US3796588A - Process for rendering a steel piece superficially hard and corrosion resistive,piece obtained by the carrying out of this process and use of the latter - Google Patents
Process for rendering a steel piece superficially hard and corrosion resistive,piece obtained by the carrying out of this process and use of the latter Download PDFInfo
- Publication number
- US3796588A US3796588A US00184628A US3796588DA US3796588A US 3796588 A US3796588 A US 3796588A US 00184628 A US00184628 A US 00184628A US 3796588D A US3796588D A US 3796588DA US 3796588 A US3796588 A US 3796588A
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- United States
- Prior art keywords
- layer
- chromium
- piece
- metal
- carbide
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired - Lifetime
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- 238000000034 method Methods 0.000 title abstract description 15
- 238000009877 rendering Methods 0.000 title abstract description 4
- 229910000831 Steel Inorganic materials 0.000 title description 19
- 239000010959 steel Substances 0.000 title description 19
- 238000005260 corrosion Methods 0.000 title description 7
- 230000007797 corrosion Effects 0.000 title description 7
- 239000011651 chromium Substances 0.000 abstract description 29
- 229910052804 chromium Inorganic materials 0.000 abstract description 25
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 abstract description 18
- 229910052751 metal Inorganic materials 0.000 abstract description 18
- 239000002184 metal Substances 0.000 abstract description 18
- MTPVUVINMAGMJL-UHFFFAOYSA-N trimethyl(1,1,2,2,2-pentafluoroethyl)silane Chemical compound C[Si](C)(C)C(F)(F)C(F)(F)F MTPVUVINMAGMJL-UHFFFAOYSA-N 0.000 abstract description 14
- -1 CHROMIUM HALIDE Chemical class 0.000 abstract description 9
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 abstract description 7
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 abstract description 5
- 239000010953 base metal Substances 0.000 abstract description 5
- 150000004767 nitrides Chemical class 0.000 abstract description 5
- 229910021332 silicide Inorganic materials 0.000 abstract description 5
- FVBUAEGBCNSCDD-UHFFFAOYSA-N silicide(4-) Chemical compound [Si-4] FVBUAEGBCNSCDD-UHFFFAOYSA-N 0.000 abstract description 5
- 229930195733 hydrocarbon Natural products 0.000 abstract description 3
- 150000002430 hydrocarbons Chemical class 0.000 abstract description 3
- 239000006185 dispersion Substances 0.000 abstract description 2
- 239000003870 refractory metal Substances 0.000 abstract description 2
- XJDNKRIXUMDJCW-UHFFFAOYSA-J titanium tetrachloride Chemical compound Cl[Ti](Cl)(Cl)Cl XJDNKRIXUMDJCW-UHFFFAOYSA-J 0.000 abstract description 2
- 239000010410 layer Substances 0.000 description 39
- 239000000758 substrate Substances 0.000 description 9
- 239000000463 material Substances 0.000 description 7
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 5
- 238000006243 chemical reaction Methods 0.000 description 5
- 230000008021 deposition Effects 0.000 description 5
- 239000000047 product Substances 0.000 description 5
- 239000003638 chemical reducing agent Substances 0.000 description 4
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 4
- 229910052715 tantalum Inorganic materials 0.000 description 4
- NRTOMJZYCJJWKI-UHFFFAOYSA-N Titanium nitride Chemical compound [Ti]#N NRTOMJZYCJJWKI-UHFFFAOYSA-N 0.000 description 3
- 229910052782 aluminium Inorganic materials 0.000 description 3
- 239000000460 chlorine Substances 0.000 description 3
- UFGZSIPAQKLCGR-UHFFFAOYSA-N chromium carbide Chemical compound [Cr]#C[Cr]C#[Cr] UFGZSIPAQKLCGR-UHFFFAOYSA-N 0.000 description 3
- QSWDMMVNRMROPK-UHFFFAOYSA-K chromium(3+) trichloride Chemical compound [Cl-].[Cl-].[Cl-].[Cr+3] QSWDMMVNRMROPK-UHFFFAOYSA-K 0.000 description 3
- 239000007789 gas Substances 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- 239000001257 hydrogen Substances 0.000 description 3
- 239000000203 mixture Substances 0.000 description 3
- 229910052759 nickel Inorganic materials 0.000 description 3
- 229910052710 silicon Inorganic materials 0.000 description 3
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 3
- 229910003470 tongbaite Inorganic materials 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 229910000975 Carbon steel Inorganic materials 0.000 description 2
- 229910021556 Chromium(III) chloride Inorganic materials 0.000 description 2
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 2
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 2
- 229910001566 austenite Inorganic materials 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 229960000359 chromic chloride Drugs 0.000 description 2
- 238000009792 diffusion process Methods 0.000 description 2
- 239000010703 silicon Substances 0.000 description 2
- 239000002344 surface layer Substances 0.000 description 2
- 229910000859 α-Fe Inorganic materials 0.000 description 2
- HECLRDQVFMWTQS-RGOKHQFPSA-N 1755-01-7 Chemical compound C1[C@H]2[C@@H]3CC=C[C@@H]3[C@@H]1C=C2 HECLRDQVFMWTQS-RGOKHQFPSA-N 0.000 description 1
- KZBUYRJDOAKODT-UHFFFAOYSA-N Chlorine Chemical compound ClCl KZBUYRJDOAKODT-UHFFFAOYSA-N 0.000 description 1
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- 229910021555 Chromium Chloride Inorganic materials 0.000 description 1
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 1
- 239000005977 Ethylene Substances 0.000 description 1
- 102000010029 Homer Scaffolding Proteins Human genes 0.000 description 1
- 108010077223 Homer Scaffolding Proteins Proteins 0.000 description 1
- 240000005893 Pteridium aquilinum Species 0.000 description 1
- 235000009936 Pteridium aquilinum Nutrition 0.000 description 1
- 208000036366 Sensation of pressure Diseases 0.000 description 1
