CN1935746A - 具有含铪阻隔层的硅基基材 - Google Patents
具有含铪阻隔层的硅基基材 Download PDFInfo
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- CN1935746A CN1935746A CNA2006101061366A CN200610106136A CN1935746A CN 1935746 A CN1935746 A CN 1935746A CN A2006101061366 A CNA2006101061366 A CN A2006101061366A CN 200610106136 A CN200610106136 A CN 200610106136A CN 1935746 A CN1935746 A CN 1935746A
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- 230000004888 barrier function Effects 0.000 title claims abstract description 73
- 229910052735 hafnium Inorganic materials 0.000 title claims abstract description 49
- VBJZVLUMGGDVMO-UHFFFAOYSA-N hafnium atom Chemical compound [Hf] VBJZVLUMGGDVMO-UHFFFAOYSA-N 0.000 title claims abstract description 48
- 239000000758 substrate Substances 0.000 title claims abstract description 16
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 title claims description 30
- 239000010703 silicon Substances 0.000 title claims description 30
- 229910052710 silicon Inorganic materials 0.000 title claims description 28
- 238000000576 coating method Methods 0.000 claims abstract description 35
- 239000011248 coating agent Substances 0.000 claims abstract description 33
- GFQYVLUOOAAOGM-UHFFFAOYSA-N zirconium(iv) silicate Chemical compound [Zr+4].[O-][Si]([O-])([O-])[O-] GFQYVLUOOAAOGM-UHFFFAOYSA-N 0.000 claims abstract description 19
- 238000000034 method Methods 0.000 claims abstract description 17
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 claims abstract 16
- 239000000463 material Substances 0.000 claims description 44
- 239000000203 mixture Substances 0.000 claims description 19
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 16
- 239000000654 additive Substances 0.000 claims description 14
- 230000000996 additive effect Effects 0.000 claims description 13
- 229910010271 silicon carbide Inorganic materials 0.000 claims description 12
- 229910052581 Si3N4 Inorganic materials 0.000 claims description 10
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 claims description 10
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 claims description 8
- 239000000377 silicon dioxide Substances 0.000 claims description 8
- 239000002131 composite material Substances 0.000 claims description 7
- 239000002002 slurry Substances 0.000 claims description 7
- 229910000323 aluminium silicate Inorganic materials 0.000 claims description 6
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 6
- 229960001866 silicon dioxide Drugs 0.000 claims description 6
- 235000012239 silicon dioxide Nutrition 0.000 claims description 6
- 238000007669 thermal treatment Methods 0.000 claims description 6
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 5
