CN112853156B - High-structure-stability nickel-based high-temperature alloy and preparation method thereof - Google Patents
High-structure-stability nickel-based high-temperature alloy and preparation method thereof Download PDFInfo
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- CN112853156B CN112853156B CN202110032939.6A CN202110032939A CN112853156B CN 112853156 B CN112853156 B CN 112853156B CN 202110032939 A CN202110032939 A CN 202110032939A CN 112853156 B CN112853156 B CN 112853156B
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- C22C19/05—Alloys based on nickel or cobalt based on nickel with chromium
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- C22C19/057—Alloys based on nickel or cobalt based on nickel with chromium and Mo or W with the maximum Cr content being less 10%
Abstract
The invention discloses a high-structure stability nickel-based high-temperature alloy and a preparation method thereof, belonging to the field of high-temperature alloys, wherein the high-structure stability nickel-based high-temperature alloy comprises the following chemical components in percentage by weight: al: 5.8-6.5%, W: 1-2%, Co: 8-9%, Cr: 3-4%, Mo: 1-2%, Re: 6.8-7.2%, Ru: 2.8-3.2%, Ta: 8-9% of Ni and 9.6% or more and 10% or less of Re + Ru in balance. The invention carries out solid solution heat treatment at 1300-1330 ℃, and carries out graded aging treatment at 1100-1150 ℃ and 850-870 ℃. The alloy of the invention has a gamma/gamma ' two-phase structure, and the gamma ' still keeps a cubic shape after 1150 ℃/100 hours of heat exposure, and the length-width ratio of the gamma ' is between
And
the thickness of gamma 'is less than 0.8 micron, the volume fraction of gamma' is more than 50 percent, no harmful phase TCP is precipitated, and the high-temperature tissue stability is good.
Description
Technical Field
The invention belongs to the technical field of high-temperature alloys, and relates to a high-structure-stability nickel-based high-temperature alloy and a preparation method thereof.
Background
The nickel-based single crystal superalloy has excellent high-temperature comprehensive performance and is the first choice material of high-pressure turbine blades of advanced aeroengines. In recent years, with the increase of the temperature of the turbine front inlet of an aeroengine, higher requirements are put on the heat resistance and the bearing capacity of the nickel-based single crystal superalloy, so that a great amount of refractory elements (such as Re, Mo, Ta, W and the like) are added into the modern superalloy for alloying, and compared with other traditional structural materials, the alloying degree of the nickel-based single crystal superalloy is very high. Therefore, from the thermodynamic perspective, the nickel-base single crystal superalloy is an unbalanced complex alloy system, and under the action of a complex temperature field/stress field, a gamma/gamma' two-phase microstructure can be inevitably changed in a long-term service process, and even harmful TCP (transmission control protocol) phases are precipitated, so that the performance is degraded, and the long-term structure stability of the nickel-base single crystal superalloy is crucial to the service performance of the nickel-base single crystal superalloy.
Re is the most effective solid solution strengthening element in the nickel-based high-temperature alloy, the high-temperature mechanical property of the nickel-based single crystal high-temperature alloy is greatly improved by adding Re, but the precipitation of a harmful phase TCP is easily promoted by adding Re in a large amount, the high-temperature tissue stability of the alloy is damaged, and the creep endurance of the alloy is rapidly deteriorated; in consideration of the cost and density of Re, although the development of low Re alloy is an important direction for the composition optimization of the nickel-based superalloy at present, in the present view, before a more appropriate substitute element is found, if the Re content is controlled below the 2 generation level (2-3 wt.%), the high temperature mechanical property of the alloy is difficult to break through. Ru is used as a structural stability element and is introduced into the nickel-based single crystal superalloy from the fourth generation, and the addition of Ru can inhibit the precipitation of a TCP phase and improve the structural stability of the nickel-based single crystal superalloy, thereby improving the mechanical property. Therefore, from the development trend, Re and Ru have become indispensable elements in high-performance nickel-base superalloy as the most effective creep strengthening elements and structure stability elements, respectively.
