CN118406951A - Uranium-enriched multi-element uranium alloy and application thereof - Google Patents
Uranium-enriched multi-element uranium alloy and application thereof Download PDFInfo
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- CN118406951A CN118406951A CN202410503297.7A CN202410503297A CN118406951A CN 118406951 A CN118406951 A CN 118406951A CN 202410503297 A CN202410503297 A CN 202410503297A CN 118406951 A CN118406951 A CN 118406951A
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- 229910052770 Uranium Inorganic materials 0.000 title claims abstract description 53
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 title claims abstract description 47
- 229910000711 U alloy Inorganic materials 0.000 title claims abstract description 38
- 229910045601 alloy Inorganic materials 0.000 claims abstract description 71
- 239000000956 alloy Substances 0.000 claims abstract description 71
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims abstract description 30
- 238000003723 Smelting Methods 0.000 claims abstract description 25
- 229910052786 argon Inorganic materials 0.000 claims abstract description 15
- 239000003758 nuclear fuel Substances 0.000 claims abstract description 14
- 239000000203 mixture Substances 0.000 claims abstract description 12
- 238000000034 method Methods 0.000 claims abstract description 10
- 238000013461 design Methods 0.000 claims abstract description 8
- 239000002994 raw material Substances 0.000 claims abstract description 7
- 238000010791 quenching Methods 0.000 claims abstract description 6
- 230000000171 quenching effect Effects 0.000 claims abstract description 6
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 6
- 238000002360 preparation method Methods 0.000 claims abstract description 4
- 238000000137 annealing Methods 0.000 claims abstract description 3
- 238000004321 preservation Methods 0.000 claims abstract description 3
- 230000001681 protective effect Effects 0.000 claims abstract description 3
- 238000005303 weighing Methods 0.000 claims abstract description 3
- 238000002844 melting Methods 0.000 claims description 13
- 230000008018 melting Effects 0.000 claims description 13
- 238000007789 sealing Methods 0.000 claims description 4
- 239000007789 gas Substances 0.000 claims description 2
- 238000001816 cooling Methods 0.000 claims 1
- 238000011160 research Methods 0.000 abstract description 23
- 230000008961 swelling Effects 0.000 abstract description 8
- 239000000446 fuel Substances 0.000 description 10
- 239000000243 solution Substances 0.000 description 10
- 238000001000 micrograph Methods 0.000 description 9
- 239000013078 crystal Substances 0.000 description 8
- 238000000354 decomposition reaction Methods 0.000 description 7
- 238000012360 testing method Methods 0.000 description 7
- 230000004907 flux Effects 0.000 description 6
- XMBWDFGMSWQBCA-UHFFFAOYSA-M iodide Chemical compound [I-] XMBWDFGMSWQBCA-UHFFFAOYSA-M 0.000 description 5
- -1 uranium-silicon-aluminum Chemical compound 0.000 description 5
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 4
- 229910052802 copper Inorganic materials 0.000 description 4
- 239000010949 copper Substances 0.000 description 4
- 229940006461 iodide ion Drugs 0.000 description 4
- 229910052751 metal Inorganic materials 0.000 description 4
- 239000002184 metal Substances 0.000 description 4
- 238000004626 scanning electron microscopy Methods 0.000 description 4
- 230000004992 fission Effects 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 230000000087 stabilizing effect Effects 0.000 description 3
- 229910020018 Nb Zr Inorganic materials 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 210000001787 dendrite Anatomy 0.000 description 2
- 229910001325 element alloy Inorganic materials 0.000 description 2
- 238000009472 formulation Methods 0.000 description 2
- 230000006872 improvement Effects 0.000 description 2
- 230000001678 irradiating effect Effects 0.000 description 2
- 229910052750 molybdenum Inorganic materials 0.000 description 2
- 238000013097 stability assessment Methods 0.000 description 2
- 238000012546 transfer Methods 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 229910020012 Nb—Ti Inorganic materials 0.000 description 1
- WZECUPJJEIXUKY-UHFFFAOYSA-N [O-2].[O-2].[O-2].[U+6] Chemical compound [O-2].[O-2].[O-2].[U+6] WZECUPJJEIXUKY-UHFFFAOYSA-N 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- MVXWAZXVYXTENN-UHFFFAOYSA-N azanylidyneuranium Chemical compound [U]#N MVXWAZXVYXTENN-UHFFFAOYSA-N 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000005520 cutting process Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 230000001939 inductive effect Effects 0.000 description 1
- 229910001068 laves phase Inorganic materials 0.000 description 1
