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WO2014204480A1 - Systèmes de couche d'ancrage pour revêtement barrière environnemental - Google Patents

Systèmes de couche d'ancrage pour revêtement barrière environnemental Download PDF

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Publication number
WO2014204480A1
WO2014204480A1 PCT/US2013/046946 US2013046946W WO2014204480A1 WO 2014204480 A1 WO2014204480 A1 WO 2014204480A1 US 2013046946 W US2013046946 W US 2013046946W WO 2014204480 A1 WO2014204480 A1 WO 2014204480A1
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Prior art keywords
bond coat
silicon
component
oxide
substrate
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Ceased
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PCT/US2013/046946
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Inventor
Dongming Zhu
Janet B. Hurst
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National Aeronautics and Space Administration NASA
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National Aeronautics and Space Administration NASA
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Priority to PCT/US2013/046946 priority Critical patent/WO2014204480A1/fr
Publication of WO2014204480A1 publication Critical patent/WO2014204480A1/fr
Anticipated expiration legal-status Critical
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    • F01D5/00—Blades; Blade-carrying members; Heating, heat-insulating, cooling or antivibration means on the blades or the members
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Definitions

  • the general field of this innovation is environmental barrier coatings, and embodiments relate more specifically to environmental barrier coatings for silicon-based ceramic components.
  • EBC Environmental barrier coating
  • CMC monolithic ceramic or ceramic matrix composite
  • a coating system consisting of a high temperature capable advanced zirconia-based (or hafhia-based) oxide top coat (thermal barrier) and a less temperature capable rare earth silicates and mullite/barium-strontium-aluminosilicate (BSASySi environmental barrier is a state-of-the-art protective T/EBC coating system for the Si-based ceramic applications.
  • SiC/SiC turbine ceramic matrix composition applications including advanced
  • the innovation disclosed and claimed herein in aspects thereof, comprises systems, methods and articles that can include environmental barrier coating bond coat systems.
  • One example article can include a substrate, such as a SiC/SiC ceramic matrix composite substrate, and a bond coat system.
  • the bond coat system can include a bond coat that can include one or more of a silicon/silicide component or an oxide/silicate component.
  • interlayers can be included between the substrate and bond coat and external to the bond coat, and an optional environmental barrier coating top coat can be included external to the bond coat system.
  • FIG. 1 illustrates a first example environmental barrier coating (EBC) bond coat system in accordance with aspects of the subject innovation.
  • EBC environmental barrier coating
  • FIG. 2 illustrates a second example EBC bond coat system in accordance with aspects of the subject innovation.
  • FIG. 3 illustrates a third example EBC bond coat system in accordance with aspects of the subject innovation.
  • FIG. 4 illustrates a fourth example EBC bond coat system in accordance with aspects of the subject innovation.
  • FIG. 5 illustrates an example embodiment of an EBC bond coat system comprising a bond coat with a mixture phased region, in accordance with aspects of the subject innovation.
  • FIG. 6 illustrates an example bond coat system with self-healing in accordance with aspects of the subject innovation.
  • FIG. 7 illustrates the high temperature strength of several tested bond coat materials useable in aspects of the subject innovation.
  • FIG. 8 illustrates the flexural strength and deflection of Hf0 2 -Si bond coat materials useable in aspects of the subject innovation at various temperatures.
  • FIG. 9 illustrates testing results for RESi(0)-based bond coats.
  • FIG. 10 illustrates flexural strength for various bond coats of the subject innovation at room temperature and elevated temperatures.
  • FIGS. 1 1A, 1 IB, and 1 1C include specific examples of compositions useable in connection with various aspects of the subject innovation.
  • embodiments of the subject innovation can include systems, articles, and methods that can employ an advanced high temperature capable, low expansion and low diffusion environmental barrier coating (EBC) bond coat system for Si-based ceramics and ceramic matrix composites (CMCs).
  • EBC environmental barrier coating
  • Various aspects of the subject innovation can provide coating compositions and architecture arrangements that can achieve exceptional environmental barrier coating bond coat adhesion, oxidation and fatigue resistance, and environmental protection performance, along with self-healing capabilities that can ensure log-term durability for Si-based turbine ceramic components.