By now, nickel-based single crystal superalloys have been developed to the sixth generation. Wherein the fifth Generation and sixth Generation high performance nickel-based Superalloys are mainly developed by NIMS, and the developed fifth Generation Single Crystal superalloy TMS-162, TMS-173, TMS-196 series [ Y.Koizumi, T.Kobayashi, T.Yokokawa, et al, "Development of Next-Generation Ni-Base Single Crystal Superalloys", Superalloy 2004, (TMS,2004),35-43.Sato A, Yeh A C, Kobayashi T, et al.Fifth Generation Ni based Crystal with superior properties [ J ] Energy Materials,2007,2(1): 19-25.) the main characteristic of high Ru high Re is high Mo, which is increased by increasing the content of Mo in the alloy, and the mechanical property of the alloy is increased by a small amount of Mo, which is increased by a small amount of heat, and the temperature of the TMS-600 ℃ is increased, reflecting the high temperature tissue instability. The sixth generation nickel-based single crystal superalloy TMS-238[ Kawagishi K, Yeh A C, Yokokawa T, et al. development of an oxidation-resistant high-strength si xth-generation single-crystal super alloy TMS-238[ J ]. Superalloys,2012,2012:189 (195.) ] is mainly optimized for oxidation and corrosion resistance on the basis of the 5 th generation, and thus still shows the characteristics of high Ru (5 wt.%) and high Re (6.4 wt.%).
In summary, in order to ensure the high-temperature mechanical properties, the addition of Re and Ru is unavoidable, but the current alloying method is to increase the upper limit of the addition of TCP phase promoting elements Re, Mo, etc. by greatly increasing the content of Ru, and considering the cost and density of Re Ru, the alloying idea is difficult to continue to develop. Therefore, the key point for further optimizing the components of the nickel-based single crystal superalloy is to inhibit the TCP phase in the Re-containing alloy by adjusting the matching relation among alloy elements, particularly strengthening elements Re, Mo, Ta and W, reduce the total addition amount of Re and Ru by using lower Ru content and maintain the long-term structure stability of the alloy at high temperature.
Disclosure of Invention
The invention aims to provide a nickel-based high-temperature alloy with high structure stability and relatively low total refractory elements and a preparation method thereof, the obtained nickel-based high-temperature alloy can form a gamma/gamma 'two-phase structure with a gamma' shape cube after repeated smelting, solid solution and aging treatment, and the gamma 'shape cube can still be kept after being exposed for 100 hours at 1150 ℃, the gamma' volume fraction is more than 50%, and no TCP phase is precipitated.
The invention is realized by the following technical scheme:
the nickel-based high-temperature alloy with high structure stability is characterized by comprising the following chemical components in percentage by weight: 5.8-6.5%, W: 1-2%, Co: 8-9%, Cr: 3-4%, Mo: 1-2%, Re: 6.8-7.2%, Ru: 2.8-3.2%, Ta: 8-9% and the balance of Ni.
The chemical components are more than or equal to 9.6 percent and less than or equal to 10 percent of Re + Ru according to weight percentage.
The alloy is subjected to solution treatment and aging treatment to form a two-phase structure which is a gamma matrix phase and an L matrix phase of an A1 crystal structure respectively12And (3) gamma 'precipitated phase with a crystal structure, wherein the gamma' morphology is cubic. After the alloy is subjected to solid solution and aging treatment, the alloy is subjected to 1150 ℃/100h heat treatment, gamma' keeps cubic,
aspect ratio
The thickness of gamma 'is less than 0.8 μm, and the volume fraction of gamma' is more than 50%.
The preparation process of the alloy comprises the following steps:
(1) weighing high-purity Ni, Al, Co, Cr, Mo, Re, Ru, Ta and W elementary substance materials according to the component proportion;
(2) placing the weighed high-purity simple substance raw materials in a vacuum arc melting furnace, melting the alloy in a high-purity argon protective atmosphere, controlling the current of a melting arc at 280-350A, keeping for 30-60 seconds after the alloy is completely liquefied, then cutting off the power and cooling until the alloy is completely solidified, repeating the melting step, and finally obtaining a nickel-based high-temperature alloy ingot;
(3) in a high-purity argon protective atmosphere, preserving the temperature of the prepared nickel-based high-temperature alloy ingot for 10-24 hours at the solid solution temperature of 1300-1330 ℃, and cooling in the air; and then preserving heat for 4-5 h at 1100-1150 ℃, air cooling, then preserving heat for 16-24 h at 850-870 ℃, and air cooling to obtain the nickel-based high-temperature alloy with high structure stability.
In the step (2), the smelting step is repeated for 8-12 times to ensure the uniformity of the alloy.
The alloy comprehensively considers the influence of alloy elements on the tissue stability, the oxidation resistance, the high-temperature mechanical property and the cost density when designing the components, and the specific consideration factors are as follows:
al: the precipitation strengthening phase gamma 'forming element in the nickel-based high-temperature alloy is beneficial to ensuring the content of gamma', and has the functions of oxidation resistance and corrosion resistance at high temperature, but researches show that the precipitation tendency of a TCP (transmission control protocol) phase can be increased due to overhigh Al content, and the high-temperature structure stability and the mechanical property of the alloy are not facilitated, so that the Al content is 5.8-6.5 wt.%.
