CN114350997B - Uranium molybdenum niobium alloy fuel pellet and preparation method and application thereof - Google Patents
Uranium molybdenum niobium alloy fuel pellet and preparation method and application thereof Download PDFInfo
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- CN114350997B CN114350997B CN202111493781.9A CN202111493781A CN114350997B CN 114350997 B CN114350997 B CN 114350997B CN 202111493781 A CN202111493781 A CN 202111493781A CN 114350997 B CN114350997 B CN 114350997B
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- Y02E30/00—Energy generation of nuclear origin
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Abstract
The invention provides a uranium molybdenum niobium alloy fuel pellet and a preparation method and application thereof, wherein the method comprises the following steps: s1: preparing metal uranium ingots into uranium powder by a hydrogenation dehydrogenation method; s2: adding molybdenum powder and niobium powder into uranium powder and uniformly mixing to form uranium molybdenum niobium metal powder, wherein the content of molybdenum is 6-8 wt%, the content of niobium is 1-2 wt%, and then pressing the uranium molybdenum niobium metal powder into a blank under the pressure of 5-8 tons; s3: and (3) putting the blank into a high-temperature heating furnace in an argon atmosphere, heating to 1200-1450 ℃ at the speed of 7-10 ℃/min, preserving heat for 1.5-3 h, then cooling to 800-1000 ℃ at the speed of 7-10 ℃/min, preserving heat for 3-5h, and cooling along with the furnace to finally obtain the gamma-U uranium-molybdenum-niobium alloy fuel pellet. The preparation process of the invention has short period, and realizes the preparation of the uranium molybdenum niobium alloy with stable gamma phase.
Description
Technical Field
The invention relates to the technical field of uranium-based alloy metal fuel pellet preparation, in particular to a uranium-molybdenum-niobium alloy fuel pellet and a preparation method and application thereof.
Background
The uranium-molybdenum alloy has good high-temperature mechanical property and radiation resistance. The common uranium is alpha phase below 668 deg.c, and has poor anticorrosive performance and radiation resistance. It can generate irradiation growth under irradiation conditions. Alpha-uranium is orthorhombic lattice, anisotropic, and under irradiation, the crystal grows anisotropically, the [010] axis of the lattice grows, the [100] axis shortens, and the [001] axis is basically unchanged. The presence of textured uranium can therefore undergo significant changes in macroscopic dimensions, resulting in significant deformation of the fuel element, with a reduction in strength and consequent destruction. Compared with the conventional alpha-phase uranium, the gamma-uranium has greatly improved irradiation stability, and the isotropy of the cubic structure effectively reduces the distortion effect caused by irradiation growth. In order to improve the irradiation stability of the fuel, a uranium alloy is generally formed by adding a small amount of alloy elements into metallic uranium as a fuel material. Molybdenum atoms in the uranium molybdenum alloy have extremely low diffusion speed, so that the thermal activation energy and soaking time of gamma-phase eutectoid reaction are greatly improved, and the metastable gamma uranium with a cubic structure can still be kept after the uranium molybdenum alloy is cooled to room temperature under conventional conditions. Adding enough alloy elements capable of partially or completely stabilizing the gamma phase of the cubic lattice to obtain an isotropic lattice structure and enhance the radiation resistance of the cubic lattice.
Since the function of maintaining the stability of the gamma phase is mainly assumed by the Mo element, the content of the third alloying element is not too high. The primary requirement for this is that the neutron absorption cross section must be small. In order to prevent the melting point from being greatly lowered, the melting point of the alloy element is also required to be relatively high, so that Nb is preferably selected. As an alloy with important application prospect, the uranium molybdenum niobium ternary alloy has been researched by scholars at home and abroad, but a large number of documents do not introduce a detailed preparation process.
At present, the prior art at home and abroad generally adopts methods such as vacuum induction melting, electric arc melting and the like to obtain homogeneous uranium alloy, but has the defect of complex process, needs to be repeatedly melted for many times, has long process period, and increases the risk of material loss and impurity rise. Therefore, a new preparation process is urgently needed to solve the above problems.
Disclosure of Invention
The invention aims to provide a uranium molybdenum niobium alloy fuel pellet as well as a preparation method and application thereof, so as to solve the problems that in the prior art, a uranium molybdenum niobium ternary alloy is prepared by adopting methods such as vacuum induction melting or arc melting, repeated melting is needed for many times, the process period is long, and the risk of material loss and impurity rise is increased.
