CN114561603B - NbHfZrU series uranium-containing high entropy alloy - Google Patents
NbHfZrU series uranium-containing high entropy alloy Download PDFInfo
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Abstract
The invention discloses a Nb-Hf-Zr-U system structure function integration-based high-entropy alloy containing uranium and capable of being used as nuclear fuel, belonging to the field of high-entropy alloy materials, wherein Nb-Hf-Zr-U system alloy components comprise the following components in atomic percentage: niobium: 15-60%; zirconium: 10-35%; hafnium: 10-35%; uranium: 15-50%; aluminum: 0.01-10%, and the balance of chromium and inevitable impurities. Aiming at the bottleneck problems that the traditional metal type fuel with poor radiation resistance performance such as alloys of UZr, UAl and the like is easy to change phase at high temperature, is easy to generate radiation damage after a reactor irradiates for a long time, and radiation swelling caused by fission products, and the like, and other researches do not pay full attention to the research on U, Hf-containing high-entropy alloy fuel, the invention provides the high-entropy alloy based on the Nb-Hf-Zr-U system, and fully considers the special action of U, Hf elements, thereby realizing the structural function integration of the high-entropy alloy.
Description
Technical Field
The invention belongs to the field of alloy fuel materials, and particularly relates to a novel high-entropy alloy capable of being used as nuclear fuel and a preparation method thereof.
Background
The high-entropy alloy is used as a novel multi-principal-element solid solution alloy, and has a series of excellent comprehensive properties such as high strength, good heat resistance and the like due to the multi-principal-element effect, so that the design idea of the high-entropy alloy has great development potential. Related researches in recent years show that the high-entropy alloy also has radiation resistance superior to that of the traditional radiation-resistant alloy. The literature reports the structure evolution process of the single-phase FCC structure CoCrCuFeNi high-entropy alloy under the action of fast electron irradiation observed by an in-situ transmission electron microscope, and the high-entropy alloy is found to have no obvious structure evolution phenomenon within the temperature range of 25-500 ℃, and the phase structure and the grain size are kept stable. In addition, the group also found that the Zr-Hf-Nb alloy with single-phase BCC structure has stable structure under the electron irradiation condition that the irradiation damage reaches 10dpa at 25 ℃. Therefore, the high-entropy alloy has the capacity of serving a nuclear reactor under the high-temperature irradiation condition, and has wide application prospects in the nuclear field, but the development work of the high-entropy alloy which can be used as metal type nuclear fuel and contains uranium is rarely reported at present.
The nuclear fuel can be divided into three types, namely ceramic nuclear fuel, dispersion nuclear fuel and metal nuclear fuel, wherein the metal nuclear fuel mainly refers to uranium and alloy thereof, and comprises fuels such as U-Zr, U-Pu-Zr and the like. The traditional metal nuclear fuel has the advantages of high fissile atomic density, high thermal conductivity, easy processing and the like, but has very poor irradiation resistance, easy occurrence of irradiation growth and irradiation swelling caused by fission gas, and short service life. The U element is used as a main fuel of nuclear fission, the corrosion resistance of the alloy can be improved by adding microelements such as niobium, titanium and the like, the mechanical property of the alloy can be fundamentally changed, and the alloy can form an infinite solid solution high-entropy alloy with a BCC structure with elements such as Nb, Zr, Hf and the like, and comprises [ TaNb ]0.31(TiUHf)0.69 and UMoNbTaHf alloy with a single-phase BCC structure and UMoNbTaTi high-entropy alloy with a double-phase BCC structure, the high entropy of the uranium-containing alloy obviously improves the comprehensive property of the uranium-containing alloy, and provides a theoretical basis for designing novel high-entropy alloy with uranium and capable of being used as nuclear fuel.
As a common main element of the BCC-structure high-entropy alloy, the addition of the Hf element with the characteristics of high melting point and high hardness can obviously enhance the strength and hardness of the high-entropy alloy. For example, research on the preparation of UHfNbTi single-phase BCC-structure high-entropy alloy shows that the high-entropy alloy has excellent mechanical properties. In addition, compared with low thermal neutron absorption cross section elements such as Nb and Zr, the absorption cross section of the Hf element thermal neutron is higher by 1-2 orders of magnitude and is 115barn, so that the thermal neutron absorption cross section of the high-entropy alloy can be regulated and controlled by properly adjusting the content of the Hf element, the high-entropy alloy is applied to various multi-core field scenes, and the structural function integration characteristic is expressed.
