WO2022062102A1 - Matériau de revêtement en alliage à haute entropie résistant à la diffusion, matériau de revêtement résistant à la chaleur, son procédé de préparation et application correspondante - Google Patents

Matériau de revêtement en alliage à haute entropie résistant à la diffusion, matériau de revêtement résistant à la chaleur, son procédé de préparation et application correspondante Download PDF

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WO2022062102A1
WO2022062102A1 PCT/CN2020/127792 CN2020127792W WO2022062102A1 WO 2022062102 A1 WO2022062102 A1 WO 2022062102A1 CN 2020127792 W CN2020127792 W CN 2020127792W WO 2022062102 A1 WO2022062102 A1 WO 2022062102A1
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diffusion
coating
entropy alloy
alloy coating
resistant
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PCT/CN2020/127792
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English (en)
Chinese (zh)
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汪唯
许中湛
王磊
洪悦
石倩
林松盛
郭朝乾
唐鹏
苏一凡
代明江
王红莉
唐春梅
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广东省科学院新材料研究所
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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
    • C23C28/02—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 only including layers of metallic material
    • C23C28/021—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 only including layers of metallic material including at least one metal alloy layer
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C30/00—Alloys containing less than 50% by weight of each constituent
    • 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
    • C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
    • C23C14/06—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the coating material
    • C23C14/14—Metallic material, boron or silicon
    • C23C14/16—Metallic material, boron or silicon on metallic substrates or on substrates of boron or silicon
    • 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
    • C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
    • C23C14/06—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the coating material
    • C23C14/14—Metallic material, boron or silicon
    • C23C14/16—Metallic material, boron or silicon on metallic substrates or on substrates of boron or silicon
    • C23C14/165—Metallic material, boron or silicon on metallic substrates or on substrates of boron or silicon by cathodic sputtering
    • 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
    • C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
    • C23C14/22—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the process of coating
    • C23C14/24—Vacuum evaporation
    • C23C14/32—Vacuum evaporation by explosion; by evaporation and subsequent ionisation of the vapours, e.g. ion-plating
    • C23C14/325—Electric arc evaporation
    • 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
    • C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
    • C23C14/22—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the process of coating
    • C23C14/34—Sputtering
    • C23C14/35—Sputtering by application of a magnetic field, e.g. magnetron sputtering

Definitions

  • the present disclosure relates to the technical field of coating preparation, and in particular, to diffusion-resistant high-entropy alloy coating materials, high-temperature resistant coating materials, and preparation methods and applications thereof.
  • diffusion barrier is considered to be one of the most direct and effective methods. It usually adds a barrier layer (ie diffusion barrier) between the coating and the substrate to block the interdiffusion between elements.
  • the diffusion barrier materials are mainly metals (precious metals or refractory metals) and ceramics, but the metal diffusion barrier has the problem of poor chemical matching with the coating/substrate, and its blocking effect is not good when multiple elements are interdiffused at the same time.
  • the ceramic layer diffusion barrier has the problem of poor physical matching with the substrate, and is prone to thermal shock failure. It can be seen that the good physical and chemical matching between the diffusion barrier and the substrate is the key problem to be solved urgently in the current diffusion barrier research process.
  • Embodiments of the present disclosure propose a diffusion-resistant high-entropy alloy coating material, which includes a substrate and a diffusion-resistant high-entropy alloy coating, and elements of the diffusion-resistant high-entropy alloy coating include Al, Co, Cr, Ni, and Mo.
  • the elements of the diffusion barrier high-entropy alloy coating include Al 15%-30%, Co 15%-30%, Cr 15%-30%, Ni 15%-30% and Mo 15%-30%.
  • the ratio of Al, Co, Cr, Ni and Mo in the diffusion-resistant high-entropy alloy coating is 1:1:1:1:1 by atomic percentage.
  • the ratio of Al, Co, Cr, Ni and Mo in the diffusion-resistant high-entropy alloy coating is 1.1:1.1:1.1:1.1:0.6 in atomic percentage.
  • the ratio of Al, Co, Cr, Ni and Mo in the diffusion-resistant high-entropy alloy coating is 1.1:1.1:1:1:0.8 in atomic percentage.
  • the ratio of Al, Co, Cr, Ni and Mo in the diffusion-resistant high-entropy alloy coating is 1:1.5:0.75:1:0.75 in atomic percentage.