In order to solve the technical problem, the invention adopts the following technical scheme:
according to a first aspect of the invention, a method for preparing uranium molybdenum niobium alloy fuel pellets is provided, which comprises the following steps: s1: preparing metal uranium ingots into uranium powder by a hydrogenation dehydrogenation method; s2: adding molybdenum powder and niobium powder into the uranium powder and uniformly mixing to form uranium molybdenum niobium metal powder, wherein the content of molybdenum is 6-8 wt%, and the content of niobium is 1-2 wt%, and then pressing the uranium molybdenum niobium metal powder into a blank under the pressure of 5-8 tons; s3: and (3) putting the blank into a high-temperature heating furnace in an argon atmosphere, heating to 1200-1450 ℃ at a speed of 7-10 ℃/min, preserving heat for 1.5-3 h, cooling to 800-1000 ℃ at a speed of 7-10 ℃/min, preserving heat for 3-5h, and cooling to room temperature along with the furnace to finally obtain the gamma-U uranium-molybdenum-niobium alloy fuel pellet.
The step S1 comprises the following steps: and heating the metal uranium ingots to 270-300 ℃ under a hydrogen atmosphere to enable the metal uranium ingots to fall off in the form of hydride powder, completing hydrogenation, and then heating the hydride powder under vacuum to enable hydrogen to be dissociated and released, so that uranium powder is formed.
The step S2 comprises the following steps: and keeping the pressure of 5-8 tons for 4-6min by using a tablet press, and pressing the uranium molybdenum niobium metal powder into a blank with the diameter of 5-15 mm.
The step S3 comprises the following steps: and (3) putting the blank into a tungsten crucible, and then putting the blank into a high-temperature heating furnace for high-temperature treatment.
According to a preferred embodiment of the present invention, step S3 includes: and (3) putting the blank into a high-temperature heating furnace in an argon atmosphere, heating to 1200-1400 ℃ at the speed of 7-10 ℃/min, preserving heat for 2-3h, cooling to 800-1000 ℃ at the speed of 7-10 ℃/min, preserving heat for 3-5h, and cooling to room temperature along with the furnace to finally obtain the gamma-U uranium-molybdenum-niobium alloy fuel pellet.
According to another preferred embodiment of the present invention, step S3 includes: and (3) putting the blank into a high-temperature heating furnace in an argon atmosphere, heating to 1300-1400 ℃ at the speed of 7-10 ℃/min, preserving heat for 2-3h, cooling to 900-1000 ℃ at the speed of 7-10 ℃/min, preserving heat for 3-5h, and cooling to room temperature along with the furnace to finally obtain the gamma-U uranium-molybdenum-niobium alloy fuel pellet.
According to a preferred embodiment of the present invention, step S3 includes: and (3) putting the blank into a high-temperature heating furnace in an argon atmosphere, heating to 1300 ℃ at the speed of 7 ℃/min, preserving heat for 2h, cooling to 1000 ℃ at the speed of 7 ℃/min, preserving heat for 3h, and cooling to room temperature along with the furnace to finally obtain the gamma-U uranium molybdenum niobium alloy fuel pellet.
According to the preparation process provided by the invention, firstly, a metal uranium ingot is prepared into uranium powder by a hydrogenation dehydrogenation method, then molybdenum powder, niobium powder and uranium powder in a certain proportion are uniformly mixed and pre-pressed for forming, and a formed U-Mo-Nb blank is sintered at high temperature under the argon atmosphere and subjected to component homogenization treatment, so that the gamma-U metal fuel pellet is finally obtained. The preparation process provided by the invention has a short period, and the obtained uranium molybdenum niobium fuel pellet has a gamma phase, and the gamma phase is isotropic, so that the irradiation growth of the fuel is greatly reduced, and the prepared metal fuel pellet has better irradiation resistance.
According to a second aspect of the invention there is provided a uranium molybdenum niobium alloy fuel pellet comprising: 6-8wt.% molybdenum, 1-2wt.% niobium, balance uranium and unavoidable impurities; the uranium-molybdenum-niobium alloy fuel pellets contain complete gamma-phase uranium.
According to a third aspect of the invention, there is provided the use of a method of manufacturing pellets of uranium molybdenum niobium alloy as described above in the field of nuclear fuel.
The current commercial nuclear fuel is mainly UO 2 The composite fuel pellet belongs to ceramic fuel, but the uranium loading of the fuel is low, a novel nuclear fuel is researched internationally nowadays, the metal fuel belongs to one of the fuel, the metal material is usually prepared by smelting-heat treatment and other processes, most of the uranium-molybdenum alloy is also prepared into the metal fuel pellet by smelting-sintering, and the invention can also prepare the gamma-phase uranium by a large amount of experiments and finds out the powder solid phase sintering process, and simultaneously directly forms the pellet once. Conventional sintering is typically used below 1000 ℃ for the forming process, while the present invention teaches higher and appropriate temperaturesThe phase of uranium and the pellet molding are changed, and the process is completed at one time. According to the preparation method, the preparation of the gamma-phase stable uranium-molybdenum-niobium alloy is realized by adding Mo and Nb elements in a certain ratio and reasonably controlling process parameters, and finally the metal fuel pellet of the gamma-phase uranium-molybdenum-niobium ternary alloy is prepared.