However, the research on NbHfZrU high-entropy alloy is rarely reported, and the action mechanism of elements such as U, Hf in Nb-Hf-Zr-U system is not clear. The high-entropy alloy based on the Nb-Ti-Zr-U system and the Nb-Hf-Zr-U system is developed, and the special effect that U, Hf elements can be used as nuclear fuel is fully considered, so that the structural function integration of the uranium-containing high-entropy alloy is realized, and the high-entropy alloy has important significance for developing a novel high-toughness neutron-absorbing metal type fuel phase and promoting the safe development of the field of nuclear materials.
Disclosure of Invention
Aiming at the bottleneck problems that the traditional metal type fuel with poor radiation resistance performance such as alloys of UZr, U-Pu-Zr and the like is easy to change phase at high temperature, is easy to generate radiation damage after a reactor is irradiated for a long time, radiation swelling caused by fission products and the like, and other researches do not give full attention to the research on the U-containing high-entropy alloy fuel, the invention provides the Nb-Hf-Zr-U system-based high-entropy alloy which can be used as nuclear fuel, and fully considers the special action of U, Hf elements, thereby realizing the structural function integration of the high-entropy alloy.
The uranium-containing element can be used as a structural function integrated high-entropy alloy of nuclear fuel based on a Nb-Hf-Zr-U system, and comprises the following components in atomic percent: niobium: 15-60%; zirconium: 10-35%; hafnium: 10-35%; uranium: 15-50%; aluminum: 0.01-10%; the balance of chromium and inevitable impurities.
The technical scheme is further improved and optimized, and the components of the alloy comprise the following components in atomic percentage: niobium: 15-35 percent; zirconium: 10-35%; hafnium: 10-35%; uranium: 30-50%; aluminum: 0.01-10%, and the balance of chromium and inevitable impurities.
The technical scheme is further improved and optimized, and the components of the alloy comprise the following components in atomic percentage: niobium: 15 percent; zirconium: 10 percent; hafnium: 10 percent; uranium: 50 percent; aluminum: 10% and the balance of chromium and inevitable impurities.
The technical scheme is further improved and optimized, and the components of the alloy comprise the following components in atomic percentage: niobium: 35-60 percent; zirconium: 10-35 percent; hafnium: 10-15%; uranium: 15-30%; aluminum: 0.01-10%, and the balance of chromium and inevitable impurities.
The technical scheme is further improved and optimized, and the components of the alloy material are as follows by atomic percentage: niobium: 35 percent; zirconium: 10 percent; hafnium: 15 percent; uranium: 30 percent; aluminum: 9.99 percent, and the balance being chromium and inevitable impurities.
The technical scheme is further improved and optimized, and the components of the alloy comprise the following components in atomic percentage: niobium: 15-35%; zirconium: 10-35%; hafnium: 10-35%; uranium: 15-30%; aluminum: 0.01 to 4.99 percent, and the balance of chromium element and inevitable impurities.
The uranium-containing element based Nb-Hf-Zr-U system can be used as a structure function integrated high-entropy alloy of nuclear fuel, and has the following tensile yield strength: 887-1379 MPa, plasticity: 6-15 percent.
The invention discloses a preparation method of a structure-function integrated high-entropy alloy which contains uranium elements and can be used as nuclear fuel based on Nb-Hf-Zr-U series, which comprises the following steps:
(1) preparing raw materials: weighing required alloy raw materials according to the Nb-Hf-Zr-U series high-entropy alloy proportion;
(2) arc melting: under the protection of protective gas, rapidly heating and melting Nb, Hf, Zr, U, Al and Cr powder; in order to obtain alloy ingots with uniform components, all samples are repeatedly smelted for five times, and the samples are turned over after each smelting. In order to avoid that the structure and the performance of the sample are possibly influenced to a certain extent due to the difference of smelting time and smelting current, the current is directly closed after all alloy elements are completely melted into liquid state in each smelting of the sample and the smelting is kept for 1 min. Ensure that the surface of all the samples after melting remains bright, i.e. no significant oxidation of the alloy occurs during the melting preparation.