  • the ratio of Al, Co, Cr, Ni and Mo in the diffusion-resistant high-entropy alloy coating is 0.9:0.9:1:1:1.2 in atomic percentage.
  • the ratio of Al, Co, Cr, Ni and Mo in the diffusion-resistant high-entropy alloy coating is 0.8:1.1:0.9:1.2:1 by atomic percentage.
  • the base material is a superalloy.
  • the base material is an iron-based superalloy, a nickel-based superalloy or a cobalt-based superalloy.
  • Embodiments of the present disclosure also provide a preparation method for preparing a diffusion-resistant high-entropy alloy coating material, including: forming a diffusion-resistant high-entropy alloy coating on the surface of the substrate.
  • the forming of the diffusion-resistant high-entropy alloy coating on the surface of the substrate includes preparing Al, Co, Cr, Ni and Mo into a single alloy target, and then magnetron sputtering the single alloy target.
  • the diffusion-resistant high-entropy alloy coating is formed on the surface of the substrate by means of radiation or arc ion plating.
  • the single alloy target is prepared by smelting or powder metallurgy.
  • the thickness of the diffusion-resistant high-entropy alloy coating is 2 ⁇ m-8 ⁇ m, preferably 2 ⁇ m-7 ⁇ m, more preferably 2 ⁇ m-6 ⁇ m, more preferably 2 ⁇ m-5 ⁇ m, and more preferably 2 ⁇ m-4 ⁇ m.
  • the diffusion-resistant high-entropy alloy coating is formed by means of magnetron sputtering, it is performed under the conditions that the background vacuum degree is less than or equal to 5 ⁇ 10 -3 Pa and the substrate temperature is 100-300°C;
  • the target power is 200-300W
  • the DC bias of the substrate is -100--500V
  • the duty cycle is 60-90%
  • the target-base distance is 10-15cm
  • the working argon gas pressure is 0.6-0.8Pa
  • the ion source is 0.8 -1.2A.
  • the diffusion-resistant high-entropy alloy coating when forming the diffusion-resistant high-entropy alloy coating by means of arc ion plating, it is performed under the conditions that the background vacuum degree is less than or equal to 5 ⁇ 10 -3 Pa and the substrate temperature is 200-400°C; preferably ground, the target current is 70-90A, the substrate DC bias is -100--500V, the duty cycle is 60-90%, the target-base distance is 20-30cm, the working argon gas pressure is 1-1.3Pa, and the permanent magnet strength is 1500- 2000Gs, solenoid voltage 20-30V.
  • the preparation method of the diffusion-resistant high-entropy alloy coating material further comprises: pre-processing the substrate, the pre-treatment The treatment includes grinding and polishing the surface of the substrate, then ultrasonic cleaning with acetone, alcohol and deionized water, respectively, and drying.
  • Embodiments of the present disclosure also provide a high temperature resistant coating material, comprising a material body and a high temperature resistant coating applied on the material body, wherein the material body is the above-mentioned diffusion-resistant high-entropy alloy coating material or the above-mentioned diffusion-resistant high-entropy alloy coating material.
  • the anti-diffusion high-entropy alloy coating material obtained by the preparation method of the entropy alloy coating material.
  • the high temperature resistant coating is PtAl coating, NiAl coating, NiAlHf coating, NiCrAlY coating, CoCrAlY coating, NiAlPtNb coating, NiAlHfRu coating, CoCrAlYSi coating, NiCoCrAlYTa coating, NiCrAlYLaB coating , any one of NiCoCrAlYHf coating and NiCoCrAlYTaRe coating.
  • Embodiments of the present disclosure also provide a method for preparing a high temperature resistant coating material, which includes preparing a high temperature resistant coating on the surface of the material body.
  • the method for preparing the high temperature resistant coating is selected from magnetron sputtering, electron beam physical vapor deposition, arc ion plating, flame spraying, atmospheric plasma spraying, vacuum plasma spraying, cold spraying, plasma spraying-physical vapor deposition and at least one of pulse plating.
  • the embodiments of the present disclosure also propose the application of the above-mentioned high-temperature resistant coating material or the high-temperature resistant coating material obtained by the above-mentioned preparation method of the above-mentioned high temperature resistant coating material in the preparation of aero-engine or gas turbine hot-end components.