According to the preparation process provided by the invention, firstly, the highest temperature and the holding time in the step S3 are the most critical, the highest temperature is determined according to the melting point of the alloy and is beyond the melting point of the alloy, and on the other hand, a certain time is needed for Mo and Nb to diffuse and dissolve in U, the higher the temperature is, the faster the diffusion is, the overhigh temperature can cause coarse crystal grains to influence the performance of the alloy, and the invention gropes out a proper range of the highest temperature to be 1200-1450 ℃, and the holding time is 1.5h-3h according to a large number of experiments. Secondly, the content ratio of Mo and Nb in the step S2 is also critical, if the content of Mo and Nb is too low, gamma-U cannot be completely formed, and alpha-U appears, so that the irradiation performance of the fuel is reduced, and if the content of Mo and Nb is too high, mo and Nb which are not completely dissolved form a second phase, so that the uranium loading is reduced. Thirdly, the pressure in the step S2 is the key for forming the powder into the blank, if the pressure is too low, the blank is not dense enough, the blank is seriously oxidized after sintering, and further can not be in the required pellet shape, and the invention finds out the proper pressure to be 5-8 tons according to a large amount of experiments.
In summary, the preparation method of the uranium molybdenum niobium alloy fuel pellet provided by the invention has the following beneficial effects:
1) The uniformity of the components is better: the method adopts a powder solid phase sintering process, prepares uranium powder through a hydrogenation dehydrogenation method, uniformly mixes U-Mo-Nb powder, presses and forms the powder, and then sinters the powder to realize the preparation of the gamma-phase stable uranium-molybdenum-niobium alloy, and meanwhile, the prepared alloy has good component uniformity;
2) The preparation process cycle is shortened: the traditional smelting process needs alloy smelting, alloy powdering and sintering to prepare the gamma-phase metal fuel pellet, while the powder solid phase sintering adopted by the invention can change the phase of uranium and pellet forming by adopting one procedure, so that the gamma-phase uranium molybdenum niobium metal fuel pellet is prepared, the raw material loss is lower, and the process period is shorter.
Drawings
FIG. 1 shows the XRD results of pellets of uranium molybdenum niobium metal fuel prepared in example 1;
FIG. 2 shows the XRD results of pellets of uranium molybdenum niobium metal fuel prepared in comparative example 1;
figure 3 is an XRD result of the uranium molybdenum metal fuel pellets prepared in comparative example 2.
Detailed Description
The present invention will be further described with reference to the following specific examples. It is to be understood that the following examples are illustrative of the present invention only and are not intended to limit the scope of the present invention.
Example 1
Carrying out a hydrogenation experiment on the uranium ingot at the temperature of 280 ℃/1h, closing hydrogen and introducing argon, simultaneously heating to 500 ℃, keeping for 2.5h, and cooling to normal temperature to obtain metal uranium powder.
Preparing U-Mo-Nb powder with the corresponding proportion, wherein the content of molybdenum is 8wt.%, the content of niobium is 1.2wt.%, the balance is uranium and inevitable impurities, uniformly mixing, keeping for 5min at 7tons by using a tablet press, and pressing into a blank with the diameter of 10 mm.
And (3) putting the blank sample into a heating furnace in an argon atmosphere in a glove box, heating to 1300 ℃ at the speed of 7 ℃/min, preserving heat for 2h, cooling to 1000 ℃ at the speed of 7 ℃/min, preserving heat for 3h, cooling to room temperature along with the furnace, and finally preparing the U-Mo-Nb metal fuel pellet.
The XRD results of the uranium molybdenum niobium metal fuel pellets prepared are shown in fig. 1, which are isotropic gamma-U pellets.
Comparative example 1
Carrying out a hydrogenation experiment on the uranium ingot at 280 ℃/1h, closing hydrogen and introducing argon, simultaneously heating to 500 ℃, keeping for 2.5h, and cooling to normal temperature to obtain metal uranium powder.
Preparing U-Mo-Nb powder with the corresponding proportion, wherein the content of molybdenum is 8wt.%, the content of niobium is 1.2wt.%, the balance is uranium and inevitable impurities, uniformly mixing, keeping for 5min at 7tons by using a tablet press, and pressing into a blank with the diameter of 10 mm.
And (3) putting the blank sample into a heating furnace in an argon atmosphere in a glove box, heating to 1100 ℃ at the speed of 7 ℃/min, preserving heat for 2h, cooling to 1000 ℃ at the speed of 7 ℃/min, preserving heat for 3h, cooling to room temperature along with the furnace, and finally preparing the U-Mo-Nb metal fuel pellet.