Has the advantages that:
the uranium-containing element based Nb-Hf-Zr-U system provided by the invention can be used as a structural function integrated high-entropy alloy of nuclear fuel, and due to the addition of the U element, the strength of the alloy is greatly improved at room temperature compared with that of the traditional BCC structure multi-principal element alloy NbTiHfZr; in addition, the addition of Al and Cr elements improves the high-temperature oxidation resistance of the alloy on the premise of keeping higher yield strength, so that the high-entropy alloy can be widely applied to the field of nuclear industry; hf element is used as a high thermal neutron absorption cross section element, and can be used for regulating and controlling the thermal neutron absorption cross section coefficient of the alloy while improving the mechanical property of the alloy; more importantly, the high-entropy alloy contains U element, and not only can keep good mechanical property when the high-entropy alloy is used in a reactor, but also can be used as nuclear fuel of the reactor to provide energy, so that the high-entropy alloy provides the best candidate material with good mechanical property, high-temperature oxidation resistance and irradiation resistance for the research field of nuclear fuel. Therefore, the high-entropy alloy based on the Nb-Hf-Zr-U system realizes the structural function integration of the high-entropy alloy by fully considering the special action of the U element, and has important significance for the development and application of the novel high-entropy metal nuclear fuel field.
Detailed Description
The present invention will be described in further detail in order to make the objects, technical solutions and advantages of the present invention more apparent. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
On the contrary, the invention is intended to cover alternatives, modifications, equivalents and alternatives which may be included within the spirit and scope of the invention as defined by the appended claims. Furthermore, in the following detailed description of the present invention, certain specific details are set forth in order to provide a better understanding of the present invention. It will be apparent to one skilled in the art that the present invention may be practiced without these specific details. The present invention will be further described with reference to the following embodiments.
Example 1
A novel uranium-containing high-entropy alloy of Nb-Hf-Zr-U series comprises the following specific alloy components: 15 at.% Nb, 10% Zr, 10% Hf, 50% U, 10% Al, 5% Cr, the balance unavoidable impurity elements.
The preparation method of the novel uranium-containing high-entropy alloy comprises the following steps:
(1) preparing raw materials: weighing required alloy raw materials according to the proportion of the novel uranium-containing high-entropy Nb-Hf-Zr-U-Al-Cr alloy, wherein the specific alloy components are as follows: 15 at.% Nb, 10% Zr, 10% Hf, 50% U, 10% Al, 5% Cr;
(2) arc melting: under the protection of protective gas, rapidly heating and melting Nb, Hf, Zr, U, Al and Cr powder; in order to obtain alloy ingots with uniform components, all samples are repeatedly smelted for five times, and the samples are turned over after each smelting. In order to avoid that the structure and the performance of the sample are possibly influenced to a certain extent due to the difference of smelting time and smelting current, the current is directly closed after all alloy elements are completely melted into liquid state in each smelting of the sample and the smelting is kept for 1 min.
The mechanical property test of the novel uranium-containing high-entropy Nb-Hf-Zr-U-Al-Cr alloy ingot prepared by the embodiment shows that: the tensile yield strength is 1379MPa, the plasticity is 6%, and the ultrahigh strength characteristic is shown.
Example 2
A novel uranium-containing high-entropy alloy of Nb-Hf-Zr-U series comprises the following specific alloy components: 35 at.% Nb, 10% Zr, 15% Hf, 30% U, 9.99% Al, 0.01% Cr, the balance unavoidable impurity elements.