- HSFWRNGVRCDJHI-UHFFFAOYSA-N alpha-acetylene Natural products C#C HSFWRNGVRCDJHI-UHFFFAOYSA-N 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- QDWJUBJKEHXSMT-UHFFFAOYSA-N boranylidynenickel Chemical compound [Ni]#B QDWJUBJKEHXSMT-UHFFFAOYSA-N 0.000 description 1
- 239000010962 carbon steel Substances 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 235000019642 color hue Nutrition 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 125000002534 ethynyl group Chemical group [H]C#C* 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000008246 gaseous mixture Substances 0.000 description 1
- 150000004687 hexahydrates Chemical class 0.000 description 1
- 229910001026 inconel Inorganic materials 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- NFFIWVVINABMKP-UHFFFAOYSA-N methylidynetantalum Chemical compound [Ta]#C NFFIWVVINABMKP-UHFFFAOYSA-N 0.000 description 1
- 229910052750 molybdenum Inorganic materials 0.000 description 1
- 229910052758 niobium Inorganic materials 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- 238000007747 plating Methods 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 230000001681 protective effect Effects 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 239000007858 starting material Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 229910003468 tantalcarbide Inorganic materials 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 150000003609 titanium compounds Chemical class 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
Classifications
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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
- 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
- C23C28/30—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer
- C23C28/36—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including layers graded in composition or physical properties
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- C—CHEMISTRY; METALLURGY
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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
- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/22—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the deposition of inorganic material, other than metallic material
- C23C16/30—Deposition of compounds, mixtures or solid solutions, e.g. borides, carbides, nitrides
- C23C16/32—Carbides
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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
- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/22—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the deposition of inorganic material, other than metallic material
- C23C16/30—Deposition of compounds, mixtures or solid solutions, e.g. borides, carbides, nitrides
- C23C16/34—Nitrides
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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
- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/22—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the deposition of inorganic material, other than metallic material
- C23C16/30—Deposition of compounds, mixtures or solid solutions, e.g. borides, carbides, nitrides
- C23C16/36—Carbonitrides
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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
- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/22—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the deposition of inorganic material, other than metallic material
- C23C16/30—Deposition of compounds, mixtures or solid solutions, e.g. borides, carbides, nitrides
- C23C16/38—Borides
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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
- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/22—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the deposition of inorganic material, other than metallic material
- C23C16/30—Deposition of compounds, mixtures or solid solutions, e.g. borides, carbides, nitrides
- C23C16/40—Oxides
- C23C16/403—Oxides of aluminium, magnesium or beryllium
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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
- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/22—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the deposition of inorganic material, other than metallic material
- C23C16/30—Deposition of compounds, mixtures or solid solutions, e.g. borides, carbides, nitrides
- C23C16/42—Silicides
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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
- 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
- C23C28/30—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer
- C23C28/32—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one pure metallic layer
- C23C28/322—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one pure metallic layer only coatings of metal elements only
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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
- 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
- C23C28/30—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer
- C23C28/32—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one pure metallic layer
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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
- 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
- C23C28/30—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer
- C23C28/34—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates
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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
- 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
- C23C28/30—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer
- C23C28/34—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates
- C23C28/341—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates with at least one carbide layer