  • Environmental barrier coating bond coat systems, articles, and methods of the subject innovation can be employed in thin environmental barrier coating configurations, which can help enable the realization of ceramic turbine engine SiC/SiC CMC combustor and turbine airfoil applications.
  • FIG. 1 illustrates a first example
  • EBC bond coat system 100 in accordance with aspects of the subject innovation.
  • the EBC bond coat systems, articles, and methods employed in various aspects of the subject innovation can utilize compositions and architecture designs disclosed herein to enhance the coating high temperature stability, high toughness and strength, and durability performance.
  • the EBC bond coat system 100 is the coating layer directly adjacent to the substrate 102 (e.g., SiC/SiC ceramic matrix composite substrate, etc.), as shown in FIG. 1, which can improve environmental barrier coating adhesion and bonding strength, provide enhanced environmental protection, and, in various aspects of the subject innovation, can be designed to incorporate dynamic slow growth protective scale formation for oxidation resistance and seal healing.
  • EBC bond coat system 100 can include a bond coat 104, which can be as described herein.
  • environmental barrier bond coats 104 of the subject innovation can have any of a range of coating thicknesses, e.g., ranging from around 10 micrometers to around 200 micrometers.
  • Layers 106 and 108 which can be included in some
  • embodiments and can be excluded in other embodiments can be interlayers, e.g., diffusion barriers with crystalline and/or amorphous coatings as described herein, with the thickness ranging from around around 10 micrometers to around 200 micrometers .
  • EBC bond coat systems in accordance with the subject innovation can comprise one or both of two composition categories, referred to herein as Group A (also referred to herein as an "silicon/silicide component”) and Group B (also referred to herein as a “oxide/silicate component”).
  • Group A and Group B have low oxygen activities (or called “oxgen getter”) and higher oxygen but lower silica activities, respectively.
  • Members of Group A generally have superior oxidation resistance, while members of Group B generally have superior temperature resistance and combustion environmental resistance.
  • Group A (the "silicon/silicide component") can be an advanced silicon based alloy system as described herein, e.g., a rare earth (RE) based or doped silicon alloy or compound.
  • RE rare earth
  • Rare earth metals that can be employed in connection with group A include Ytterbium, Gadolinium, Neodymium, Samarium, Lutetium, Erbium, Europium, Terbium, Dysprosium, Holmium, Lanthanum, Cerium, Praseodymium, Promethium, Thulium (i.e., lanthanides), plus Yttrium and Scandium; Group A can also include doped Carbide-Nitrides of these.
  • Group B (the "oxide/silicate component”) can include highly stable Oxide and Silicate based material systems described herein.
  • bond coats of the subject innovation can include Hf0 2 (or Zr0 2 , etc.) and
  • Si/alloyed/doped Si optionally with various dopants as described herein.
  • Various embodiments of bond coats of the subject innovation incorporating Hf0 2 and Si or their alloys have been demonstrated to have excellent temperature and environmental resistance, including resistance to CMAS (Calcium Magnesium Alumino-Silicate) attack.
  • CMAS Calcium Magnesium Alumino-Silicate
  • EBC bond coats in accordance with the subject innovation can have advanced multi-component compositions, which can be arranged to form thermodynamically stable, multi-scale composites that have superior performance as compared to the current state of the art silicon bond coat.
  • Bond coat systems and articles in accordance with the subject innovation can have thermal expansion co-efficients in a range from 4-6 10 "6 m/nvK, comparable to the Si-based ceramics, and conventional Silicon bond coats.
  • Coatings of the subject innovation can be processed consistent with any of the current state-of-the-art coating processing methods.
  • embodiments of the subject innovation can comprise systems articles and methods that can utilize multi-component bond coat systems, which can include one or more of alloy doped Silicon; alloy-doped or silicon- rich Rare Earth (RE) Silicides; Rare Earth (RE) doped transition metal Silicides;
  • Embodiments of the subject innovation can form highly stable bond coat systems useable in connection with SiC/SiC CMC components.