  • Fig. 1 is AlCoCrNiMo high-entropy alloy coating scanning electron microscope (SEM) cross-sectional topography and X-ray diffraction pattern in this embodiment;
  • Figure 2 shows the cross-sectional morphologies of the high-temperature coating (NiAlHf)/diffusion barrier (AlCoCrNiMo)/superalloy (N5) sample in the example after being oxidized at 1100°C for 0h and 50h;
  • Figure 3 shows the cross-sectional morphologies of the NiAlHf/N5 sample in the comparative example after being oxidized at 1100 °C for 0 h and 50 h;
  • Fig. 4 is the oxidation weight gain curve of NiAlHf/AlCoCrNiMo/N5 sample (NCN) and NiAlHf/N5 sample (NN) under the condition of 1100 °C in the embodiment;
  • Figure 5 shows the cross-sectional morphologies of the NiAlHf/AlTiCrNiMo/N5 samples in the comparative example after being oxidized at 1100 °C for 0 h and 50 h.
  • the beneficial effects of the diffusion-resistant high-entropy alloy coating material and the preparation method thereof provided by the embodiments of the present disclosure are: the diffusion-resistant high-entropy alloy coating is formed by using Al, Co, Cr, Ni, and Mo, and the diffusion-resistant high-entropy alloy coating is formed by using Al, Co, Cr, Ni and Mo.
  • the coating has good physical and chemical matching with the substrate and other coatings (such as high temperature coatings), which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high temperature resistance of the coating. Oxidation ability, and at the same time avoid mutual diffusion to reduce the mechanical properties of the substrate, prolong the service life of the parts, and its diffusion resistance effect is significantly improved compared with traditional metal or ceramic diffusion resistance materials.
  • the embodiments of the present disclosure also provide a high temperature resistant coating material and a preparation method thereof.
  • a high temperature resistant coating material By forming the above-mentioned anti-diffusion high-entropy alloy coating on a substrate, and then using this as a material body to form a high-temperature resistant coating, using the high-entropy anti-diffusion alloy coating
  • the alloy coating has a unique slow diffusion effect, and has good physical and chemical matching with the substrate and the high temperature resistant coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, improve the coating performance.
  • high temperature oxidation resistance The high temperature resistant coating material can be used in the preparation of aero-engine or gas turbine hot-end components, so as to improve the service life and working reliability of the components.
  • Embodiments of the present disclosure provide a method for preparing a high temperature resistant coating material, which comprises first forming a diffusion-resistant high-entropy alloy coating on a substrate, and using this as a material body to form a high temperature resistant coating thereon, so as to obtain a High temperature resistant coating material. details as follows:
  • a diffusion-resistant high-entropy alloy coating is formed on the surface of the substrate, and the elements of the diffusion-resistant high-entropy alloy coating include Al, Co, Cr, Ni and Mo.
  • the present disclosure finds that the diffusion-resistant high-entropy alloy coating formed by the above five elements can effectively inhibit the interdiffusion of alloy components and the precipitation of harmful phases at the interface between the substrate and other coatings (especially high-temperature coatings), and improve the high-temperature resistance of the coating. Oxidation ability, while avoiding interdiffusion to reduce the mechanical properties of the substrate and prolong the service life of the parts. If the elements are replaced, such as replacing Co with Ti, such a good diffusion resistance effect cannot be achieved at all.
  • the elements of the diffusion-resistant high-entropy alloy coating include Al 15%-30%, Co 15%-30%, Cr 15%-30%, Ni 15%-30% and Mo 15%- 30%.
  • the amount of elements in the high-entropy alloy is about the same amount.
  • the inventors of the present disclosure further control the amount of each component, so that the formation of the diffusion-resistant high-entropy alloy coating can be a single-phase solid solution or an amorphous phase structure to ensure the diffusion barrier composition.
  • the structure is uniform, and there is no component segregation or precipitation phase, which is beneficial to the diffusion resistance of elements.
  • a single alloy target can be prepared by smelting or powder metallurgy after uniformly mixing Al, Co, Cr, Ni and Mo metal powders at a ratio of 1:1:1:1:1 atomic percentage; Al, Co, Cr, Ni and Mo metal powders are uniformly mixed in a ratio of 1.1:1.1:1.1:0.6 atomic percentage, and then a single alloy target is prepared by smelting or powder metallurgy; Al, Co, Cr can be selected , Ni and Mo metal powders are uniformly mixed in a ratio of 1.1:1.1:1:1:0.8 atomic percentage, and then a single alloy target is prepared by smelting or powder metallurgy; Al, Co, Cr, Ni and Mo metal powders can be selected.