- 150000001875 compounds Chemical class 0.000 claims description 5
- KZHJGOXRZJKJNY-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Si]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O KZHJGOXRZJKJNY-UHFFFAOYSA-N 0.000 claims description 5
- 229910001092 metal group alloy Inorganic materials 0.000 claims description 5
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- 238000002360 preparation method Methods 0.000 claims description 5
- 229910000449 hafnium oxide Inorganic materials 0.000 claims description 4
- WIHZLLGSGQNAGK-UHFFFAOYSA-N hafnium(4+);oxygen(2-) Chemical compound [O-2].[O-2].[Hf+4] WIHZLLGSGQNAGK-UHFFFAOYSA-N 0.000 claims description 4
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims description 4
- 238000007750 plasma spraying Methods 0.000 claims description 4
- WOIHABYNKOEWFG-UHFFFAOYSA-N [Sr].[Ba] Chemical group [Sr].[Ba] WOIHABYNKOEWFG-UHFFFAOYSA-N 0.000 claims description 3
- -1 silicon aluminium keto nitride Chemical class 0.000 claims description 3
- 229930194542 Keto Natural products 0.000 claims description 2
- 229910003070 TaOx Inorganic materials 0.000 claims description 2
- 229910010413 TiO 2 Inorganic materials 0.000 claims description 2
- 239000004411 aluminium Substances 0.000 claims description 2
- 229910052782 aluminium Inorganic materials 0.000 claims description 2
- 238000005229 chemical vapour deposition Methods 0.000 claims description 2
- 238000007598 dipping method Methods 0.000 claims description 2
- 238000001652 electrophoretic deposition Methods 0.000 claims description 2
- 238000005367 electrostatic precipitation Methods 0.000 claims description 2
- 229910052574 oxide ceramic Inorganic materials 0.000 claims description 2
- 239000011224 oxide ceramic Substances 0.000 claims description 2
- 238000005240 physical vapour deposition Methods 0.000 claims description 2
- 229910001404 rare earth metal oxide Inorganic materials 0.000 claims description 2
- 229910052712 strontium Inorganic materials 0.000 claims description 2
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 claims description 2
- 229910004298 SiO 2 Inorganic materials 0.000 claims 1
- 229910052727 yttrium Inorganic materials 0.000 claims 1
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 claims 1
- 230000007613 environmental effect Effects 0.000 abstract description 3
- IJKVHSBPTUYDLN-UHFFFAOYSA-N dihydroxy(oxo)silane Chemical compound O[Si](O)=O IJKVHSBPTUYDLN-UHFFFAOYSA-N 0.000 description 31
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 6
- 229910004129 HfSiO Inorganic materials 0.000 description 6
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- 101100373011 Drosophila melanogaster wapl gene Proteins 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 2
