase and increasing concentration of porosity as furnace cycling time increased, whereas the YbDS/YbMS EBC displayed negligible microstructural evolution. For both EBC systems, thermally grown oxide growth rates in steam were found to increase by approximately an order magnitude compared to dry air oxidation. The (Y/Yb)DS EBC displayed a reduced steam oxidation rate compared to YbDS/YbMS.  相似文献   

15.
The impact of calcium–magnesium–alumino-silicate (CMAS) degradation is a critical factor for development of new thermal and environmental barrier coatings. Several methods of preventing damage have been explored in the literature, with formation of an infiltration inhibiting reaction layer generally given the most attention. Gd2Zr2O7 (GZO) exemplifies this reaction with the rapid precipitation of apatite when in contact with CMAS. The present study compares the CMAS behavior of GZO to an alternative thermal barrier coating (TBC) material, GdAlO3 (GAP), which possesses high temperature phase stability through its melting point as well as a significantly higher toughness compared with GZO. The UCSB laboratory CMAS (35CaO–10MgO–7Al2O3–48SiO2) was utilized to explore equilibrium behavior with 50:50 mol% TBC:CMAS ratios at 1200, 1300, and 1400°C for various times. In addition, 8 and 35 mg/cm2 CMAS surface exposures were performed at 1425°C on dense pellets of each material to evaluate the infiltration and reaction in a more dynamic test. In the equilibrium tests, it was found that GAP appears to dissolve slower than GZO while producing an equivalent or higher amount of pore blocking apatite. In addition, GAP induces the intrinsic crystallization of the CMAS into a gehlenite phase, due in part to the participation of the Al2O3 from GAP. In surface exposures, GAP experienced a substantially thinner reaction zone compared with GZO after 10 h (87 ± 10 vs. 138 ± 4 μm) and a lack of strong sensitivity to CMAS loading when tested at 35 mg/cm2 after 10 h (85 ± 13 versus 246 ± 10 μm). The smaller reaction zone, loading agnostic behavior, and intrinsic crystallization of the glass suggest this material warrants further evaluation as a potential CMAS barrier and inclusion into composite TBCs.  相似文献   

16.
    
A protocol for selecting representative silicate compositions for comparative testing of gas turbine coating materials is presented. It begins with a curated dataset of compositions of engine deposits and naturally occurring siliceous debris including volcanic ashes, sands, and dusts. The compositions are first reduced to the five major oxides—those of Ca, Mg, Fe, Al, and Si—and then distilled further using principal component analysis and k-means clustering. The process ultimately yields four classes of possible deposits with common chemical characteristics. Each class is represented by a composition centroid and a range in Ca:Si ratios. Key thermophysical properties of the possible deposits are calculated and related to the glass network connectivity, characterized by the Si:O ratio. Finally, deposits from each of these classes are compared in terms of their reactions with prototypical thermal and environmental barrier oxides, with due consideration of the effects of composition variations within each deposit class. The protocol is, in principle, adaptable to datasets compiled by OEMs and researchers in gas turbine coatings.  相似文献   

17.
    
The thermochemical stability of Y2Si2O7 was assessed in a high-temperature high-velocity water vapor environment to improve the understanding of the mechanisms that lead to SiO2 depletion. Spark plasma sintered Y2Si2O7 specimens were exposed in a steam-jet furnace at 1000°C and 1200°C for 3-250 hours, steam velocities of 131-174 m/s and at 1 atm H2O pressure. These exposures resulted in the selective volatilization of SiO2 to form volatile Si(OH)4 and porous Y2SiO5. Microstructural evolution from fine rectangular pores at short times to larger rounded pores at longer times was observed. Mechanisms contributing to the overall depletion reaction kinetics were evaluated and include the interface reaction to form Y2SiO5 and Si(OH)4 (g), Y2SiO5 coarsening, development of tortuosity in the pore network and diffusion of H2O (g) and Si(OH)4 (g) through pores by molecular diffusion and/or Knudsen diffusion. SiO2 depletion was found to follow parabolic volatilization kinetics (kp = 0.38 µm2/h) at 1200°C indicating the reaction is limited by a diffusion process, most likely the outward diffusion of Si(OH)4 (g) through pores. Results are utilized to assess the viability of Y2Si2O7 and other rare-earth silicates as environmental barrier coating (EBC) materials for SiC ceramic matrix composites (CMCs).  相似文献   

18.
    
The oxidation behavior of SiC fibers coated with (a) undoped polysilazane and (b) precursors containing a mixture of polysilazane and hafnium butoxide in equal weight fractions, is reported. The coatings were prepared by repetitive cycles of nanolayer depositions, as reported in recent publications. The oxidation experiments were carried out at 1400°C in ambient air (Boulder, CO) for up to 100 hours. The extent of degradation of SiC was measured by the recession in the diameter of the fibers as a function of time. The fibers with undoped polymer precursor recessed significantly, whereas the fibers coated with HfSiCNO remained essentially unchanged. These results are in agreement with earlier work from our laboratory where the resilience of hafnon and zircon, as well as hafnia and zirconia, against high-temperature corrosion in streaming humid environments had been highlighted.  相似文献   

19.
This work advances the understanding of the influence of rare earth (RE) ion radius on the stability and extent of the garnet solid solution phase in the (ytterbia/yttria/gadolinia)-calcia-magnesia-alumina-silica systems. Guided by the crystal chemistry and charge neutrality constraints, selected compositions in the notional garnet stability field were synthesized, equilibrated at 1400°C, and characterized to determine the equilibrium phases and their compositions. The results show a significant reduction in the stability of the silicate garnet relative to apatite with increasing RE ion radius. Apatite was not observed for any composition in the Yb-containing system, the Y-containing system formed both garnet and apatite, and there was no evidence of silicate garnets in the Gd-containing system. However, despite the apparent differences in stability relative to apatite, the extent of the garnet solid solution increases only slightly for the Yb- compared to Y-containing systems. The quantitative microchemical analysis suggests that Mg2+ prefers the octahedral site over the dodecahedral site in the garnet structure, and that the solubility of Mg2+ in the dodecahedral site increased in the system containing Yb3+ compared to Y3+. The results are discussed for their relevance to reactions between RE-containing thermal and environmental barrier coatings and CMAS-type silicate deposits.  相似文献   

20.
    
The K[AlSi2O6]-Cs[AlSi2O6] pseudo-binary system was synthesized by geopolymer crystallization. The thermal expansion properties of these materials were studied by in situ high-temperature X-ray diffraction to characterize thermal expansion behavior for potential application as environmental barrier coatings. Tailorable thermal expansion through changing cation stoichiometry allowed reduced thermal expansion mismatch with SiCf/SiC composites compared to rare-earth-based coatings.  相似文献   

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