  • a single alloy target is prepared by smelting or powder metallurgy after uniform mixing in the ratio of atomic percentage of 1:1.5:0.75:1:0.75; Al, Co, Cr, Ni and Mo metal powders can be selected in atomic percentage of 0.9:
  • a single alloy target is prepared by smelting or powder metallurgy after uniform mixing in a ratio of 0.9:1:1:1.2; or Al, Co, Cr, Ni and Mo metal powders can be selected in an atomic percentage of 0.8:1.1:0.9:1.2
  • a single alloy target is prepared by smelting or powder metallurgy after uniform mixing in the ratio of : 1.
  • Al, Co, Cr, Ni and Mo are prepared into a single alloy target, and then the single alloy target is formed on the surface of the substrate by means of magnetron sputtering or arc ion plating to form a diffusion-resistant high-entropy alloy coating.
  • the specific process of magnetron sputtering or arc ion plating can refer to the existing process steps, wherein the high-entropy alloy coating with uniform composition and structure formed by the method of magnetron sputtering has more excellent diffusion resistance performance.
  • the base material is a superalloy, such as a common superalloy material such as iron-based superalloy, nickel-based superalloy, or cobalt-based superalloy, which is not limited in the embodiments of the present disclosure.
  • the thickness of the diffusion barrier high entropy alloy coating is 2 ⁇ m-8 ⁇ m, preferably 2 ⁇ m-7 ⁇ m, more preferably 2 ⁇ m-6 ⁇ m, more preferably 2 ⁇ m-5 ⁇ m, and more preferably 2 ⁇ m-4 ⁇ m. In the art, generally, the thicker the diffusion-resistant high-entropy alloy coating, the better its diffusion-resistant performance, but the thicker the coating, the heavier the coating will be.
  • this thickness range can not only effectively suppress the interdiffusion of alloy components between the substrate and the high-temperature coating, but also ensure the applicability of the high-entropy alloy diffusion barrier layer (that is, realize the thin coating and Good diffusion resistance performance can be achieved, and the deposition time of the thin coating is not too long, and the influence on the weight gain of the component is small, that is, the effect of small weight gain is guaranteed).
  • the thickness of the coating layer can also be adjusted according to requirements, which is not limited by the embodiments of the present disclosure.
  • the specific parameters are as follows: the background vacuum is less than or equal to 5 ⁇ 10 -3 Pa, the substrate temperature is 100-300°C, the target power is 200-300W, and the substrate temperature is 200-300W.
  • the DC bias voltage is -100--500V, the duty ratio is 60-90%, the target-base distance is 10-15cm, the working argon gas pressure is 0.6-0.8Pa, and the ion source is 0.8-1.2A.
  • the specific parameters are as follows: the background vacuum is less than or equal to 5 ⁇ 10 -3 Pa, the substrate temperature is 200-400°C, the target current is 70-90A, the substrate DC The bias voltage is -100--500V, the duty ratio is 60-90%, the target base distance is 20-30cm, the working argon gas pressure is 1-1.3Pa, the permanent magnet strength is 1500-2000Gs, and the electromagnetic coil voltage is 20-30V.
  • the formed coating has a dense structure, uniform composition and better high temperature oxidation resistance.
  • process parameters may also be adjusted according to requirements, which are not limited in the embodiments of the present disclosure.
  • a high-temperature resistant coating is prepared on the surface of the material body by using the diffusion-resistant high-entropy alloy coating material as the material body.
  • the formed high-temperature resistant coating material utilizes the slow diffusion effect unique to the diffusion-resistant high-entropy alloy coating, and has good physical and chemical matching with the substrate and the high-temperature resistant coating, which can effectively inhibit the substrate and the coating.
  • the interdiffusion of interlayer alloy components and the precipitation of harmful phases at the interface improve the high temperature oxidation resistance of the coating. It can be used in the preparation of aero-engine or gas turbine hot-end components to improve the service life and working reliability of components.