  • Group A (the "silicon/silicide component") useable in connection with bond coat systems disclosed herein, can include (a) Rare Earth doped or alloyed Silicon, (b) Rare Earth (RE) Silicides (e.g., any of various stoichiometry compounds, such as RE5S13, RE5S14, RESi, RE3S15, RES-2, etc. and also particularly non-stoichiometry silicide compound compositions disclosed herein for optimum performance enhancement), which can include Ytterbium Silicides, Yttrium Silicides, Gadolinium Silicides, Erbium
  • RE Rare Earth
  • the Group A can be doped or oxidized with minor "oxygen" dopant or with oxygen gradients.
  • Group B (the "oxide/silicate component”) useable in connection with bond coat systems disclosed herein can significantly improve the temperature capability, environmental stability and strength capability, and can include (a) Rare Earth (RE) oxides (e.g., RE2O3), which can include Ytterbium Oxide, Yttrium Oxide, Gadolinium Oxide, Europium Oxide, etc.; (b) Rare Earth Mono-Silicates (RE 2 Si05) or Di-Silicates (RE2S12O7) such as Yb 2 Si0 5 , Yb 2 Si 2 0 7 , Y 2 SiO s , Gd 2 Si 2 0 7 , Gd 2 SiO s and Gd 2 Si 2 0 7 ; (c) other oxides such as Barium Oxide (BaO), Strontium Oxide (SrO), etc.; (d) Titanium and Tantalum-doped and un-doped Rare Earth Zirconium and Hafnium Pyrochlore
  • each of layer 106 and layer 108 can be a diffusion barrier, which in one embodiment can be a thin crystalline and/or amorphous coating of a silicon/silicide component (e.g., a member of Group A), which can have the capability of operating at temperatures of at least 1600°C (2912°F), and can have ultra low oxygen and water vapor diffusivity.
  • a silicon/silicide component e.g., a member of Group A
  • a silicon/silicide component e.g., a member of Group A
  • either or both of 106 (near the EBC top coats/bond coat interface) and layer 108 (near the bond coat/CMC interface) can comprise an extremely thin layered low diffusional coating, and can incorporate, utilizing a higher silicon content than bond coat 104, high temperature capable amorphous or crystalline phased Ta x SiCN, RETa x SiCN, Ti x (AlCrTa) y SiCN, or other compositions from Groups A or B.
  • layers 106 and 108 can be included, while in other embodiments they can be omitted.
  • bond coat 104 can be a multicomponent doped bond coat, comprising a silicon/silicide component (e.g., from Group A).
  • FIG. 2 illustrates a second example EBC bond coat system 200 in accordance with aspects of the subject innovation.
  • Substrate 202 and layers 206 and 208 (which can be optional, as with EBC bond coat system 100) can be as described elsewhere herein in connection with analogous components, e.g., those of FIG. 1.
  • Bond coat 204 can be a multicomponent doped bond coat, comprising an oxide/silicate component (e.g., from Group B).
  • an oxide/silicate component e.g., from Group B
  • members of Group A or Group B either individual members or combination thereof, can be used for EBC bond coats, as shown in FIGS. 1 and 2.
  • FIG. 3 illustrated is a third example of an EBC bond coat system 300 comprising a composite bond coat 304 in accordance with aspects of the subject innovation.
  • Substrate 302 and layers 306 and 308 can be as described above in connection with FIGS. 1 and 2 (with layers 306 and 308 again optional).
  • Bond coat 304 can comprise a composite of both a silicon/silicide component (e.g., from Group A) and an oxide/silicate component (e.g., from Group B), such as an oxide/silicate component (e.g., from Group B) as reinforcements 310 and embedded in a layer 312 composed of a silicon/silicide component (e.g., from Group A) or vice versa, as shown in bond coat 304.
  • silicon/silicide components useable in connection with bond coat 304, of the Rare Earth Silicides, dopants such as Aluminum can ensure superior cyclic and oxidation resistance under lower temperature conditions, which can prevent "pesting" from occurring.
  • the combination of components from both Group A and Group B can provide superior integrity and performance for the bond coat, via the sophisticated composite system of an Oxide-Silicate in combination with a Silicon alloy.