- 150000001247 metal acetylides Chemical class 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- KTEXACXVPZFITO-UHFFFAOYSA-N molybdenum uranium Chemical compound [Mo].[U] KTEXACXVPZFITO-UHFFFAOYSA-N 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 238000005204 segregation Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000010301 surface-oxidation reaction Methods 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- 229910000439 uranium oxide Inorganic materials 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
Classifications
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
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- Manufacture And Refinement Of Metals (AREA)
Abstract
The invention discloses a uranium-enriched multi-element uranium alloy, a preparation method and application thereof, wherein the multi-element uranium alloy is proportioned according to the form of an expression U x MoZrNb, x is more than or equal to 4.5 and less than or equal to 6.0, and atomic percentages of Mo element, zr element and Nb element are equal. The preparation method comprises the steps of S1, designing the composition of U x MoZrNb according to the design requirement of a reactor core, weighing the proportioned alloy raw materials, and preparing uranium alloy ingots with uniform components by adopting a plurality of vacuum smelting methods; and S2, annealing the U x MoZrNb alloy cast ingot prepared in the step S1 in vacuum or argon protective atmosphere, and directly performing water quenching after heat preservation is finished. The uranium alloy disclosed by the invention has the advantages of considering the uranium density, the high-temperature structural stability and the anti-irradiation swelling performance, and can meet the use requirement of a high-flux research stack on nuclear fuel.
Description
Technical Field
The invention belongs to the technical field of nuclear fuel, and particularly relates to a uranium-enriched multi-element uranium alloy and application thereof.
Background
In research reactors pursuing high neutron flux and power reactors pursuing high power density, nuclear fuels should possess high uranium density, good heat transfer capacity and irradiation stability so that the core attains as high a fission density and neutron flux as possible to accelerate material irradiation experiments. The uranium density of uranium-silicon-aluminum dispersion fuel widely used in the research reactor at present is low, and the design requirement of a novel research reactor pursuing higher neutron flux is difficult to meet. While uranium-molybdenum metal nuclear fuels for research stacks developed in the united states, korea and the like have a relatively high uranium density, a key problem faced by the nuclear fuels is that phase transformation occurs below 600 ℃, which causes decomposition of body-centered cubic structure crystals (gamma phase) to generate anisotropic hexagonal closest packed crystals (alpha phase), thereby inducing irradiation deformation and irradiation swelling of the metal fuel to be intensified, threatening the structural integrity of the research stack fuel, and thus the application temperature of the nuclear fuel in the research stack is limited to below 200 ℃.
In order to further increase the upper limit of the use temperature of the research stack fuel, it is desirable to modify the metal fuel composition so that it remains gamma-phase stable at higher temperatures while retaining the advantages of its high uranium density, high heat transfer capability. The prior research shows that the improvement of the configuration entropy by adding various alloy elements is feasible for stabilizing the gamma phase, for example, the Chinese engineering physical institute researches U-Hf-Nb-Ti quaternary high-entropy alloy to improve the mechanical property and maintain the body-centered cubic structure (J.Shi,Y et al,Development of single-phase bcc UHfNbTi high-entropy alloy with excellent mechanical properties,Materials Letters(2021)),, but the U atom share of uranium alloy in the research is lower (not more than 35%), the alloy elements are excessive, the uranium content is lower than that of uranium nitride, uranium oxide and other ceramic fuels, and the requirement of high-flux research reactor core design on the uranium density of the nuclear fuel is difficult to meet.
In view of this, the present patent application is presented.
Disclosure of Invention
In order to solve the problems, the invention aims to provide a uranium-enriched multi-element uranium alloy and application thereof, the uranium density of the obtained uranium alloy is not less than 11.68gU/cm 3, the requirement of a high-flux research reactor on nuclear fuel uranium density can be met, and meanwhile, a body-centered cubic crystal structure can be maintained in a reactor operating temperature range (200 ℃ -500 ℃), so that the uranium-enriched multi-element uranium alloy has better irradiation swelling resistance, is beneficial to improving the operating temperature and burnup of a fuel element for the research reactor, and takes the uranium density, high-temperature structural stability and irradiation swelling resistance into consideration.