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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
- 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
- C23C28/30—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer
- C23C28/34—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates
- C23C28/345—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates with at least one oxide layer
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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
- C23C28/30—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer
- C23C28/34—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates
- C23C28/347—Coatings combining at least one metallic layer and at least one inorganic non-metallic layer including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates with layers adapted for cutting tools or wear applications
-
- G—PHYSICS
- G04—HOROLOGY
- G04B—MECHANICALLY-DRIVEN CLOCKS OR WATCHES; MECHANICAL PARTS OF CLOCKS OR WATCHES IN GENERAL; TIME PIECES USING THE POSITION OF THE SUN, MOON OR STARS
- G04B37/00—Cases
- G04B37/22—Materials or processes of manufacturing pocket watch or wrist watch cases
- G04B37/223—Materials or processes of manufacturing pocket watch or wrist watch cases metallic cases coated with a nonmetallic layer
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10S428/00—Stock material or miscellaneous articles
- Y10S428/922—Static electricity metal bleed-off metallic stock
- Y10S428/9335—Product by special process
- Y10S428/938—Vapor deposition or gas diffusion
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/12—All metal or with adjacent metals
- Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
- Y10T428/12535—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.] with additional, spatially distinct nonmetal component
- Y10T428/12583—Component contains compound of adjacent metal
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/12—All metal or with adjacent metals
- Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
- Y10T428/12535—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.] with additional, spatially distinct nonmetal component
- Y10T428/12611—Oxide-containing component
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/12—All metal or with adjacent metals
- Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
- Y10T428/12674—Ge- or Si-base component
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/12—All metal or with adjacent metals
- Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
- Y10T428/12736—Al-base component
- Y10T428/1275—Next to Group VIII or IB metal-base component
- Y10T428/12757—Fe
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/12—All metal or with adjacent metals
- Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
- Y10T428/12771—Transition metal-base component
- Y10T428/12778—Alternative base metals from diverse categories
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/12—All metal or with adjacent metals
- Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
- Y10T428/12771—Transition metal-base component
- Y10T428/12806—Refractory [Group IVB, VB, or VIB] metal-base component
- Y10T428/12826—Group VIB metal-base component
- Y10T428/12847—Cr-base component
- Y10T428/12854—Next to Co-, Fe-, or Ni-base component
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
- Y10T428/12—All metal or with adjacent metals
- Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
- Y10T428/12771—Transition metal-base component
- Y10T428/12861—Group VIII or IB metal-base component
- Y10T428/12951—Fe-base component
- Y10T428/12972—Containing 0.01-1.7% carbon [i.e., steel]
Definitions
- the present invention concerns a process for rendering a steel piece superficially hard and corrosion resistant; it also concerns the piece obtained by the carrying out of this process and the use of the latter.
- the object of the present invention is to remedy this drawback and to provide a process for simultaneously hardening such steels and make them corrosion resistant.
- the process of the invention is characterized by the fact that an intermediate or first layer of at least one passive metal is applied onto the steel piece, said layer difiusing at least partially into the base metal, and that a hardening layer consisting of a metal carbide, nitride, boride, or silicide is thereafter applied chemically in the gas-phase.
- passive metal is utilized as defining a metal characterized by resistance to corrosion-socalled passivity to chemical attack-and is to be interpreted as such when reference is made thereto throughout the specification and in the claims.
- the piece obtained by the carrying out of this process is characterized by the fact that it is made of a steel base coated with an intermediate or first layer of a passive metal diifusing at least partially into the base metal, this layer being itself coated with a hardening layer consisting of a metal carbide, nitride or silicide.
- the above mentioned first layer of at least one passive metal is deposited, as is the hardening layer, in the gas-phase.
- the metal used can be chromium, tantalum, aluminum, silicon and nickel, the latter being only considered, however, when the second or hardening layer 3,796,588 Patented Mar. 12,, 1974 does not consist of titanium carbide.
- chromium experiments have shown that the metal deposited forms, together with the carbon of the steel, chromium carbides which fit particularly well, in a carbide containing base, for the subsequent deposition of the titanium carbide hardening layer.
- the starting material is a chromium halide, for instance chromium trichloride known in the trade under the name of CrCl Hexahydrate, written CrCl in Equations I and II for simplification, but which comprises actually chromium halides corresponding to numbers 2 and 3 of the chromium valences.