Co: the gamma phase forming element and some researches show that Co can inhibit TCP phase precipitation and plays a role in tissue stability, but the addition of a large amount of Co can reduce the dissolution temperature of the gamma 'phase, so that the stability of the gamma' phase at high temperature is reduced, and therefore, the content of Co is 8-9 wt%.
Cr: the forming element of the gamma phase belongs to weak solid solution strengthening elements, the purpose of adding Cr is mainly to improve the oxidation resistance and corrosion resistance and promote the precipitation tendency of a TCP phase, so that the content of Cr needs to be controlled to further increase the content of other more effective solid solution strengthening elements while ensuring the oxidation resistance, and the content of Cr is limited to 3-4 wt.%.
Mo: the gamma phase forming element is beneficial to the high-temperature creep property of the alloy, but is easy to promote the precipitation of the TCP phase and is unfavorable for oxidation resistance, so that the content of Mo is limited to: 1-2 wt.%.
Re: the most effective solid solution strengthening element is easy to cause TCP phase precipitation, and has higher cost and density, so the content of Re is 6.8-7.2 wt.%.
Ru: the most effective element for the structural stability mainly acts to inhibit the precipitation of TCP phase, but the cost is high, so the best possible effect needs to be achieved by the minimum content, and the content of Ru is 2.8-3.2 wt.%.
Ta: is a forming element of a gamma ' phase, is favorable for delaying the re-dissolution of the gamma ' phase at high temperature and improving the high-temperature strength of the gamma ' phase, and simultaneously, Ta has little influence on the precipitation of a TCP phase, so that the content of Ta is improved within a reasonable range, and the ratio of Ta: 8-9 wt.%.
W: solid solution strengthening elements improve the solution temperature of the solid phase, the liquidus phase and the gamma' phase, but have higher density and are TCP phase forming elements, so in order to improve the proportion (such as Re) of more effective solid solution strengthening elements, thereby being beneficial to maximizing high-temperature creep property, the content of W is controlled to be 1-2 wt.%.
Re + Ru: on one hand, Re and Ru are respectively the most effective strengthening elements and the most effective structural stability elements, and must be added in the design process of the components of the nickel-based single crystal superalloy in order to ensure higher high-temperature mechanical property; on the other hand, Re and Ru are rare elements, have high cost and strategic significance, and are easily influenced by the market and international environment in reality, so that the addition amount of Re + Ru needs to be ensured as small as possible and the maximum effect is achieved, and therefore, the range of Re + Ru is controlled to be more than or equal to 9.6% and less than or equal to 10%.
The invention has the beneficial effects that: the nickel-based superalloy prepared by the method has a uniform gamma/gamma ' two-phase structure, the gamma ' still keeps a nearly cubic shape after being exposed for 100 hours at 1150 ℃, the volume fraction of the gamma ' is more than 50%, and no TCP phase is precipitated, so that the nickel-based superalloy has strong high-temperature long-term structure stability and indicates good high-temperature creep property; on the other hand, the total amount of the alloy Re and Ru is less than 10.9 wt.% of a fifth generation nickel-based single crystal superalloy TMS-162(4.9 wt.% Re 6 wt.% Ru), 11.9 wt.% of TMS-173(6.9 wt.% Re 5 wt.% Ru) and 11.4 wt.% of TMS-196(6.4 wt.% Re 5 wt.% Ru), the Ru content is only about half of that of a fifth generation single crystal, and the W content is lower, the W content in the conventional nickel-based high temperature alloy of 4 generations and above is generally 5-6 wt.%, the W content of the alloy of the invention is controlled to be 1-2 wt.%, the proportioning of more effective solid solution strengthening elements is favorably improved, and the high temperature creep property is favorably maximized, and the Ta element content is obviously higher than that of the conventional nickel-based single crystal high temperature alloy, the higher Ta element is favorably improved in the gamma' -phase high temperature strength, so the alloy can be used as a candidate material of a hot end part of an aeroengine, has good application prospect.
Drawings
FIG. 1 is a scanning electron micrograph of the typical morphology of the alloy of example 1 of the present invention.
FIG. 2 is a scanning electron micrograph of a typical morphology of the alloy of example 1 of the present invention after heat treatment at 1150 ℃ for 100 hours.
FIG. 3 is a scanning electron micrograph of a typical morphology of the alloy of example 1 of the present invention after heat treatment at 1100 ℃ for 1000 hours.
FIG. 4 is a scanning electron micrograph of the typical morphology of the alloy of example 2 of the present invention.