  • the high temperature resistant coatings are PtAl coating, NiAl coating, NiAlHf coating, NiCrAlY coating, CoCrAlY coating, NiAlPtNb coating, NiAlHfRu coating, CoCrAlYSi coating, NiCoCrAlYTa coating, NiCrAlYLaB coating, NiCoCrAlYHf coating layer and NiCoCrAlYTaRe coating.
  • the above coating materials are all existing high temperature resistant coatings, which are suitable for the high temperature resistant coatings of the high temperature resistant coating materials provided in the embodiments of the present disclosure, and have good physical and chemical compatibility.
  • the method for preparing the high temperature resistant coating is selected from magnetron sputtering, electron beam physical vapor deposition, arc ion plating, flame spraying, atmospheric plasma spraying, vacuum plasma spraying, cold spraying, plasma spraying-physical vapor deposition and pulse electroplating at least one of them. It can be a common coating formation method such as supersonic flame spraying, low-pressure plasma spraying, etc. The specific process can refer to the prior art records, and will not be repeated here.
  • the present embodiment provides a preparation method of a high temperature resistant coating material, which is prepared by the following methods:
  • Target preparation Al, Co, Cr, Ni and Mo metal powders are uniformly mixed in a ratio of 1:1:1:1:1 atomic percentage, and a single alloy is prepared by powder metallurgy as a target.
  • Substrate pretreatment Using nickel-based superalloy (N5) as the substrate, the surface of the substrate was ground and polished, and then ultrasonically cleaned with acetone, alcohol and deionized water, respectively, and dried.
  • N5 nickel-based superalloy
  • Diffusion-resistant high-entropy alloy coating deposition use magnetron sputtering to deposit the target material on the surface of the substrate after cleaning and blowing to form a diffusion-resistant high-entropy alloy coating, and the process parameters are: the background vacuum degree is less than 5 ⁇ 10 -3 Pa, substrate temperature of 200°C, target power of 250W, substrate DC bias of -100V, duty cycle of 70%, target-to-substrate distance of 12cm, working argon pressure of 0.7Pa, and ion source of 1A.
  • the thickness of the control coating is about 3 ⁇ m.
  • Arc ion plating is used to deposit NiAlHf high temperature resistant coating with a thickness of about 30 ⁇ m on the surface of the diffusion resistance high entropy alloy coating.
  • the process parameters are: the background vacuum is less than 5 ⁇ 10 -3 Pa, the base The material temperature is 350°C, the argon gas pressure is 2Pa, the arc current is 120A, the DC bias voltage is -100V, and the duty ratio is 70%.
  • the chemical composition of the NiAlHf coating is as follows: the Ni content is 68 wt.%, the Al content is 31 wt.%, and the Hf content is 1 wt.%.
  • the obtained high-temperature resistant coating material utilizes the unique resistance-diffusion effect of the resistance-diffusion high-entropy alloy coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high-temperature oxidation resistance of the coating.
  • This embodiment provides a method for preparing a high temperature resistant coating material, which is different from Embodiment 1 only in that: in step (3), the magnetron sputtering process parameters for the deposition of the diffusion-resistant high-entropy alloy coating are: background The vacuum degree is less than 5 ⁇ 10 -3 Pa, the substrate temperature is 150°C, the target power is 300W, the substrate DC bias is -300V, the duty cycle is 90%, the target-base distance is 10cm, the working argon gas pressure is 0.8Pa, the ion source is 1.2A.
  • the control coating thickness was 4 ⁇ m.
  • the obtained high-temperature resistant coating material utilizes the unique resistance-diffusion effect of the resistance-diffusion high-entropy alloy coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high-temperature oxidation resistance of the coating.
  • This embodiment provides a method for preparing a high temperature resistant coating material, which is different from Embodiment 1 only in that: in step (3), the magnetron sputtering process parameters for the deposition of the diffusion-resistant high-entropy alloy coating are: background The vacuum degree is less than 5 ⁇ 10 -3 Pa, the substrate temperature is 250°C, the target power is 250W, the substrate DC bias is -500V, the duty cycle is 60%, the target-base distance is 15cm, the working argon gas pressure is 0.6Pa, the ion source is 0.8A.
  • the control coating thickness was 2 ⁇ m.
  • the obtained high-temperature resistant coating material utilizes the unique resistance-diffusion effect of the resistance-diffusion high-entropy alloy coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high-temperature oxidation resistance of the coating.