- the reducing agent of reaction I is hydrogen which is progressively added to the chromium halide, whereas in Equation 11, the reducing agent, which is generally identical with the base metal, is iron.
- the chromium layer which forms on the surface of the sample diffuses partially or entirely into it.
- Deposition temperatures will be preferentially above 800 C. for having a high enough chromium chloride pressure.
- austenite steels or steels containing elements taking part to the formation of the austenite phase e.g. Ni, Mn, Cu and N, the diffusion is strongly decreased.
- Gaseous 'HCl can also be reacted with Cr metal to form CrCl which will be reduced thereafter to a layer of Cr metal.
- a :1 to 20:1 mixture of argon and HCl is reacted, at a temperature above 800 C. (preferentially at 850 C.) on granulated or pulverized chromium evenly dispersed in a container entirely made of alumina.
- the equilibrium reaction I applies there, but in the opposite direction.
- the mixture obtained above, Cr/Ar/H /remainder of HCl is allowed to react with the substrate, either directly or diluted with H
- Large volumes of gas under atmospheric or reduced pres sure (preferentially 50 to 100 torr) are used for eliminating, as quickly as possible, the gaseous products which are normally HCl and FeCl;.
- the first layer with several metals, e.g. by the deposition of a first layer of Si and a second with Cr.
- the final hardening coating that is the second layer, which is known as well as the methods for obtaining it,
- titanium carbide a titanium compound such as TiCl is progressively evaporated from an evaporator for liquids and continuously added to a gaseous flow of hydrocarbons.
- a titanium compound such as TiCl is progressively evaporated from an evaporator for liquids and continuously added to a gaseous flow of hydrocarbons.
- hydrocarbons such as methane, acetylene or ethylene, which are added in their normal gaseous state, and dicyclopentadiene which must be vaporized beforehand.
- a 1:1:100 to 5:5 :100 gaseous mixture of CH TiCl and H can be used on the base-material in an Inconel reactor, avoiding carefully all iron parts.
- the said second layer can also be made of an alumina layer or, further, of a composite layer, e.g. of chromium carbide and titanium carbide or of titanium carbide and nitride for having color hues varying from golden to silvered.
- a composite layer e.g. of chromium carbide and titanium carbide or of titanium carbide and nitride for having color hues varying from golden to silvered.
- the present process permits obtaining any hard and corrosion resistant pieces, particularly Watch-case elements such as middle parts, bezels, protective caps for middle parts, bezels, etc.
- a watch element comprising a shaped steel substrate having (an at least partially diffused) a gas-phase chemically deposited chromium sulface layer (of at least one corrosion resistant material having metallic characteristics selected from the group consisting of chromium, tantalum, aluminum, silicon, and nickel) at least partially diffused into said steel substrate, and a gas-phase chemically deposited second layer (formed on said first layer) on said chromium layer, said second layer (selected from the .4 group consisting of titanium carbide, titanium nitride, a mixture of titanium carbide and titanium nitride, chromium carbide, tantalum carbide, nickel boride and aluminum oxide) comprising titanium carbide.
- a watch element comprising a shaped steel substrate having-a gas-phase chemically deposited chromium surface layer at least partially diffused into said steel substrate, and a gas-phase chemically deposited second layer on said chromium layer, said second layer comprising titanium carbide.
- a watch element comprising a shaped steel substrate having a gas-phase chemically deposited chromium. surface layer at least partially diffused into said steel substrate, and a gas-phase chemically deposited second layer on said chromium layer, said second layer comprising titanium carbide.