The invention aims at solving the technical problems by adopting the following technical scheme:
The first aim of the invention is to provide a uranium-enriched multi-element uranium alloy, wherein the multi-element uranium alloy comprises the following components in a form of an expression U x MoZrNb, x is more than or equal to 4.5 and less than or equal to 6.0, and the atomic percentages of Mo element, zr element and Nb element are equal. The microstructure of the uranium-rich multi-element alloy disclosed by the formula of the invention is characterized by a body-centered cubic single-phase structure. By adding Mo, nb and Zr elements with strong capability of stabilizing the U-atom body-centered cubic structure and controlling the components of the three elements to be equal atomic percent, the configuration entropy of the maximum alloy system under the same total atomic ratio of doped elements has a single gamma phase (namely body-centered cubic structure), reduces the possibility of precipitation of Laves phase, and can still keep good gamma phase stability after long-time examination and irradiation test at high temperature.
And the inventors found that if the U content is increased, the content of the alloy element for stabilizing the gamma phase is correspondingly reduced, and the effect of maintaining the stability of the gamma phase cannot be achieved. If the U content is too low, the nuclear design requirements of the research reactor cannot be met, because the lower the U content is, the lower the atomic density is, the lower the amount of nuclear fission reaction (namely, the fission reaction density) capable of occurring in a unit space is, so that the power density and neutron flux of the nuclear reactor are correspondingly reduced, and the design requirements of the high-flux research reactor are difficult to meet. Therefore, the design objective of the application is to improve the gamma phase thermal stability and the U content. The thinking of solving the technical problem provided by the application is that three additive elements are selected and kept to be equal atomic ratio, so that the alloy configuration entropy of the alloy is maximized (S conf＝Xiln(Xi) under the same U content, and the free energy of a high-temperature phase of the alloy is lower, namely the alloy is more stable according to an alloy free energy formula of material thermodynamics. The person skilled in the art is not able to obtain the formulation according to the application by simple, limited number of formulation adjustments.
The uranium density of the uranium-enriched multi-element uranium alloy U x MoZrNb (x is more than or equal to 4.5 and less than or equal to 6.0) obtained by the embodiment of the invention is more than or equal to 11.68gU/cm 3, the requirement of a research reactor on the uranium density of nuclear fuel can be met, the neutron flux of the core of the research reactor can be improved, and meanwhile, the body-centered cubic crystal structure can be better maintained at high temperature (200-500 ℃), so that the uranium-enriched multi-element uranium alloy U x MoZrNb has better irradiation swelling resistance, and the operating temperature and burnup of the fuel element for the research reactor can be improved. The uranium-enriched multi-element uranium alloy disclosed by the invention has the advantages of high uranium density, high-temperature structural stability and irradiation swelling resistance, and solves the problem that the nuclear fuel for stacking cannot be satisfied when the uranium content is low.
In an alternative embodiment, the following steps are used:
step S1, designing the composition of U x MoZrNb and the proportion of each element according to the design requirement of a reactor core, weighing the proportioned alloy raw materials, and preparing uranium alloy ingots with uniform components by adopting a plurality of vacuum smelting methods;
and S2, annealing the U x MoZrNb alloy cast ingot prepared in the step S1 in vacuum or argon protective atmosphere, and directly performing water quenching after heat preservation is finished.
In an alternative embodiment, in step S1, the elemental substances of U, mo, nb, zr elements are 83.1%, 5.8%, 5.6% and 5.5% by weight, respectively, when the master alloy is mixed.
In an alternative embodiment, when the master alloy is melted in step S2, the melting is performed under the protection of argon gas by using a vacuum arc melting method.
In an alternative embodiment, the master alloy is vacuumized to a furnace chamber pressure of below 5X 10 -3 Pa before vacuum smelting, and then 0.6-0.8 atmosphere high-purity argon with the weight percent purity of 99.999 percent is filled into the furnace chamber.
In an alternative embodiment, in step S2, the argon arc melting current is controlled to be 350A-450A, and the melting time is 5min. The invention can melt rapidly, avoid volatilization of low melting point elements, avoid component change and obtain uniform components. In an alternative embodiment, after the smelting is finished, waiting for 10min to cool the alloy to room temperature, then turning over the primary blank, and repeating the steps for smelting for 3-5 times to obtain a mother alloy ingot with uniform components.
In an alternative embodiment, in step S2, after the master alloy ingot is subjected to vacuum tube sealing treatment, the master alloy ingot is subjected to solution treatment at a high temperature of 1000 ℃ for 80 hours, so as to obtain a homogenized alloy ingot, and the alloy ingot is directly subjected to water quenching. According to the application, the dendrite structure of the alloy ingot is eliminated by solution treatment at 1000 ℃, so that elements such as Mo, zr, nb and the like are more uniform.