  • An extremely thin layered low diffusional coating near the bond coat/substrate (e.g., CMC) interface at 308, and a similar layer near the EBC top coat/bond coat interface at 306, can be incorporated, and can utilize a higher silicon content, high temperature capable amorphous or crystalline phased Ta x SiCN, RETa x SiCN, Ti x (AlCrTa) y SiCN, for example, or other members or combinations thereof selected from Groups A and B.
  • FIG. 4 illustrates a fourth example embodiment of an EBC bond coat system 400 comprising a layered composite bond coat 404 in accordance with aspects of the subject innovation.
  • Substrate 402 and layers 406 and 408 can be as described in connection with similar components of FIGS. 1, 2, and 3.
  • Bond coat 404 can be arranged in a layered composite configuration with alternating layers 410 and 412 of a
  • EBCs when included, can be as described herein, for example, comprising a high stability multicomponent Hf0 2 - RE 2 03-Si02 RE2Si2.x07.2 X ; in other embodiments, other components described herein can be used additionally or alternatively in connection with environmental barrier coats.
  • silicon/silicide components e.g., from Group A
  • silicon/silicide components can be employed that can have relatively high silicon content designs (silicon-rich, off-stoichiometry silicide compositions) to provide superior oxidation resistance.
  • silicon-rich silicides such as RE3S15 and RES12 can provide such a relatively high silicon content, for example, and also RE3Sis+ x and RES12 where the "x" indicates a modified composition with the silicon rich silicides for superior performance.
  • FIG. 5 illustrates an example embodiment of an EBC bond coat system 500 comprising a bond coat 504 with a mixture phased region, in accordance with aspects of the subject innovation.
  • Substrate 502 and layers 506 and 508 can be as described in connection with other embodiments (again, layers 506 and 508 can be optional).
  • FIG. 5 also shows a thermal and environmental barrier coating (T/EBC) 510, which can be optionally included in any embodiments described herein.
  • Bond coat 504 can comprise a mixture phased region 512-516 of increasing silicon or silica content or silica activity at portions of bond coat 504 closer to the substrate 502 (e.g., CMC) when compared with portions more distant from substrate 502.
  • the mixture phased region is indicated in FIG.
  • RESi mixture phased region of RESi, or RESi(O), RE 3 Si 5 or RE 3 Si 5 (0) and RESi 2 (0), with the silicon concentration between 50 and 67 molar%, and can provide excellent temperature capability and oxidation resistance.
  • Various embodiments can have a silicon molar concentration in the range from 62 to 70%.
  • Other embodiments of the subject innovation can have atomic percentages for silicon between 55 and 95%, or between 60 and 90%, or between 65 and 95%, etc.
  • Silicon-rich bonded Silicide composites can provide coatings with excellent temperature capability and durability.
  • Ti x (AlCrTa) y Si-(C)N type coating systems high silicon concentration (e.g., up to 60 molar%) can produce coatings with extremely high temperature capability (1600- 1700°C), exceptional mechanical properties, and low diffusivity amorphous coating formation.
  • Bond coats that comprise both a silicon/silicide component (e.g., from Group A) and an oxide/silicate component (e.g., from Group B) can provide for a coating with capability.
  • the oxide/silicate component e.g., refractory metal or rare earth oxides or silicates, etc.
  • the advanced RE and RE doped Silicon or Silicide of Group A and the oxide-silicate compositions of Group B can also enhance the bond coat self-healing in the event cracking develops, and can also provide excellent oxidation and combustion environment protection under extreme environments.
  • FIG. 6 illustrates an example bond coat system 600 with self-healing in accordance with aspects of the subject innovation.
  • the substrate 602 can be as described elsewhere herein, and thin layers diffusion barriers can be included, although not shown in FIG. 6.
  • Bond coat 604 can be any of a variety of bond coats as described herein, although the bond coat illustrated is similar to that illustrated in connection with FIG. 5.
  • Bond coat 604 can comprise a silicon/silicide component, an oxide/silicate component, or a combination of the two, and can have a graded composition as described above in connection with mixture phased region 512-516 of FIG.
  • Bond coat 604 is capable of self-healing cracks and self-growth of a low silica activity and high stability EBC, as shown at 606.