Landscapes
- Chemical & Material Sciences (AREA)
- Inorganic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Materials Engineering (AREA)
- Mechanical Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Physics & Mathematics (AREA)
- General Physics & Mathematics (AREA)
- Chemical Vapour Deposition (AREA)
- Physical Vapour Deposition (AREA)
- Solid-Phase Diffusion Into Metallic Material Surfaces (AREA)
- Heat Treatment Of Articles (AREA)
- Preliminary Treatment Of Fibers (AREA)
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CH1466870A CH600407B5 (da) | 1970-10-02 | 1970-10-02 |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| US3796588A true US3796588A (en) | 1974-03-12 |
Family
ID=4402852
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| US00184628A Expired - Lifetime US3796588A (en) | 1970-10-02 | 1971-09-28 | Process for rendering a steel piece superficially hard and corrosion resistive,piece obtained by the carrying out of this process and use of the latter |
Country Status (16)
| Country | Link |
|---|---|
| US (1) | US3796588A (da) |
| JP (2) | JPS5411779B1 (da) |
| AT (1) | AT313018B (da) |
| AU (1) | AU3412371A (da) |
| BE (1) | BE773421A (da) |
| BR (1) | BR7106533D0 (da) |
| CA (1) | CA956216A (da) |
| CH (2) | CH600407B5 (da) |
| DE (1) | DE2149294C3 (da) |
| ES (1) | ES395606A1 (da) |
| FR (1) | FR2110202B1 (da) |
| GB (1) | GB1361427A (da) |
| IL (1) | IL37832A0 (da) |
| IT (1) | IT961073B (da) |
| NL (1) | NL7113545A (da) |
| ZA (1) | ZA716596B (da) |
Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3951612A (en) * | 1974-11-12 | 1976-04-20 | Aerospace Materials Inc. | Erosion resistant coatings |
| US3953178A (en) * | 1972-08-09 | 1976-04-27 | Engel Niels N | Coated metal product |
| JPS5165037A (ja) * | 1974-12-03 | 1976-06-05 | Seiko Instr & Electronics | Tokeibuhin |
| WO1986002290A1 (en) * | 1984-10-17 | 1986-04-24 | Sri International | Process for applying coatings to metals and resulting product |
| US5217817A (en) * | 1989-11-08 | 1993-06-08 | U.S. Philips Corporation | Steel tool provided with a boron layer |
| US20070025188A1 (en) * | 2001-02-28 | 2007-02-01 | Frederic Leuba | Use of non-magnetic coating for covering components in a clock movement |
| EP2836621A4 (en) * | 2012-04-11 | 2015-11-18 | Ihi Ionbond Inc | CERAMIC CLOTHING FOR A FIREARM RUN |
| WO2024138594A1 (zh) * | 2022-12-28 | 2024-07-04 | 无锡透平叶片有限公司 | 一种镍基高温合金表面化学气相沉积AlCr涂层方法 |
Families Citing this family (14)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| IT1123082B (it) * | 1975-11-14 | 1986-04-30 | Fulmer Res Inst Ltd | Matrice migliorata per dare forma a metallo,costituita da un substrato d'acciaio rivestito di uno strato contenente fosfuro di nichel,metodo per la sua preparazione e suo impiego per l'estrusione di alluminio |
| CH640885A5 (de) * | 1978-07-21 | 1984-01-31 | Suisse Horlogerie Rech Lab | Mit einem harten ueberzug versehene maschinenelemente. |
| FR2451949A1 (fr) * | 1979-03-22 | 1980-10-17 | Nl Vintage | Procede pour revetir des objets d'une surface en matiere dure que l'on puisse exploiter commercialement et objets fabriques par ce procede |
| US4278708A (en) * | 1979-10-31 | 1981-07-14 | Ford Motor Company | Conductive corrosion resistant material and alkali metal/polysulfide battery employing same |
| CH643421B (fr) * | 1980-04-10 | Asu Composants Sa | Procede de depot d'un revetement dur d'un compose d'or, cible de depot pour un tel procede et piece de joaillerie comportant un tel revetement. | |
| DE3318999A1 (de) * | 1983-05-25 | 1984-11-29 | M.A.N. Maschinenfabrik Augsburg-Nürnberg AG, 8000 München | Beschichteter metallischer gegenstand sowie verfahren zu dessen herstellung |
| US5514482A (en) * | 1984-04-25 | 1996-05-07 | Alliedsignal Inc. | Thermal barrier coating system for superalloy components |
| EP0186266A1 (en) * | 1984-11-19 | 1986-07-02 | Avco Corporation | Erosion-resistant coating system |