In the embodiment of the invention, the conventional vacuum arc melting and vacuum heat treatment are adopted, the preparation method is simple, the obtained alloy components are uniformly distributed, dendrite segregation is avoided in the crystal grains, and compared with the conventional melting method, the composition of the multi-element alloy can be controlled more accurately, and the introduced elements such as oxygen, carbon and the like are prevented from entering the alloy to form oxides and carbides in the air.
A second object of the invention is to provide the use of a uranium-enriched transuranic alloy as described in any of the preceding claims in a nuclear fuel.
Compared with the prior art, the invention has the following advantages and beneficial effects:
the uranium density of the uranium-enriched multi-element uranium alloy U x MoZrNb (x is more than or equal to 4.5 and less than or equal to 6.0) provided by the embodiment of the invention is more than or equal to 11.68gU/cm 3, the requirement of a research reactor on the uranium density of nuclear fuel can be met, the neutron flux of the core of the research reactor can be improved, and meanwhile, the body-centered cubic crystal structure (namely gamma phase) can be better maintained at high temperature (200-500 ℃), so that the uranium-enriched multi-element uranium alloy U x MoZrNb has better irradiation swelling resistance, and the operating temperature and the burnup of the fuel element for the research reactor are improved.
The uranium-enriched multi-element uranium alloy disclosed by the invention has the advantages of high uranium density, high-temperature structural stability and irradiation swelling resistance, and solves the problem that the nuclear fuel for stacking cannot be satisfied when the uranium content is low.
Drawings
In order to more clearly illustrate the technical solutions of the exemplary embodiments of the present invention, the drawings that are needed in the examples will be briefly described below, it being understood that the following drawings only illustrate some examples of the present invention and therefore should not be considered as limiting the scope, and that other related drawings may be obtained from these drawings without inventive effort for a person skilled in the art. In the drawings:
Fig. 1 is an XRD test pattern of the quenched sample obtained in example 1.
FIG. 2 is a scanning electron microscope image obtained by performing thermal stability examination at 460℃for 10 hours on the quenched sample obtained in example 1.
FIG. 3 is a scanning electron microscope image obtained by performing thermal stability examination on the U-10Mo alloy at 460 ℃ for 10 h.
FIG. 4 is a scanning electron microscope image obtained by irradiating a quenched sample obtained in example 1 with iodide ions at 400℃for 5 hours.
FIG. 5 is a scanning electron microscope image obtained after the U-10Mo alloy is subjected to iodide ion irradiation at 400 ℃ for 5 hours.
FIG. 6 is a scanning electron microscope image obtained by subjecting the quenched sample obtained in example 1 to iodide ion irradiation at 500℃for 5 hours.
FIG. 7 is a scanning electron microscope image obtained after the U-10Mo alloy is subjected to iodide ion irradiation at 500 ℃ for 5 hours.
Fig. 8 is an XRD test pattern of the quenched sample obtained in example 2.
FIG. 9 is a scanning electron microscope image obtained by performing thermal stability examination at 460℃for 10 hours on the quenched sample obtained in example 2.
FIG. 10 is a scanning electron microscope image obtained by irradiating a quenched sample obtained in example 2 with iodide ions at 400℃for 5 hours.
FIG. 11 is a scanning electron microscope image obtained by subjecting the quenched sample obtained in example 2 to iodide ion irradiation at 500℃for 5 hours.
Detailed Description
The present invention will be described in further detail with reference to the following examples, for the purpose of making the objects, technical solutions and advantages of the present invention more apparent, and the description thereof is merely illustrative of the present invention and not intended to be limiting.
In the following description, numerous specific details are set forth in order to provide a thorough understanding of the present invention. However, it will be apparent to one of ordinary skill in the art that: no such specific details are necessary to practice the invention. In other instances, well-known methods have not been described in detail in order to avoid obscuring the present invention.
Example 1: u 5.8 MoNbZr alloy
(1) Mixture ratio
According to the atomic percentage of the alloy components, the alloy components are converted into 83.1 percent, 5.8 percent, 5.6 percent and 5.5 percent by weight respectively, U, mo, nb, zr percent of raw materials are weighed, wherein the purity of the U by weight percent is more than 99.5 percent, and the purity of the other raw materials by weight percent is more than 99.95 percent. The quality deviation is controlled within 0.5mg when the components are configured.