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- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 1
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- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 1
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 1
- 229910020010 Nb—Si Inorganic materials 0.000 description 1
- BOTDANWDWHJENH-UHFFFAOYSA-N Tetraethyl orthosilicate Chemical compound CCO[Si](OCC)(OCC)OCC BOTDANWDWHJENH-UHFFFAOYSA-N 0.000 description 1
- HMDDXIMCDZRSNE-UHFFFAOYSA-N [C].[Si] Chemical compound [C].[Si] HMDDXIMCDZRSNE-UHFFFAOYSA-N 0.000 description 1
- 238000009825 accumulation Methods 0.000 description 1
- 238000000137 annealing Methods 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 229910052788 barium Inorganic materials 0.000 description 1
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
- 239000011575 calcium Substances 0.000 description 1
- 239000012159 carrier gas Substances 0.000 description 1
- 229910010293 ceramic material Inorganic materials 0.000 description 1
- AIOWANYIHSOXQY-UHFFFAOYSA-N cobalt silicon Chemical compound [Si].[Co] AIOWANYIHSOXQY-UHFFFAOYSA-N 0.000 description 1
- 229910052681 coesite Inorganic materials 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 238000010668 complexation reaction Methods 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 229910052906 cristobalite Inorganic materials 0.000 description 1
- 238000003618 dip coating Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000003628 erosive effect Effects 0.000 description 1
- 238000007731 hot pressing Methods 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- XWHPIFXRKKHEKR-UHFFFAOYSA-N iron silicon Chemical compound [Si].[Fe] XWHPIFXRKKHEKR-UHFFFAOYSA-N 0.000 description 1
- 229910052744 lithium Inorganic materials 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 239000011777 magnesium Substances 0.000 description 1
- 229910021645 metal ion Inorganic materials 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 229910021471 metal-silicon alloy Inorganic materials 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- HFLAMWCKUFHSAZ-UHFFFAOYSA-N niobium dioxide Inorganic materials O=[Nb]=O HFLAMWCKUFHSAZ-UHFFFAOYSA-N 0.000 description 1
- LIZIAPBBPRPPLV-UHFFFAOYSA-N niobium silicon Chemical compound [Si].[Nb] LIZIAPBBPRPPLV-UHFFFAOYSA-N 0.000 description 1
- 239000003921 oil Substances 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 230000002035 prolonged effect Effects 0.000 description 1
- 239000011253 protective coating Substances 0.000 description 1
- 239000003870 refractory metal Substances 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