The preparation method of the novel uranium-containing high-entropy alloy comprises the following steps:
(1) preparing raw materials: weighing required alloy raw materials according to the proportion of the novel uranium-containing high-entropy Nb-Hf-Zr-U-Al-Cr alloy, wherein the specific alloy components are as follows: 35 at.% Nb, 10% Zr, 15% Hf, 30% U, 9.99% Al, 0.01% Cr;
(2) arc melting: under the protection of protective gas, rapidly heating and melting Nb, Hf, Zr, U, Al and Cr powder; in order to obtain alloy ingots with uniform components, all samples are repeatedly smelted for five times, and the samples are turned over after each smelting. In order to avoid that the structure and the performance of the sample are possibly influenced to a certain extent due to the difference of smelting time and smelting current, the current is directly closed after all alloy elements are completely melted into liquid state in each smelting of the sample and the smelting is kept for 1 min.
The mechanical property test of the novel uranium-containing high-entropy Nb-Hf-Zr-U-Al-Cr alloy ingot prepared by the embodiment shows that: the tensile yield strength is 1245 MPa, the plasticity is 7%, and the good mechanical property matching characteristic is shown.
Example 3
A novel uranium-containing high-entropy alloy of Nb-Hf-Zr-U series comprises the following specific alloy components: 60 at.% Nb, 10% Zr, 10% Hf, 15% U, 0.01% Al, 4.99% Cr, and the balance unavoidable impurity elements.
The preparation method of the novel uranium-containing high-entropy alloy comprises the following steps:
(1) preparing raw materials: weighing required alloy raw materials according to the proportion of the novel uranium-containing high-entropy Nb-Hf-Zr-U-Al-Cr alloy, wherein the specific alloy components are as follows: 60 at.% Nb, 10% Zr, 10% Hf, 15% U, 0.01% Al, 4.99% Cr;
(2) arc melting: under the protection of protective gas, rapidly heating and melting Nb, Hf, Zr, U, Al and Cr powder; in order to obtain alloy ingots with uniform components, all samples are repeatedly smelted for five times, and the samples are turned over after each smelting. In order to avoid that the structure and the performance of the sample are possibly influenced to a certain extent due to the difference of smelting time and smelting current, the current is directly closed after all alloy elements are completely melted into liquid state in each smelting of the sample and the smelting is kept for 1 min.
The mechanical property test of the novel uranium-containing high-entropy Nb-Hf-Zr-U-Al-Cr alloy ingot prepared by the embodiment shows that: the tensile yield strength is 1132 MPa, the plasticity is 10%, and the high-strength plastic has good characteristics.
Example 4
A novel uranium-containing high-entropy alloy of Nb-Hf-Zr-U series comprises the following specific alloy components: 15 at.% Nb, 35% Zr, 10% Hf, 29.9% U, 0.01% Al, 10% Cr, the balance unavoidable impurity elements.
The preparation method of the novel uranium-containing high-entropy alloy comprises the following steps:
(1) preparing raw materials: weighing required alloy raw materials according to the proportion of the novel uranium-containing high-entropy Nb-Hf-Zr-U-Al-Cr alloy, wherein the specific alloy components are as follows: 15 at.% Nb, 35% Zr, 10% Hf, 29.9% U, 0.01% Al, 10% Cr;
(2) arc melting: under the protection of protective gas, rapidly heating and melting Nb, Hf, Zr, U, Al and Cr powder; in order to obtain alloy ingots with uniform components, all samples are repeatedly smelted for five times, and the samples are turned over after each smelting. In order to avoid that the structure and the performance of the sample are possibly influenced to a certain extent due to the difference of smelting time and smelting current, the current is directly closed after all alloy elements are completely melted into liquid state in each smelting of the sample and the smelting is kept for 1 min.
The mechanical property test of the novel uranium-containing high-entropy Nb-Hf-Zr-U-Al-Cr alloy ingot prepared by the embodiment shows that: the tensile yield strength is 1002 MPa, the plasticity is 13%, and the excellent plasticity is shown while the good strength is maintained.
Example 5
A novel uranium-containing high-entropy alloy of Nb-Hf-Zr-U series comprises the following specific alloy components: 35 at.% of Nb, 10% of Zr, 35% of Hf, 15% of U, 4.99% of Al, 0.01% of Cr and the balance of unavoidable impurity elements.