(2) Master alloy ingot smelting
And smelting by adopting a non-consumable arc smelting method under the protection of argon. First, the prepared U-Mo-Nb-Zr mixture was placed in a copper crucible of an arc melting furnace. The furnace chamber is then evacuated to below 5x10 -3 Pa. Then 0.6 atmosphere pressure and 99.999 percent by weight of high-purity argon are filled into the smelting chamber. And finally, argon arc smelting is carried out, the current is controlled at 350A, and the smelting time is 5min. And after the smelting is finished, waiting for the alloy to cool to room temperature to obtain a primary blank, turning over the primary blank, putting the primary blank into a water-cooled copper crucible again, and repeating the smelting steps for 5 times to obtain a mother alloy ingot with uniform components.
(3) Alloy solution treatment
In order to obtain uranium alloy with uniform components, vacuum tube sealing treatment is carried out on a master alloy ingot, the solution treatment temperature is 1000 ℃, water quenching is directly carried out after 80 hours, and finally a quenched sample is obtained.
(4) Performance testing
The sample was subjected to a crystal structure test using XRD technique. Figure 1 shows the XRD results of the uranium alloy of example 1, in which sharp diffraction peaks were observed, indicating that a single body-centered cubic phase was obtained after solution treatment.
Thermal stability assessment:
After the quenched alloy ingot in the step (3) is sealed again, checking the thermal stability at 460 ℃ for 10 hours, corroding the checked sample by 5%H 3PO4 aqueous solution (volume fraction), and then carrying out phase identification and scanning electron microscope observation.
FIG. 2 shows the microstructure obtained by scanning electron microscopy at 460℃after 10 hours. It can be seen that the uranium-enriched transuranic alloy U 5.8 MoNbZr alloy does not undergo gamma-phase decomposition, whereas the U-10Mo alloy (Mo mass content 10%, see fig. 3) is in the same condition. Discontinuous precipitated lamellar structure of gamma-phase decomposition appears near the grain boundary, which indicates that the former has good gamma-phase thermal stability. Among them, U-10Mo is a new generation of research heap metal fuel developed in the United states and Japanese and Korean, has good irradiation performance and gamma phase stability, and comprises 10% of Mo and 90% of U by mass.
Irradiation stability assessment:
And (3) cutting the quenched alloy ingot in the step (3), respectively carrying out iodine ion irradiation at 400 ℃ and 500 ℃ for 5 hours under vacuum, and carrying out phase identification and scanning electron microscope observation on the irradiated sample to judge the capability of maintaining gamma-phase stability under high-temperature irradiation conditions. Fig. 4 and 6 show the microstructure of the irradiated regions obtained by scanning electron microscopy after the irradiation of iodide ions at 400 c and 500 c for 5 hours, respectively. By comparison with U-10Mo (Mo content 10% by mass) (corresponding to FIGS. 5 and 7, respectively), it can be seen that the U 5.8 MoNbZr alloy does not undergo decomposition of the gamma phase despite the presence of a smelting non-uniform microstructure. And under the same conditions, the U-10Mo alloy has discontinuous precipitated lamellar structure of gamma-phase decomposition near the grain boundary, which shows that the U 5.8 MoNbZr of the uranium-enriched multi-element uranium alloy has good gamma-phase stability under the high-temperature irradiation condition compared with the U-10Mo alloy.
Example 2: u 4.5 MoNbZr alloy
(1) Mixture ratio
According to the atomic percentage of the alloy components, the alloy components are converted into 83.1 percent, 5.8 percent, 5.6 percent and 5.5 percent by weight respectively, U, mo, nb, zr percent of raw materials are weighed, wherein the purity of the U by weight percent is more than 99.5 percent, and the purity of the other raw materials by weight percent is more than 99.95 percent. The quality deviation is controlled within 0.5mg when the components are configured.
(2) Master alloy ingot smelting
And smelting by adopting a non-consumable arc smelting method under the protection of argon. First, the prepared U-Mo-Nb-Zr mixture was placed in a copper crucible of an arc melting furnace. The furnace chamber is then evacuated to below 5x10 -3 Pa. Then 0.8 atmosphere pressure and 99.999 percent by weight of high-purity argon are filled into the smelting chamber. Finally, argon arc smelting is carried out, the current is controlled at 450A, and the smelting time is 5min. And after the smelting is finished, waiting for the alloy to cool to room temperature to obtain a primary blank, turning over the primary blank, putting the primary blank into a water-cooled copper crucible again, and repeating the smelting steps for 5 times to obtain a mother alloy ingot with uniform components.