  • a thermal and environmental barrier coating (T/EBC) top coat 608 can be included, but it need not be included in all embodiments, due to the ability of bond coat 604 to self-grow an EBC for superior stress and fatigue resistance.
  • environmental barrier coating bond coat systems described herein can employ any of a variety of compositions and architectures described herein. Experimental results obtained in connection with embodiments of EBC bond coat systems useable in connection with Si-based ceramic and CMC component applications have demonstrated higher temperature capabilities and durability than state-of-the-art coatings in laboratory simulated engine environments. Various aspects and embodiments of bond coating systems disclosed herein have been successfully tested and demonstrated at the sub-element and sub-component levels. 10039) In various aspects, embodiments can employ an oxide-Si bond coat as described herein, in combination with an RE silicate or RE aluminosilicate EBC.
  • Interlayers in such an embodiment can comprise RE-Hf02/Zr02-aluminosilicate layered coatings.
  • Various high stability coatings can be employed in various aspects of the innovation, which can include one or more of RE oxide doped HfCVZrC , pyrochlores (RE 2 Zr 2 07- RE 2 Zr207), perovskites (e.g., RE-SrZr03, etc.), magnetoplumbites (e.g., REMgAlnOi9, etc.), or RE-Hafhia plus RE aluminosilicate composite coatings.
  • embodiments of the subject innovation can also comprise other coats that can form an EBC system, such as top coats described herein.
  • top coats of the subject innovation can employ various materials, such as those of the form RE-Hf0 2 -X, RE-Hf0 2 -graded Silica, RE-Hf0 2 -Alumino Silicate, etc.
  • Top coats can be applied via EB-PVD or other suitable techniques, such as EB-PVD Hf0 2 -RE 2 0 2 , etc.
  • coats and coat systems of the subject innovation can be applied via a variety of techniques, such as applied by Electron Beam-Physical Vapor Deposition (EB-PVD), Plasma-Spray Physical Vapor Deposition (PS-PVD), Plasma- Spray - Thin Film (PS-TF), High temperature Vacuum Vapor Deposition, Chemical vapor Deposition, etc.
  • EB-PVD Electron Beam-Physical Vapor Deposition
  • PS-PVD Plasma-Spray Physical Vapor Deposition
  • PS-TF Plasma- Spray - Thin Film
  • High temperature Vacuum Vapor Deposition Chemical vapor Deposition, etc.
  • silicate/HfC -RE-Silicate with distinct vapor pressures can be applied via EB-PVD with co-deposition.
  • PS-PVD and/or PS-TF coating processes can be employed, with PVD splat coating processing at low pressure (e.g., around 1 torr, etc.).
  • high velocity vapor and non-line-of-sight coating processing can be employed.
  • PS techniques used herein can employ a high enthalpy plasma vapor stream for efficient and complex thin film coating processing.
  • FIG. 7 illustrates the high temperature strength of several tested bond coat materials useable in aspects of the subject innovation.
  • FIG. 8 illustrates the flexural strength and deflection of HfC>2-Si bond coat materials useable in aspects of the subject innovation at various temperatures.
  • the bond coat systems of the subject innovation have excellent strength and toughness.
  • Other tested bond coats included RESiO+X (Ta, Al, Hf, Zr, etc.) bond coats, RESi+X bond coats, Zr/Hf-RE-Si bond coats, etc.
  • FIG. 9 illustrates testing results for RESiO-based bond coats, showing a Silicon concentration range that can provide for improved oxidation resistance at 1500°C.
  • FIG. 10 illustrates flexural strength for various environmental barrier bond coats of the subject innovation at room temperature and elevated
  • coatings in accordance with various aspects of the subject innovation can comprise (a) Silicon cladded ⁇ 2 (e.g., agglomerated or sinter crushed ⁇ 1 ⁇ 2 powders, which can be at or near a 30:70 weight ratio of Si:HfC>2); (b) Yttrium monosilicate, with approximately a 50:50 molar ratio of Y2O3 and Si0 2 (i.e., around 78.984% weight and 21.016% weight, respectively); (c) Silicon cladded ytterbium monosilicate plus minor t' HfC> 2 (e.g., in a weight ratio of approximately 30:60:10 of Si : Ytterbium monosilicate : t' Hf0 2 ); (d) Silicon cladded ytterbium monosilicate (e.g., in a weight ratio of approximately 30:70 of Si: Ytterbium monosilicate
  • bond coats in certain embodiments can comprise (a) Silicon with 30% atomic weight of Ytterbium; (b) alternating and co- deposition of 50% Gd 2 0 3 with Si plus 30 at.% Yb and 50% Yb 2 0 3 with Si plus 30 at.% Yb; or (c) a composite bond coat of HfO 2 with Si plus 30 at.% Yb.