| EP0188057A1 (en) * | 1984-11-19 | 1986-07-23 | Avco Corporation | Erosion resistant coatings |
| FR2579997A1 (fr) * | 1985-04-03 | 1986-10-10 | Preci Coat Sa | Procede de traitment de surface d'un objet et objet obtenu par ce procede |
| GB2285632B (en) * | 1985-08-19 | 1996-02-14 | Garrett Corp | Thermal barrier coating system for superalloy components |
| NL8902760A (nl) * | 1989-11-08 | 1991-06-03 | Philips Nv | Werkwijze voor het aanbrengen van een boorlaag op een stalen substraat en gereedschap voorzien van een boorlaag. |
| EP0616050B1 (de) * | 1993-03-16 | 1997-08-13 | Balzers Aktiengesellschaft | Verfahren zur Standzeiterhöhung von Werkzeugen und Verschleissschutz-beschichtetes Werkzeug |
| JP3203256B2 (ja) * | 1996-01-31 | 2001-08-27 | 日本板硝子株式会社 | 光モジュールおよびその製造方法 |
-
1970
- 1970-10-02 CH CH1466870A patent/CH600407B5/xx not_active IP Right Cessation
- 1970-10-02 CH CH1466870D patent/CH1466870A4/xx unknown
-
1971
- 1971-09-28 US US00184628A patent/US3796588A/en not_active Expired - Lifetime
- 1971-09-29 DE DE2149294A patent/DE2149294C3/de not_active Expired
- 1971-09-30 ES ES395606A patent/ES395606A1/es not_active Expired
- 1971-10-01 GB GB4577871A patent/GB1361427A/en not_active Expired
- 1971-10-01 NL NL7113545A patent/NL7113545A/xx unknown
- 1971-10-01 BE BE773421A patent/BE773421A/xx unknown
- 1971-10-01 IT IT53219/71A patent/IT961073B/it active
- 1971-10-01 AT AT850971A patent/AT313018B/de not_active IP Right Cessation
- 1971-10-01 FR FR7136863A patent/FR2110202B1/fr not_active Expired
- 1971-10-01 AU AU34123/71A patent/AU3412371A/en not_active Expired
- 1971-10-01 IL IL37832A patent/IL37832A0/xx unknown
- 1971-10-01 BR BR6533/71A patent/BR7106533D0/pt unknown
- 1971-10-01 ZA ZA716596A patent/ZA716596B/xx unknown
- 1971-10-01 CA CA124,239A patent/CA956216A/en not_active Expired
- 1971-10-02 JP JP7745271A patent/JPS5411779B1/ja active Pending
-
1978
- 1978-10-17 JP JP12776578A patent/JPS5474286A/ja active Pending
Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3953178A (en) * | 1972-08-09 | 1976-04-27 | Engel Niels N | Coated metal product |
| US3951612A (en) * | 1974-11-12 | 1976-04-20 | Aerospace Materials Inc. | Erosion resistant coatings |
| JPS5165037A (ja) * | 1974-12-03 | 1976-06-05 | Seiko Instr & Electronics | Tokeibuhin |
| JPS5512551B2 (da) * | 1974-12-03 | 1980-04-02 | ||
| WO1986002290A1 (en) * | 1984-10-17 | 1986-04-24 | Sri International | Process for applying coatings to metals and resulting product |
| GB2178449A (en) * | 1984-10-17 | 1987-02-11 | Stanford Res Inst Int | Process for applying coatings to metals and resulting product |
| US5217817A (en) * | 1989-11-08 | 1993-06-08 | U.S. Philips Corporation | Steel tool provided with a boron layer |
| US20070025188A1 (en) * | 2001-02-28 | 2007-02-01 | Frederic Leuba | Use of non-magnetic coating for covering components in a clock movement |
| EP2836621A4 (en) * | 2012-04-11 | 2015-11-18 | Ihi Ionbond Inc | CERAMIC CLOTHING FOR A FIREARM RUN |
| WO2024138594A1 (zh) * | 2022-12-28 | 2024-07-04 | 无锡透平叶片有限公司 | 一种镍基高温合金表面化学气相沉积AlCr涂层方法 |
Also Published As
| Publication number | Publication date |
|---|---|
| DE2149294B2 (de) | 1975-02-20 |
| AT313018B (de) | 1974-01-25 |
| DE2149294A1 (de) | 1972-04-06 |
| JPS5411779B1 (da) | 1979-05-17 |
| BR7106533D0 (pt) | 1973-01-02 |
| ZA716596B (en) | 1972-08-30 |
| GB1361427A (da) | 1974-07-24 |
| IT961073B (it) | 1973-12-10 |
| IL37832A0 (en) | 1971-12-29 |
| AU3412371A (en) | 1973-04-05 |
| FR2110202B1 (da) | 1976-02-13 |
| CA956216A (en) | 1974-10-15 |
| DE2149294C3 (de) | 1975-09-25 |
| CH1466870A4 (da) | 1977-08-15 |
| FR2110202A1 (da) | 1972-06-02 |
| CH600407B5 (da) | 1978-06-15 |
| NL7113545A (da) | 1972-04-05 |
| BE773421A (fr) | 1972-01-31 |
| JPS5474286A (en) | 1979-06-14 |
| ES395606A1 (es) | 1973-11-01 |
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