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- 239000012779 reinforcing material Substances 0.000 description 1
- 230000000630 rising effect Effects 0.000 description 1
- 150000003377 silicon compounds Chemical class 0.000 description 1
- HWEYZGSCHQNNEH-UHFFFAOYSA-N silicon tantalum Chemical compound [Si].[Ta] HWEYZGSCHQNNEH-UHFFFAOYSA-N 0.000 description 1
- 239000011863 silicon-based powder Substances 0.000 description 1
- 229910021484 silicon-nickel alloy Inorganic materials 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000011734 sodium Substances 0.000 description 1
- 238000003980 solgel method Methods 0.000 description 1
- 239000007921 spray Substances 0.000 description 1
- 238000005507 spraying Methods 0.000 description 1
- 229910052682 stishovite Inorganic materials 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 230000008646 thermal stress Effects 0.000 description 1
- 239000004408 titanium dioxide Substances 0.000 description 1
- 229910052905 tridymite Inorganic materials 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
- C04B41/80—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone of only ceramics
- C04B41/81—Coating or impregnation
- C04B41/85—Coating or impregnation with inorganic materials
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B9/00—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00
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- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
- C04B41/009—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone characterised by the material treated
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
- C04B41/45—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements
- C04B41/50—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements with inorganic materials
- C04B41/5024—Silicates
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- C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
- C04B41/45—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements
- C04B41/52—Multiple coating or impregnating multiple coating or impregnating with the same composition or with compositions only differing in the concentration of the constituents, is classified as single coating or impregnation
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- C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
- C04B41/80—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone of only ceramics
- C04B41/81—Coating or impregnation
- C04B41/89—Coating or impregnation for obtaining at least two superposed coatings having different compositions