(3) Alloy solution treatment
In order to obtain uranium alloy with uniform components, vacuum tube sealing treatment is carried out on a master alloy ingot, the solution treatment temperature is 1000 ℃, water quenching is directly carried out after 80 hours, and finally a quenched sample is obtained.
(4) Performance testing
The sample was subjected to a crystal structure test using XRD technique. Figure 8 shows the XRD results of the uranium alloy of example 2, in which sharp gamma-phase diffraction peaks and minor amounts of surface oxidation-induced UO 2 diffraction peaks were observed, indicating that a single body-centered cubic phase was obtained after solution treatment.
FIG. 9 shows the microstructure obtained by scanning electron microscopy at 460℃after 10 hours. It can be seen that the uranium-enriched multi-uranium alloy U 4.5 MoNbZr alloy does not undergo gamma-phase decomposition. Fig. 10 and 11 show the microstructure of the irradiated regions obtained by scanning electron microscopy after the irradiation of iodide ions at 400 c and 500 c for 5 hours, respectively. By comparison with U-10Mo (Mo content 10% by mass) (corresponding to FIGS. 5 and 7, respectively), it can be seen that the U 4.5 MoNbZr alloy also has a microstructure that is not uniformly melted, but does not undergo decomposition of the gamma phase as such. Compared with the microstructure of the U-10Mo alloy under the same condition, the uranium-enriched multi-element uranium alloy U 4.5 MoNbZr has better gamma-phase stability under the high-temperature irradiation condition than the U-10Mo alloy.
The foregoing detailed description of the invention has been presented for purposes of illustration and description, and it should be understood that the invention is not limited to the particular embodiments disclosed, but is intended to cover all modifications, equivalents, alternatives, and improvements within the spirit and principles of the invention.
Claims (10)
1. The uranium-enriched multi-element uranium alloy is characterized in that the multi-element uranium alloy is proportioned according to the expression U x MoZrNb, x is more than or equal to 4.5 and less than or equal to 6.0, and the atomic percentages of Mo element, zr element and Nb element are equal.
2. The uranium-enriched multi-element uranium alloy according to claim 1, wherein elements U, mo, nb, zr are mixed in proportions of 83.1%, 5.8%, 5.6% and 5.5% by weight.
3. A uranium rich multi-element uranium alloy according to any one of claims 1 to 2 and characterised in that: the preparation method comprises the following steps:
step S1, designing the composition of U x MoZrNb and the proportion of each element according to the design requirement of a reactor core, weighing the proportioned alloy raw materials, and preparing uranium alloy ingots with uniform components by adopting a plurality of vacuum smelting methods;
and S2, annealing the U x MoZrNb alloy cast ingot prepared in the step S1 in vacuum or argon protective atmosphere, and directly performing water quenching after heat preservation is finished.
4. A uranium rich multi-element uranium alloy according to claim 3, wherein in step S1, elements U, mo, nb, zr are 83.1%, 5.8%, 5.6% and 5.5% by weight, respectively, of the master alloy.
5. A uranium rich multi-element uranium alloy according to claim 3, wherein the master alloy is melted in step S1 by vacuum arc melting under argon.
6. A uranium enriched multi-element uranium alloy according to claim 3, wherein prior to vacuum melting of the master alloy, vacuum is applied to a furnace chamber at a pressure of 5 x 10 -3 Pa or less, and then high purity argon gas having a weight percentage purity of 99.999% is introduced into the furnace chamber at a pressure of 0.6 to 0.8 atmospheres.
7. A uranium rich multi-element uranium alloy according to claim 3, wherein in step S1, argon arc melting current is controlled to be 350-450A, and melting time is 5min.
8. The uranium rich multi-element uranium alloy according to claim 7, wherein after the smelting is completed, the alloy is cooled to room temperature for 10min, the primary blank is turned over, and the above steps are repeated for smelting for 3 to 5 times to obtain a mother alloy ingot with uniform composition.
9. A uranium enriched multi-element uranium alloy according to claim 3, wherein in step S2, after the mother alloy ingot is subjected to vacuum tube sealing treatment, the mother alloy ingot is subjected to solution treatment at a high temperature of 1000 ℃ or higher for not less than 80 hours to obtain a homogenized alloy ingot, and the alloy ingot is directly subjected to rapid cooling.
10. Use of a uranium-enriched transuranic alloy according to any one of claims 1 to 9 in nuclear fuel.
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