  • the present embodiment provides a method for preparing a high temperature resistant coating material, which differs from Embodiment 1 only in that: in step (3), the arc ion plating technology is used for the deposition of the diffusion-resistant high-entropy alloy coating, and the process parameters are: The background vacuum is less than 5 ⁇ 10 - 3 Pa, the substrate temperature is 300°C, the target current is 70A, the substrate pulse bias is -100V, the duty cycle is 70%, the target-to-base distance is 20cm, and the working argon gas pressure is 1.3 Pa, permanent magnet strength 2000Gs, electromagnetic coil voltage 30V.
  • the obtained high-temperature resistant coating material utilizes the unique resistance-diffusion effect of the resistance-diffusion high-entropy alloy coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high-temperature oxidation resistance of the coating.
  • the present embodiment provides a method for preparing a high temperature resistant coating material, which is different from Embodiment 1 only in that in step (3), arc ion plating technology is used for coating deposition, and the process parameters are: the background vacuum degree is less than 5 ⁇ 10 -3 Pa, substrate temperature is 350°C, target current is 90A, substrate pulse bias is -300V, duty cycle is 90%, target-base distance is 30cm, working argon gas pressure is 1Pa, permanent magnet strength is 1500Gs , the solenoid voltage is 25V.
  • the obtained high-temperature resistant coating material utilizes the unique resistance-diffusion effect of the resistance-diffusion high-entropy alloy coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high-temperature oxidation resistance of the coating.
  • the present embodiment provides a method for preparing a high temperature resistant coating material, which is different from the embodiment 1 only in that in step (1), the atomic percentages of the Al, Co, Cr, Ni, and Mo metal powders used are: 1.1:1.1:1.1:1.1:0.6.
  • the obtained high-temperature resistant coating material utilizes the unique resistance-diffusion effect of the resistance-diffusion high-entropy alloy coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high-temperature oxidation resistance of the coating.
  • This embodiment provides a preparation method of a high temperature resistant coating material, the difference between which is different from that in Embodiment 1 is only that in step (2), the base material used is a cobalt-based superalloy (GH605).
  • the obtained high-temperature resistant coating material utilizes the unique resistance-diffusion effect of the resistance-diffusion high-entropy alloy coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high-temperature oxidation resistance of the coating.
  • This embodiment provides a method for preparing a high temperature resistant coating material, which is different from Embodiment 1 only in that in step (2), the substrate material used is an iron-based superalloy (GH706).
  • the obtained high-temperature resistant coating material utilizes the unique resistance-diffusion effect of the resistance-diffusion high-entropy alloy coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high-temperature oxidation resistance of the coating.
  • This embodiment provides a method for preparing a high temperature resistant coating material, which is different from Embodiment 1 only in that in step (4), magnetron sputtering is used to deposit a thickness of about 20 ⁇ m on the surface of the diffusion resistance high entropy alloy coating.
  • the process parameters of the CoCrAlY anti-high temperature coating are as follows: the background vacuum is less than 5 ⁇ 10 -3 Pa, the substrate temperature is 150°C, the argon pressure is 0.4Pa, the target current is 2.5A, the bias voltage is -100V, and the ion source is 1.5A.
  • the chemical composition of CoCrAlY coating is: Cr content is 40wt.%, Al content is 15wt.%, Y content is 3wt.%, and the rest is Co.
  • the obtained high-temperature resistant coating material utilizes the unique resistance-diffusion effect of the resistance-diffusion high-entropy alloy coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high-temperature oxidation resistance of the coating.
  • This embodiment provides a method for preparing a high temperature resistant coating material, which differs from Example 1 only in that: in step (4), a CoCrAlYSi high temperature resistant coating of about 40 ⁇ m is prepared by supersonic flame spraying, and the process parameters are: : Spray gun power 3kW, gas flow rate: 50m3/h, powder feeding amount: 5g/min, spraying distance: 300mm.
  • the chemical composition of CoCrAlYSi coating is: Cr content is 18wt.%, Al content is 12wt.%, Y content is 3wt.%, Si content is 1.5wt.%, and the rest is Ni.
  • the obtained high-temperature resistant coating material utilizes the unique resistance-diffusion effect of the resistance-diffusion high-entropy alloy coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high-temperature oxidation resistance of the coating.