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- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C28/00—Coating for obtaining at least two superposed coatings either by methods not provided for in a single one of groups C23C2/00 - C23C26/00 or by combinations of methods provided for in subclasses C23C and C25C or C25D
- C23C28/04—Coating for obtaining at least two superposed coatings either by methods not provided for in a single one of groups C23C2/00 - C23C26/00 or by combinations of methods provided for in subclasses C23C and C25C or C25D only coatings of inorganic non-metallic material
- C23C28/042—Coating for obtaining at least two superposed coatings either by methods not provided for in a single one of groups C23C2/00 - C23C26/00 or by combinations of methods provided for in subclasses C23C and C25C or C25D only coatings of inorganic non-metallic material including a refractory ceramic layer, e.g. refractory metal oxides, ZrO2, rare earth oxides
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- C23C28/00—Coating for obtaining at least two superposed coatings either by methods not provided for in a single one of groups C23C2/00 - C23C26/00 or by combinations of methods provided for in subclasses C23C and C25C or C25D
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- C23C30/00—Coating with metallic material characterised only by the composition of the metallic material, i.e. not characterised by the coating process
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- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C4/00—Coating by spraying the coating material in the molten state, e.g. by flame, plasma or electric discharge
- C23C4/04—Coating by spraying the coating material in the molten state, e.g. by flame, plasma or electric discharge characterised by the coating material
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- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C4/00—Coating by spraying the coating material in the molten state, e.g. by flame, plasma or electric discharge
- C23C4/18—After-treatment
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Abstract
一种制品，其包含含硅基材和阻隔层，该阻隔层起环境阻隔涂层的作用，更具体地是包含硅酸铪和任选地硅酸锆的阻隔层，以及用于形成作为阻隔涂层的硅酸铪的方法。
Description
政府所有权声明
作为根据合同NO0014-03-C-0477由美国海军研究所赞助的结果，美国政府在本发明中可能拥有权力。
技术领域
本发明涉及一种制品，其包含基材，该基材包含硅和阻隔层，该阻隔层起环境阻隔涂层的作用，并且更具体地这样一种阻隔层，其包含硅酸铪和任选地硅酸锆。本发明进一步包括作为阻隔涂层形成硅酸铪的方法。
背景技术
已经提出了将含硅陶瓷材料和含硅金属合金用于在高温应用中使用的结构，例如燃气轮机、换热器、内燃机等等。含硅陶瓷具有有吸引力的物理和机械性能，并且特别可用于气轮机高温段，其在高温、高压和富含高速蒸汽的环境下操作。已经发现，这些含硅材料易于受到蒸汽的侵蚀，因为当暴露于在气轮机应用中遇到的高温、含水环境时会形成挥发性的硅物质，特别是Si(OH)x和SiO。含硅物质从含硅基材中挥发导致基材凹陷，这在长期应用中显然是不希望的。已经将环境阻隔涂层(EBCs)应用于硅基陶瓷上，以防止基材凹陷和延长气轮机部件的寿命。
对于EBC涂层，在基材上使用一个或多个层，例如阻隔层、粘合层、中间层等等，也是常见的。在选择阻隔层/粘合层/中间层中一个重要的标准是层的热膨胀系数(CTE)。为了使各种涂层和基材之间的热应力积累最小化，重要的是涂层系统的各种成分的CTE接近于基材的CTE。邻近的涂层和/或基材之间CTE的不匹配可能导致非保护性涂层，因为在气轮机操作中遇到的热周期期间涂层出现剥落和/或龟裂。