The preparation method of the novel uranium-containing high-entropy alloy comprises the following steps:
(1) preparing raw materials: weighing required alloy raw materials according to the proportion of the novel uranium-containing high-entropy Nb-Hf-Zr-U-Al-Cr alloy, wherein the specific alloy components are as follows: 35 at.% Nb, 10% Zr, 35% Hf, 15% U, 4.99% Al, 0.01% Cr;
(2) arc melting: under the protection of protective gas, rapidly heating and melting Nb, Hf, Zr, U, Al and Cr powder; in order to obtain alloy ingots with uniform components, all samples are repeatedly smelted for five times, and the samples are turned over after each smelting. In order to avoid that the structure and the performance of the sample are possibly influenced to a certain extent due to the difference of smelting time and smelting current, the current is directly closed after all alloy elements are completely melted into liquid state in each smelting of the sample and the smelting is kept for 1 min.
The mechanical property test of the novel uranium-containing high-entropy Nb-Hf-Zr-U-Al-Cr alloy ingot prepared by the embodiment shows that: the tensile yield strength is 887MPa, the plasticity is-15%, and good strength and plasticity matching characteristics are shown.
Compared with the existing material, the novel uranium-containing high-entropy Nb-Hf-Zr-U alloy and the preparation method thereof provided by the invention have the following advantages:
1. due to the addition of the U element, the yield strength of the high-entropy alloy at room temperature is greatly improved compared with that of NbHfZr alloy with a multi-principal-element BCC structure, such as the compressive yield strength of the Nb35-Hf35-Zr10-U15-Al4.99-Cr0.01 alloy with the U content of 15 at.% to 887MPa, and the tensile yield strength of the Nb15-Hf10-Zr10-U50-Al10-Cr5 alloy is improved to 1379MPa after the U content is improved to 50 at.%;
2. the addition of the Al element and the Cr element ensures the strong plasticity to a greater extent, improves the high-temperature oxidation resistance of the alloy, and improves the industrial application value, so that the NbHfZrU high-entropy alloy has good application prospect under the condition of irradiating a nuclear reactor at high temperature;
3. the addition of Hf element improves the mechanical property of the NbHfZrU high-entropy alloy, and the high-thermal neutron absorption section of the alloy also plays a role in regulating and controlling the neutron absorption capacity of the NbHfZrU high-entropy alloy, so that the alloy can be applied to various multi-core field scenes;
4. due to the addition of the high-content U element, the novel Nb-Hf-Zr-U series high-entropy alloy can also be used as nuclear fuel for nuclear reactor application, so that the optimal candidate fuel with high toughness and good anti-irradiation property is provided for the field of metal nuclear fuel, and the structural function integration property is realized.
Claims (3)
1. A uranium-containing element based Nb-Hf-Zr-U system can be used as a structural function integrated high-entropy alloy of nuclear fuel, which is characterized by comprising the following components in atomic percent: niobium: 35-60%; zirconium: 10-35 percent; hafnium: 10-15%; uranium: 15-30%; aluminum: 0.01-10%, and the balance of chromium and inevitable impurities.
2. The structure-function integrated high-entropy alloy based on Nb-Hf-Zr-U system containing uranium elements and used as nuclear fuel according to claim 1 is characterized by comprising the following components in atomic percentage: niobium: 35 percent; zirconium: 10 percent; hafnium: 15 percent; uranium: 30 percent; aluminum: 9.99 percent, and the balance of chromium element and inevitable impurities.
3. The method for preparing the structure-function integrated high-entropy alloy containing uranium elements and used as nuclear fuel based on the Nb-Hf-Zr-U system as claimed in claim 1 or 2, which comprises the following steps:
(1) preparing raw materials: weighing required alloy raw materials according to the Nb-Hf-Zr-U-Al-Cr high-entropy alloy proportion;
(2) arc melting: under the protection of protective gas, rapidly heating and melting Nb, Hf, Zr, U, Al and Cr powder; in order to obtain alloy ingots with uniform components, all samples are repeatedly smelted for five times, and the samples are turned over after each smelting; in order to avoid the influence on the structure and the performance of the sample caused by the melting time and the melting current difference, the current is directly closed after all alloy elements are completely melted into liquid state in each melting of each sample for 1 min; ensure that the surface of all the samples after melting remains bright, i.e. no significant oxidation of the alloy occurs during the melting preparation.
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