  • the thickness of these example bond coats can be in the range of 3 to 5 mils, although greater or lesser thicknesses can be used in various embodiments.
  • certain embodiments of bond coat systems can comprise (a) Silicon with 15% atomic weight of Gadolinium; (b) alternating and co-deposition of 50% Gd 2 0 3 with Si and 50% ⁇ 13 ⁇ 40 3 with Si; or (c) a composite bond coat of Hf0 2 with Si plus 15 at.% Gd.
  • an alternating layer system can be employed with a total thickness of around 10 mils.
  • a bottom system (of thickness around 5 mils) can be included that alternates between (a) Hf0 2 (5% molar, 6.086% weight), Y 2 0 3 (5% molar, 6.529% weight), Gd 2 0 3 (5% molar, 20.962% weight), Yb 2 0 3 (25% molar, 45.576% weight), with co-deposition of Si0 2 (60% molar, 20.847% weight) and (b) Hf0 2 (96% molar, 90.7333% weight), Y 2 0 3 (2% molar, 3.464% weight), Gd 2 0 3 (1% molar, 2.780% weight), and Yb 2 0 3 (1% molar, 3.023% weight).
  • a top system can be included (also of thickness around 5 mils) that alternates between (a) HfO 2 (30% molar, 27.598% weight), Y 2 0 3 (5% molar, 4.934% weight), Gd 2 0 3 (5% molar, 7.921% weight), Yb 2 0 3 (30% molar, 51.669% weight), with co- deposition of Si0 2 (30% molar, 7.878% weight) and (b) Hf0 2 (96% molar, 90.7333% weight), Y 2 0 3 (2% molar, 3.464% weight), Gd 2 0 3 (1% molar, 2.780% weight), and Yb 2 0 3 (1% molar, 3.023% weight).
  • Si0 2 grading can be used with both.
  • the chemical compositions can vary from the specific ratios provided, while remaining within the scope of the subject innovation.
  • FIGS. 1 1 A, 1 IB, and 1 1C include other specific examples of compositions useable in connection with various aspects of the subject innovation; again, these examples are provided for purposes of illustration, and are not intended to be limiting.
  • the subject innovation in various embodiments, can provide bond coat systems that can be critical for future development of advanced high performance gas turbine engine applications.
  • the environmental barrier bond coating system is one of the most critical technologies that can lead to the future realization of SiC/SiC CMC turbine engine combustor liners and vanes, and turbine blades, allowing the engines to be operated at much higher temperatures with significantly reduced cooling requirements.
  • This technology can be also used in a variety of other settings in which ceramic components will be subjected to extreme temperature or environmental conditions, such as land-based stationary gas turbines for power generation, and other energy related heat engine systems.

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Abstract

La présente invention concerne des systèmes avancés de couches d'ancrage pour revêtement barrière environnemental présentant de meilleures caractéristiques thermiques et une meilleure résistance environnementale. Ces systèmes de couches d'ancrage peuvent être appliqués à des substrats céramiques tels que les substrats composites de matrice céramique SiC/SiC, et peuvent conférer une protection vis-à-vis des températures extrêmes, des charges mécaniques et des conditions environnementales, comme dans les turbines à gaz à haute température. Les exemples de systèmes de couches d'ancrage peuvent inclure soit un composant avancé silicium/siliciure, soit un composant oxyde/silicate, soit l'une de leurs combinaisons.
PCT/US2013/046946 2013-06-21 2013-06-21 Systèmes de couche d'ancrage pour revêtement barrière environnemental Ceased WO2014204480A1 (fr)

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