  • the present embodiment provides a method for preparing a high temperature resistant coating material, which is different from the embodiment 1 only in that in step (1), the atomic percentages of the Al, Co, Cr, Ni, and Mo metal powders used are: 1.1:1.1:1:1:0.8.
  • the obtained high-temperature resistant coating material utilizes the unique resistance-diffusion effect of the resistance-diffusion high-entropy alloy coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high-temperature oxidation resistance of the coating.
  • the present embodiment provides a method for preparing a high temperature resistant coating material, which is different from the embodiment 1 only in that in step (1), the atomic percentages of the Al, Co, Cr, Ni, and Mo metal powders used are: 1:1.5:0.75:1:0.75.
  • the obtained high-temperature resistant coating material utilizes the unique resistance-diffusion effect of the resistance-diffusion high-entropy alloy coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high-temperature oxidation resistance of the coating.
  • the present embodiment provides a method for preparing a high temperature resistant coating material, which is different from the embodiment 1 only in that in step (1), the atomic percentages of the Al, Co, Cr, Ni, and Mo metal powders used are: 0.9:0.9:1:1:1.2.
  • the obtained high-temperature resistant coating material utilizes the unique resistance-diffusion effect of the resistance-diffusion high-entropy alloy coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high-temperature oxidation resistance of the coating.
  • the present embodiment provides a method for preparing a high temperature resistant coating material, which is different from the embodiment 1 only in that in step (1), the atomic percentages of the Al, Co, Cr, Ni, and Mo metal powders used are: 0.8:1.1:0.9:1.2:1.
  • the obtained high-temperature resistant coating material utilizes the unique resistance-diffusion effect of the resistance-diffusion high-entropy alloy coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high-temperature oxidation resistance of the coating.
  • This comparative example provides a preparation method of a high temperature resistant coating material, which differs from Example 1 only in that the NiAlHf high temperature resistant coating is directly formed on the nickel-based superalloy without depositing the diffusion-resistant high-entropy alloy coating.
  • the present comparative example provides a preparation method of a high temperature resistant coating material, which is different from Example 1 only in that Co metal powder is replaced with Ti metal powder.
  • the SEM image of the cross-section of the diffusion resistance high-entropy alloy coating is shown in Figure 1 (a), the coating structure is dense and the composition is uniform, and its phase structure is detected by XRD, as shown in Figure 1 (b), the coating is non- crystal phase. As shown in Fig. 1(c), the coating is a single solid solution phase (FCC structure).
  • Fig. 2 show that after 50 hours of oxidation at 1100 °C, no obvious interdiffusion zone and secondary reaction zone were observed in the NiAlHf/AlCoCrNiMo/N5 coating sample, and no TCP harmful phase was precipitated. This shows that the AlCoCrNiMo high-entropy alloy coating can effectively prevent the interdiffusion of alloy elements and inhibit the precipitation of harmful phases caused by interdiffusion.
  • Figure 3 shows that after 50 hours of oxidation at 1100 °C, the NiAlHf/N5 coating sample has an obvious element interdiffusion zone, a secondary reaction zone (SRZ) is formed under the interdiffusion layer, and a large number of needle-like TCP harmful phases are precipitated .
  • SRZ secondary reaction zone
  • the oxidation weight gain curves of the high temperature resistant coating materials prepared in Test Example 1 and Comparative Example 1 are shown in FIG. 4 , where NCN is the test result of Example 1, and NN is the test result of Comparative Example 1. It can be shown that the preparation method provided in this application can effectively form the AlCoCrNiMo high-entropy alloy diffusion barrier layer, realize the barrier diffusion between the high temperature protective coating and the high temperature substrate, and improve the high temperature oxidation resistance of the coating.
  • Example 1 The high temperature interface element diffusion behavior of the high temperature resistant coating materials prepared in Example 1 and Comparative Example 2 was tested, and the high temperature coating (NiAlHf)/diffusion barrier (AlCoCrNiMo)/superalloy ( The N5) sample and the high temperature coating (NiAlHf)/diffusion barrier (AlTiCrNiMo)/superalloy (N5) sample were subjected to oxidation test at 1100 °C. , FIG. 2 is the test result in Example 1, and FIG. 5 is the test result in Comparative Example 2.