FIG. 5 is a scanning electron micrograph of a typical morphology of the alloy of example 2 of the present invention after heat treatment at 1150 ℃ for 100 hours.
FIG. 6 is a scanning electron micrograph of the typical morphology of the alloy of example 3 of the present invention.
FIG. 7 is a scanning electron micrograph of a typical morphology of the alloy of example 3 of the present invention after heat treatment at 1150 ℃ for 100 hours.
FIG. 8 is a scanning electron micrograph of a typical morphology of the TMS-196 alloy after heat treatment at 1150 ℃ for 100 hours.
Detailed Description
The following detailed description is presented to enable those skilled in the art to better understand the advantages and features of the present invention. Table 1 shows the alloy compositions (in weight percent) of the examples, and for comparison, the compositions of the fifth generation nickel-base single crystal superalloys TMS-162, TMS-173, and TMS-196 are also shown. It is apparent that the embodiments described below are only a part of the embodiments of the present invention, and not all of them. All other embodiments, which can be obtained by a person skilled in the art without any inventive step based on the embodiments of the present invention, belong to the scope of the present invention.
TABLE 1
Example 1
Weighing high-purity Ni, Al, Co, Cr, Mo, Re, Ru, Ta, W and other simple-substance metals according to the components shown in alloy 1 in Table 1, placing the weighed metal raw materials in a vacuum arc melting furnace, carrying out alloy melting in high-purity argon protection, controlling the current of a melting arc at 350A, keeping for 1 minute after the alloy is completely liquefied, and then cutting off the power and cooling until the alloy is completely solidified. Repeating the smelting step for 12 times to ensure the uniformity of the alloy and finally obtaining the nickel-based high-temperature alloy ingot; and (3) keeping the prepared nickel-based high-temperature alloy ingot at the solid solution temperature of 1320 ℃ for 24 hours in the high-purity argon protective atmosphere, air-cooling, keeping the temperature at 1150 ℃ for 4 hours, air-cooling, keeping the temperature at 870 ℃ for 24 hours, and air-cooling to obtain the nickel-based high-temperature alloy with high structure stability. As shown in FIG. 1, in the SEM of typical morphology of the alloy of example 1, the γ 'phase was cubic, the aspect ratio was 1.5, the γ' thickness was 0.49 μm, and the volume fraction was 61.7%. Then, the alloy of the example 1 of the present invention is subjected to a heat treatment experiment at 1150 ℃ for 100h, and fig. 2 is a scanning photograph of a typical structure morphology of the alloy of the example 1 after aging treatment at 1150 ℃ for 100h, wherein the gamma 'phase is cubic, the aspect ratio is 1.67, the thickness of the gamma' phase is 0.74 μm, the volume fraction is 52.2%, and no TCP phase is precipitated, which shows that the alloy of the example 1 of the present invention has good high-temperature structure stability at 1150 ℃. The alloy of example 1 of the present invention is subjected to a heat treatment experiment at 1100 ℃ for 1000h, and fig. 3 is a scanning photograph of a typical structure morphology after the alloy of example 1 of the present invention is subjected to an aging treatment at 1100 ℃ for 1000h, and compared with the typical structure morphology of the TMS-196 alloy, as shown in fig. 8, the volume fraction of the γ' phase is 60.2%, and no TCP phase is still precipitated, which indicates that the alloy of the present invention has good high temperature structure stability at 1100 ℃.
Example 2
Weighing high-purity Ni, Al, Co, Cr, Mo, Re, Ru, Ta, W and other simple-substance metals according to the components shown in the alloy 2 in the table 1, placing the weighed metal raw materials in a vacuum arc melting furnace, carrying out alloy melting in the protection of high-purity argon, controlling the current of a melting arc at 350A, keeping for 1 minute after the alloy is completely liquefied, and then cutting off the power and cooling until the alloy is completely solidified. Repeating the smelting step for 12 times to ensure the uniformity of the alloy and finally obtaining the nickel-based high-temperature alloy ingot; and (3) keeping the prepared nickel-based high-temperature alloy ingot at the solid solution temperature of 1330 ℃ for 10 hours in the atmosphere of high-purity argon gas, air-cooling, keeping the temperature at 1100 ℃ for 4 hours, air-cooling, keeping the temperature at 870 ℃ for 16 hours, and air-cooling to obtain the nickel-based high-temperature alloy with high structure stability. As shown in FIG. 4, in the SEM image of the typical morphology of the alloy of example 2 of the present invention, the γ 'phase is cubic, the aspect ratio is 1.51, the γ' thickness is 0.2 μm, and the volume fraction is 54.1%. Then, the alloy of the embodiment 2 of the present invention is subjected to a heat treatment experiment at 1150 ℃ for 100h, and fig. 5 is a scanning photograph of a typical structure morphology of the alloy of the embodiment 2 of the present invention after being subjected to a heat treatment at 1150 ℃ for 100h, wherein the gamma 'phase is cubic, the aspect ratio is 1.53, the thickness of the gamma' phase is 0.67 μm, the volume fraction is 50.6%, and no TCP phase is precipitated, which indicates that the alloy of the present invention has good high temperature structure stability at 1150 ℃.