因此，本发明的主要目的是提供一种制品，其包含含硅基材和至少一个阻隔层，其中阻隔层具有的热膨胀系数是与基材相容的，如果阻隔层邻近于基材，并且与是任何其他的相邻层相容的。本发明的阻隔层还可以用于具有低热膨胀系数的其他陶瓷基材的热和环境保护。
本发明的进一步目的和优点在下文中是显而易见的。
发明内容
本发明的制品包含基材和阻隔层，该阻隔层起环境阻隔涂层的作用，其中所述阻隔层包含硅酸铪。按照本发明，硅酸铪作为阻隔层中的组分是特别有用的，因为硅酸铪具有高熔点，大约1750℃，并且在蒸汽中是稳定的。此外，从室温到1200℃，硅酸铪的热膨胀系数是大约4.5到4.6ppm/℃，这使其与陶瓷和CTE在3-7ppm/℃范围内的复合材料相容。这些综合性能使含硅酸铪的阻隔层特别可用于环境阻隔涂层系统，用于含碳化硅和氮化硅的基材。所述基材可以包括任何适合的材料，例如含硅基材(即含硅陶瓷、含硅金属合金等等)和氧化物-氧化物基材。适合的含硅陶瓷包括，但是不局限于，氮化硅、碳化硅、碳化硅复合材料、氮化硅复合材料、氮氧化硅、氧氮化硅铝、氮化硅陶瓷基质复合材料等等。适合的含硅金属合金包括，但是不局限于，钼硅合金、铌硅合金、铁硅合金、钴硅合金、镍硅合金、钽硅合金、耐熔金属硅化物等等。适合的氧化物-氧化物基材包括，但是不局限于，纤维增强氧化物基质复合材料，其中纤维增强材料包括碳化硅、氮化硅、氧化铝、富铝红柱石等等，并且基质包括氧化铝、氧化锆和类似的耐热氧化物。
按照本发明，阻隔层包含硅酸铪和任选地硅酸锆。在优选的实施方案中，本发明的阻隔层包含硅酸铪和硅酸锆两者。除上述之外，如有必要，阻隔层可以进一步包括热膨胀系数(CTE)控制添加剂。本发明的阻隔层适合作为热和环境阻隔涂层。本发明的阻隔层还可以被用作中间层，以防止在已知的环境阻隔涂层系统(例如Si/HfO2体系)中邻近的反应性层之间的相互作用。本发明还涉及在表面上产生阻隔涂层的方法。
按照本发明，优选的方法包括：制备二氧化铪和硅源的混合物，用该混合物涂覆表面，和其后将涂层暴露于升高的温度达到足够的时间，以使二氧化铪与氧化性硅反应，产生致密的硅酸铪涂层。
根据以下详细说明能够明确本发明的其他目的和优点。
附图说明
附图比较了在90％蒸汽的环境中、在1315℃的温度下，作为相对重量损失的函数的BSAS涂层与单块硅酸铪涂层的凹陷速率。
详细说明
本发明涉及一种制品，其包含基材和阻隔层，其中阻隔层抑制在制品暴露于高温、燃烧环境时从基材中形成气态硅物质。本发明还涉及产生上述的涂层制品的方法。此外，应该理解，虽然阻隔层被称作环境阻隔层，该阻隔层还起热障层的作用，并且因此本发明广泛地包括在含硅基材上和在具有类似的热膨胀系数的基材上环境阻隔层/热障层的用途。
按照本发明，含硅基材可以是含硅陶瓷基材或者含硅金属合金。在优选的实施方案中，含硅基材是含硅陶瓷材料，例如碳化硅、氮化硅、硅碳氮化物、铝硅酸盐/富铝红柱石、氮氧化硅、氧化物/氧化物陶瓷基质复合材料和硅铝氧氮化物和其混合物。按照本发明特定的实施方案，含硅陶瓷基材包括具有增强材料的含硅基质，例如纤维、粒子等等，并且更具体地纤维增强的硅基基质。特别适合的陶瓷基材是单块氮化硅、碳化硅涂覆的碳化硅纤维-增强的碳化硅粒子和硅基质、碳纤维-增强的碳化硅基质和碳化硅纤维-增强的氮化硅基质。用作用于本发明制品的基材的特别有用的硅-金属合金包括钼-硅合金、铌-硅合金、及其他含硅合金，其具有与本发明阻隔层相容的热膨胀系数。阻隔层还可以为氧化物-氧化物基材提供环境和热保护，所述基材包括但不限于纤维增强的氧化物基质复合材料，其中纤维增强材料包括碳化硅、氮化硅、氧化铝、富铝红柱石等等，并且基质包括氧化铝、氧化锆和类似的耐热氧化物。
本发明的特别有用的阻隔层包括硅酸铪，并且优选地硅酸铪和硅酸锆的混合物。当阻隔层包括硅酸铪而没有硅酸锆时，阻隔层应该包含至少50体积％的硅酸铪。优选地，阻隔层包含50到100体积％的硅酸铪，理想地60到100体积％硅酸铪。当阻隔层包含硅酸铪及硅酸锆时，硅酸铪和硅酸锆的总体积百分数在50到100体积％之间，并且优选在65到100％之间。在优选的实施方案中，硅酸铪和硅酸锆以1∶49到49∶1、优选1∶19到19∶1的体积比存在。
按照本发明优选的实施方案，阻隔层可以包括热膨胀系数(CTE)控制添加剂，其量足以使阻隔层和任何相邻层和/或基材之间保持相容。CTE控制添加剂选自TaOx、NbOx、MgO、CaO、SrO、BaO、SiO2、HfO2、TiO2、ZrO2、Al2O3、Y2O3、La2O3、稀土氧化物和其混合物，其中x＝1到3(例如NbO、NbO2、Nb2O3、Nb2O5)。按照本发明优选的实施方案，CTE控制添加剂被加入到层材料中，用于调节该层的CTE，以便使该层与基材和可能被使用的任何其他相邻层相容。
CTE控制添加剂应该以足以在其本身和相邻层和基材之间保持相容性的量存在于该层中。当将例如HfO2加入如上所述的阻隔层时，其应该以至少5体积％、优选10到50体积％、理想地10到40体积％的量存在。
本发明的一个重要特征是保持含硅基材和所述层和/或相邻层的热膨胀系数之间的相容性。按照本发明，已经发现，所述层的CTE应该在含硅基材和/或相邻层的CTE的±3.0ppm/℃、优选±2.0ppm/℃和理想地1ppm/℃范围内。
阻隔层应该以大于或等于大约0.05密耳(0.00005英寸)、优选大约0.1到大约300密耳和理想地大约0.1到大约10密耳的厚度存在于制品中。本发明的阻隔层可以通过以下方法施加：浆液涂布技术、浆液涂漆、空气等离子体喷涂、气刷、溶胶-凝胶途径、溶胶-凝胶、热喷涂、化学蒸汽沉积、物理蒸汽沉积、电泳沉积、静电沉积、浸渍和溅射。通过浆液涂覆进行施加是挑战性的，因为硅酸铪和硅酸锆具有耐熔本性，并且它们具有缓慢的烧结速度。如果所述涂层通过浆液涂覆方法施加，则可以将添加剂例如二氧化硅、氧化铝、二氧化钛以及钠、锂、钙、锶、钡和镁的氧化物用作烧结助剂。当进行浸涂时，起始浆液可以从HfO2、ZrO2和硅或者二氧化硅的混合物制备。还可以使用其他添加剂。硅酸铪和硅酸锆的混合物还可以通过溶胶-凝胶法制造，该方法使用铪/锆氧氯化物、盐酸和TEOS在络合金属离子存在下进行，或者通过实际已知的溶胶-凝胶过程的变体制造。施加硅酸铪涂层(以及视需要的硅酸锆)的一种优选的方法是等离子喷涂。按照本发明，硅酸盐通过将铪(以及视需要的锆)氧化物与元素硅或者二氧化硅或者其他的含硅源混合，并且将该混合物等离子喷涂到表面上形成涂层来施加。然后将涂层在980到1650℃、优选1200到1485℃的温度下热处理至少0.5小时、优选2到200小时，形成包含硅酸铪(以及视需要的硅酸锆)的涂层。该阻隔层还可以在制品操作期间就地形成。当二氧化硅源是硅时，极其重要的是热处理在氧化环境中进行。