  • the present disclosure provides a diffusion-resistant high-entropy alloy coating material and a preparation method thereof, which form a diffusion-resistant high-entropy alloy coating by using Al, Co, Cr, Ni and Mo, and the diffusion-resistant high-entropy alloy coating is
  • the alloy coating has good physical and chemical matching with the substrate and other coatings (such as high-temperature coatings), which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the resistance of the coating.
  • High temperature oxidation ability while avoiding mutual diffusion to reduce the mechanical properties of the substrate, prolonging the service life of the parts, its diffusion resistance effect is significantly improved compared to traditional metal or ceramic diffusion resistance materials.
  • the present disclosure also provides a high-temperature resistant coating material and a preparation method thereof.
  • a high-temperature resistant coating material By forming the above-mentioned resistance-diffusion high-entropy alloy coating on a substrate, and then using this as the material body to form a high-temperature resistant coating, the resistance-diffusion high-entropy alloy coating is formed by using the resistance-diffusion high-entropy alloy coating.
  • the alloy coating has a unique slow diffusion effect, and has good physical and chemical matching with the substrate and the high temperature resistant coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, improve the coating performance.
  • high temperature oxidation resistance The method is mature and reliable, has good repeatability, and is easy to realize large-scale industrial production.
  • the high temperature resistant coating material can be used in the preparation of aero-engine or gas turbine hot-end components, so as to improve the service life and working reliability of the components.
  • the multi-resistance-diffusion high-entropy alloy coating material and the preparation method thereof of the present disclosure are formed by using Al, Co, Cr, Ni and Mo to form the resistance-diffusion high-entropy alloy coating, the resistance-diffusion high-entropy alloy coating and the substrate and Other coatings (such as high temperature coatings) have good physical and chemical matching, which can effectively inhibit the mutual diffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, improve the high temperature oxidation resistance of the coating, and avoid mutual diffusion. Diffusion leads to a decrease in the mechanical properties of the substrate and prolongs the service life of the parts. Compared with traditional metal or ceramic anti-diffusion materials, its diffusion resistance effect is significantly improved.
  • the high-temperature resistant coating material and the preparation method thereof of the present disclosure are formed by forming the above-mentioned anti-diffusion high-entropy alloy coating on the base material, and then using the high-entropy alloy coating as the material body to form the high-temperature resistant coating, using the unique properties of the anti-diffusion high entropy alloy coating It has slow diffusion effect, and has good physical and chemical matching with the substrate and high temperature resistant coating, which can effectively inhibit the interdiffusion of alloy components between the substrate and the coating and the precipitation of harmful phases at the interface, and improve the high temperature oxidation resistance of the coating. .
  • the high temperature resistant coating material can be used in the preparation of aero-engine or gas turbine hot-end components, so as to improve the service life and working reliability of the components.

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Abstract

La présente invention concerne un matériau de revêtement en alliage à haute entropie résistant à la diffusion et un matériau de revêtement résistant à la chaleur, comprenant un substrat et un revêtement en alliage à haute entropie résistant à la diffusion. Le revêtement d'alliage à haute entropie résistant à la diffusion comprend les éléments : Al, Co, Cr, Ni et Mo. Le matériau de revêtement résistant à la chaleur est obtenu par formation du revêtement en alliage à haute entropie résistant à la diffusion susmentionné sur le substrat, puis, à l'aide de celui-ci en tant que matériau de base, par formation d'un revêtement résistant à la chaleur sur celui-ci. En utilisant un effet de diffusion lente unique du revêtement en alliage à haute entropie résistant à la diffusion et une bonne adaptation physique et chimique correspondante avec à la fois le substrat et le revêtement résistant à la chaleur, il est possible d'inhiber efficacement la diffusion réciproque de composants d'alliage et la précipitation de phase nocive au niveau de la surface de contact entre le substrat et le revêtement et d'améliorer la capacité de résistance à l'oxydation à haute température du revêtement. Le matériau de revêtement résistant à la chaleur peut être appliqué dans la préparation de pièces d'extrémité chaude de moteurs aéronautiques ou de turbines à gaz pour améliorer la durée de vie et la fiabilité de fonctionnement des pièces.
PCT/CN2020/127792 2020-09-23 2020-11-10 Matériau de revêtement en alliage à haute entropie résistant à la diffusion, matériau de revêtement résistant à la chaleur, son procédé de préparation et application correspondante WO2022062102A1 (fr)

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