Example 3
Weighing high-purity Ni, Al, Co, Cr, Mo, Re, Ru, Ta, W and other simple-substance metals according to the components shown in alloy 3 in table 1, placing the weighed metal raw materials in a vacuum arc melting furnace, carrying out alloy melting in high-purity argon protection, controlling the current of a melting arc at 350A, keeping for 1 minute after the alloy is completely liquefied, and then cutting off the power and cooling until the alloy is completely solidified. Repeating the smelting step for 10 times to ensure the uniformity of the alloy and finally obtain the nickel-based high-temperature alloy ingot; and (3) keeping the prepared nickel-based high-temperature alloy ingot at the solid solution temperature of 1330 ℃ for 16 hours in the high-purity argon protective atmosphere, air-cooling, keeping the temperature at 1150 ℃ for 4 hours, air-cooling, keeping the temperature at 870 ℃ for 23 hours, and air-cooling to obtain the nickel-based high-temperature alloy with high structure stability. As shown in FIG. 6, which is a SEM image of the typical morphology of the alloy of example 3 of the present invention, the γ 'phase is cubic, the aspect ratio is 1.54, the γ' thickness is 0.32 μm, and the volume fraction is 57.1%. Then, the alloy of the embodiment 3 of the present invention is subjected to a heat treatment experiment at 1150 ℃ for 100h, and fig. 7 is a scanning photograph of a typical structure morphology of the alloy of the embodiment 3 of the present invention after being subjected to a heat treatment at 1150 ℃ for 100h, wherein the gamma 'phase is cubic, the aspect ratio is 1.64, the thickness of the gamma' phase is 0.62 μm, the volume fraction is 53.5%, and no TCP phase is precipitated, which indicates that the alloy of the present invention has good high temperature structure stability at 1150 ℃.
It will be evident to those skilled in the art that the invention is not limited to the details of the foregoing illustrative embodiments, and that the present invention may be embodied in other specific forms without departing from the spirit or essential attributes thereof. The present embodiments are therefore to be considered as illustrative and all changes coming within the meaning and range of equivalency of the claims are therefore intended to be embraced therein.
Claims (4)
1. The nickel-based high-temperature alloy with high structure stability is characterized by comprising the following chemical components in percentage by weight: 5.8-6.5%, W: 1-2%, Co: 8-9%, Cr: 3-4%, Mo: 1-2%, Re: 6.8-7.2%, Ru: 2.8-3.2%, Ta: 8-9% of Ni and the balance of Ni; the chemical components of the alloy meet the requirement that the weight percentage of Re + Ru is more than or equal to 9.6 percent and less than or equal to 10 percent.
2. The method for preparing the high-structure-stability nickel-base superalloy as defined in claim 1, wherein the specific preparation process comprises the following steps:
(1) weighing high-purity Ni, Al, Co, Cr, Mo, Re, Ru, Ta and W elementary substance materials according to the component proportion;
(2) placing the weighed high-purity simple substance raw materials in a vacuum arc melting furnace, melting the alloy in a high-purity argon protective atmosphere, controlling the current of a melting arc at 280-350A, keeping for 30-60 seconds after the alloy is completely liquefied, then cutting off the power and cooling until the alloy is completely solidified, repeating the melting step, and finally obtaining a nickel-based high-temperature alloy ingot;
(3) in a high-purity argon protective atmosphere, preserving the temperature of the prepared nickel-based high-temperature alloy ingot for 10-24 hours at the solid solution temperature of 1300-1330 ℃, and cooling in the air; and then preserving heat for 4-5 hours at 1100-1150 ℃, air cooling, then preserving heat for 16-24 hours at 850-870 ℃, and air cooling to obtain the nickel-based high-temperature alloy with high structure stability.
3. The method for preparing the nickel-based superalloy with high structure stability according to claim 2, wherein the melting step in the step (2) is repeated for 8-12 times.
4. The high-structure-stability nickel-base superalloy prepared according to claim 1 or 2, wherein γ' remains cubic after 1150 ℃/100 hours of heat treatment,
the thickness of gamma 'is less than 0.8 μm, and the volume fraction of gamma' is more than 50%.
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