施加本发明涂层的另一种方法是二氧化铪(以及视需要的氧化锆)与硅源(硅或者二氧化硅)的交替层的化学蒸气沉积，然后进行一个或多个反应退火步骤，以使金属氧化物与硅反应形成希望的硅酸盐或者硅酸盐混合物。
生产本发明硅酸铪涂层的优选的方法描述在下文中。
具体实施例
实施例
使用表1中列出的参数将HfO2和Si粉末的混合物进行等离子喷涂。随后将涂层在空气中在1315℃下热处理大约100小时。得到的涂层中所有硅被转化成HfSiO4。虽然在涂层中残留有游离的HfO2，但是该实施例显示，可以通过该方法通过适当选择HfO2和Si量来形成HfSiO4。为了使HfSiO4的产生完全，应该选择HfO2和硅的1∶1摩尔混合物。应当注意到，在沉积期间基材温度可以为室温到1100℃。
| 粉末组成 | HfO2-20重量％Si | HfO2-10重量％Si |
| 枪 | Metco3M(GH喷嘴) | Metco3M(GH喷嘴) |
| 第一气体 | Ar | Ar |
| 第二气体 | 氢 | 氢 |
| 电流 | 600mA | 600mA |
| 电压 | 50V | 50V |
| 载气 | Ar | Ar |
| 离开距离(英寸) | 4.75 | 4.75 |
| 喷涂温度(℃) | 1093 | 1093 |
| 涂层厚度(微米) | 125 | 125 |
| 枪速度(英寸/秒) | 6 | 6 |
为了表明本发明阻隔层与现有技术钡锶铝硅酸盐(BSAS)阻隔层相比的优点，制备了具有BSAS和HfSiO4组合物的样板，并且在富蒸汽环境中测试：致密的BSAS样板(Ba0.75Sr0.25Al2Si2O8)通过热压加工。致密的硅酸铪样板通过冷压，然后在1600℃下烧结来制备。将组合物的试件随后热处理到1600℃。在具有90％水蒸汽和10％氧气的常压蒸汽装置中将样品暴露于蒸汽。蒸汽暴露在1315℃下进行超过500小时。通过测量暴露的单位面积材料的重量损失计算凹陷速率。
附图显示了与钡锶铝硅酸盐相比的如上制备的单块硅酸铪的凹陷速率的比较结果。从图中可以看到，在蒸汽环境中，与BSAS相比硅酸铪至少要好1.5倍。HfSiO4与BSAS相比改进的蒸汽稳定性表明，使用HfSiO4层作为蒸汽阻隔层的涂层系统与使用具有相同厚度的BSAS的涂层系统相比将是更耐用的。
显然，本发明提供了具有含硅酸铪的阻隔层的硅基基材，其完全满足以上提出的目的、手段和优点。虽然本发明已经在其特定的实施方案的叙述中被描述，但是本领域技术人员在阅读上述说明书的基础上将容易得出其他的替代、修改和变化方案。因此，试图包括这些处于所附权利要求的宽范围内的替代、修改和变化方案。
Claims (30)
1.一种制品，其包含：
含硅基材；和
含硅酸铪的阻隔层。
2.权利要求1的制品，其中阻隔层包含至少50体积％的硅酸铪。
3.权利要求1的制品，其中阻隔层包含50到100体积％的硅酸铪。
4.权利要求1的制品，其中阻隔层包含60到100体积％的硅酸铪。
5.权利要求1的制品，其中阻隔层包含50到100体积％的量的硅酸铪和硅酸锆。
6.权利要求1的制品，其中阻隔层包含65到100体积％的硅酸铪和硅酸锆。
7.权利要求5的制品，其中阻隔层包含1∶49到49∶1体积比的硅酸铪和硅酸锆。
8.权利要求5的制品，其中阻隔层包含1∶19到19∶1体积比的硅酸铪和硅酸锆。
9.权利要求2的制品，其中阻隔层还包含CTE控制添加剂，其选自TaOx、NbOx、MgO、CaO、SrO、BaO、SiO2、HfO2、TiO2、ZrO2、Al2O3、Y2O3、La2O3、稀土氧化物和其混合物，其中x＝1到3。
10.权利要求9的制品，其中CTE控制添加剂以最多50体积％的量存在。
11.权利要求9的制品，其中CTE控制添加剂以10到50体积％的量存在。
12.权利要求9的制品，其中CTE控制添加剂以10到40体积％的量存在。
13.权利要求1的制品，其还包含在基材和阻隔层之间的中间层。
14.权利要求1的制品，其中阻隔层还包含CTE控制添加剂，其中该层的CTE在基材和/或中间层的CTE±3.0ppm/℃范围内。
15.权利要求1的制品，其中阻隔层还包含CTE控制添加剂，其中该层的CTE在基材和/或中间层的CTE±2.0ppm/℃范围内。
16.权利要求1的制品，其中阻隔层还包含CTE控制添加剂，其中该层的CTE在基材和/或中间层的CTE±1ppm/℃范围内。
17.权利要求13的制品，其中中间层选自钡锶铝硅酸盐、锶铝硅酸盐、硅酸钇、富铝红柱石、硅金属、二氧化硅和其混合物。
18.权利要求1的制品，其中阻隔层是在环境阻隔涂层(EBC)体系中，在EBC体系的两个反应性层之间的中间层。
19.权利要求18的制品，其中所述反应性层是硅金属或者二氧化硅和铪和/或氧化锆。
20.权利要求1的制品，其中基材的CTE为含硅酸铪涂层的CTE±3ppm/℃。
21.权利要求20的制品，其中基材选自含硅陶瓷和含硅金属合金。
22.权利要求20的制品，其中基材包括碳化硅、氮化硅、氮氧化硅、硅铝氧氮化物、富铝红柱石、铝硅酸盐、氧化铝和其混合物。
23.权利要求20的制品，其中基材是氧化物/氧化物陶瓷基质复合材料。
24.权利要求1的制品，其还包含在含硅基材上的粘合层。
25.权利要求1的制品，其中阻隔层的厚度在0.1到300密耳之间。
26.权利要求1的制品，其中阻隔层的厚度在0.1到10密耳之间。
27.权利要求1的制品，其中所述涂层通过选自以下的方法产生：热喷涂、化学蒸气沉积、物理蒸汽沉积、电泳沉积、静电沉积、溶胶-凝胶、浆液涂覆、浸渍、气刷、溅射和浆液涂漆。
28.一种用于产生包含硅酸铪的涂层的方法，其包括：
制备包含二氧化铪和硅源的混合物；
将所述混合物等离子喷涂形成涂层；和
在980到1650℃的温度下热处理所述涂层至少0.5小时，形成包含硅酸铪的涂层。
29.权利要求25的方法，其中热处理在1200到1485℃的温度下进行2到200小时的时间。
30.用于产生包含硅酸铪和硅酸锆的至少一种的涂层的方法，其包括：
制备HfO2和ZrO2的至少一种的多层涂层和硅源的层；和
在980到1650℃的温度下热处理所述多层涂层至少0.5小时，形成包含硅酸铪和硅酸锆的至少一种的涂层。
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| CNA2006101061366A Pending CN1935746A (zh) | 2005-09-19 | 2006-07-19 | 具有含铪阻隔层的硅基基材 |
Country Status (7)
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| US (2) | US20070065672A1 (zh) |
| EP (1) | EP1764351A3 (zh) |
| JP (1) | JP2007084421A (zh) |
| KR (1) | KR20070032605A (zh) |
| CN (1) | CN1935746A (zh) |
| IL (1) | IL176249A0 (zh) |
| SG (1) | SG131011A1 (zh) |
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| CN105189932A (zh) * | 2013-03-15 | 2015-12-23 | 通用电气公司 | 抗凹陷陶瓷基体复合物和环境阻隔涂层 |
| CN111233446A (zh) * | 2020-03-12 | 2020-06-05 | 武汉理工大学 | 一种用于陶瓷基复合材料基体的硅酸铪环境障涂层及其制备方法 |
| CN112250476A (zh) * | 2020-10-29 | 2021-01-22 | 昆明理工大学 | 具有高温陶瓷涂层YSZ-RETaO4的SiC基复合材料及其制备方法 |
| CN113784938A (zh) * | 2019-05-03 | 2021-12-10 | 赛峰集团 | 由硅基陶瓷或cmc制成的部件以及生产这种部件的方法 |
| CN115385726A (zh) * | 2022-08-29 | 2022-11-25 | 广东省科学院新材料研究所 | 一种纤维表面抗水氧腐蚀涂层及其制备方法与应用 |
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| DE3827068C1 (zh) * | 1988-08-10 | 1990-03-15 | Degussa Ag, 6000 Frankfurt, De | |
| JPH0789779A (ja) * | 1993-09-20 | 1995-04-04 | Hitachi Ltd | 自己修復機能被覆材およびその製法 |
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| DE10250037B3 (de) * | 2002-10-25 | 2004-05-13 | Forschungszentrum Jülich GmbH | Schutzschichtsystem für nichtoxidische, Si-haltige Substrate und dessen Verwendung |
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-
2005
- 2005-09-19 US US11/230,196 patent/US20070065672A1/en not_active Abandoned
-
2006
- 2006-06-12 IL IL176249A patent/IL176249A0/en unknown
- 2006-07-18 KR KR1020060066924A patent/KR20070032605A/ko active IP Right Grant
- 2006-07-18 EP EP06253746A patent/EP1764351A3/en not_active Withdrawn
- 2006-07-19 JP JP2006196310A patent/JP2007084421A/ja active Pending
- 2006-07-19 CN CNA2006101061366A patent/CN1935746A/zh active Pending
- 2006-08-07 SG SG200605351-6A patent/SG131011A1/en unknown
-
2007
- 2007-01-08 US US11/651,189 patent/US20070111013A1/en not_active Abandoned
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| CN112250476A (zh) * | 2020-10-29 | 2021-01-22 | 昆明理工大学 | 具有高温陶瓷涂层YSZ-RETaO4的SiC基复合材料及其制备方法 |
| CN115385726A (zh) * | 2022-08-29 | 2022-11-25 | 广东省科学院新材料研究所 | 一种纤维表面抗水氧腐蚀涂层及其制备方法与应用 |
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Also Published As
| Publication number | Publication date |
|---|---|
| EP1764351A3 (en) | 2010-03-17 |
| EP1764351A2 (en) | 2007-03-21 |
| SG131011A1 (en) | 2007-04-26 |
| JP2007084421A (ja) | 2007-04-05 |
| US20070111013A1 (en) | 2007-05-17 |
| KR20070032605A (ko) | 2007-03-22 |
| US20070065672A1 (en) | 2007-03-22 |
| IL176249A0 (en) | 2006-10-05 |
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