This comparative example 1, which uses the same uranium molybdenum niobium content and substantially the same experimental conditions as example 1, differs only in that example 1 uses a maximum soak temperature of 1300 c, whereas comparative example 1 uses a maximum soak temperature of 1100 c, and the XRD results of the uranium molybdenum niobium metal fuel pellets produced are shown in fig. 2, from which it is shown that alpha-U is clearly detected in addition to gamma-U, thus indicating that gamma-U cannot be completely formed at a maximum soak temperature of 1100 c. This is because the maximum holding temperature does not allow sufficient time for Mo and Nb to uniformly diffuse and dissolve in U.
Comparative example 2
And (3) carrying out a hydrogenation experiment on the uranium ingot at 280 ℃/1h, closing hydrogen and introducing argon, simultaneously heating to 500 ℃, keeping for 2.5h, and cooling to normal temperature to obtain metal uranium powder.
Adding 8wt.% of molybdenum into uranium powder to obtain U-Mo powder in a corresponding proportion, uniformly mixing, keeping for 5min at 7tons by using a tablet press, and pressing into a blank with the diameter of phi 10 mm.
And (3) putting the blank sample into a heating furnace in an argon atmosphere in a glove box, heating to 1300 ℃ at the speed of 7 ℃/min, preserving heat for 2h, cooling to 1000 ℃ at the speed of 7 ℃/min, preserving heat for 3h, cooling to room temperature along with the furnace, and finally preparing the U-Mo metal fuel pellet.
This comparative example 2 employed substantially the same experimental conditions as in example 1, except that no Nb element was added to this comparative example 2, and the XRD results of the uranium molybdenum metal fuel pellets produced are shown in fig. 3, from which it is shown that α -U appears in addition to γ -U, indicating that the content ratio of the alloying elements also has an important influence on the production of γ -U by the powder solid-phase sintering method.
The above description is only a preferred embodiment of the present invention, and is not intended to limit the scope of the present invention, and various modifications may be made to the above-described embodiment of the present invention. All simple and equivalent changes and modifications made according to the claims and the content of the specification of the present application fall within the scope of the claims of the present patent application. The invention has not been described in detail in order to avoid obscuring the invention.
Claims (8)
1. A preparation method of a uranium molybdenum niobium alloy fuel pellet is characterized by comprising the following steps:
s1: preparing metal uranium ingots into uranium powder by a method of removing hydrogen by hydrogenation, comprising: heating the metal uranium ingot to 270-300 ℃ under a hydrogen atmosphere, so that the metal uranium ingot falls off in the form of hydride powder, completing hydrogenation, and then heating the hydride powder under vacuum to dissociate and release hydrogen, so that uranium powder is formed;
s2: adding molybdenum powder and niobium powder into the uranium powder and uniformly mixing to form uranium molybdenum niobium metal powder, wherein the content of molybdenum is 6-8 wt%, the content of niobium is 1-2 wt%, and then pressing the uranium molybdenum niobium metal powder into a blank under the pressure of 5-8 tons;
s3: and (3) putting the blank into a high-temperature heating furnace in an argon atmosphere, heating to 1200-1450 ℃ at a speed of 7-10 ℃/min, preserving heat for 1.5-3 h, cooling to 800-1000 ℃ at a speed of 7-10 ℃/min, preserving heat for 3-5h, and cooling to room temperature along with the furnace to finally obtain the gamma-U uranium-molybdenum-niobium alloy fuel pellet.
2. The method according to claim 1, wherein step S2 includes: and keeping the pressure of 5-8 tons for 4-6min by using a tablet press, and pressing the uranium molybdenum niobium metal powder into a blank with the diameter of 5-15mm.
3. The method according to claim 1, wherein step S3 includes: and (3) putting the blank into a tungsten crucible, and then putting the blank into a high-temperature heating furnace for high-temperature treatment.
4. The method according to claim 1, wherein step S3 includes: and (3) putting the blank into a high-temperature heating furnace in an argon atmosphere, heating to 1200-1400 ℃ at the speed of 7-10 ℃/min, preserving heat for 2-3h, cooling to 800-1000 ℃ at the speed of 7-10 ℃/min, preserving heat for 3-5h, and cooling to room temperature along with the furnace to finally obtain the gamma-U uranium-molybdenum-niobium alloy fuel pellet.
5. The method according to claim 4, wherein step S3 comprises: and (3) putting the blank into a high-temperature heating furnace in an argon atmosphere, heating to 1300-1400 ℃ at the speed of 7-10 ℃/min, preserving heat for 2-3h, cooling to 900-1000 ℃ at the speed of 7-10 ℃/min, preserving heat for 3-5h, and cooling to room temperature along with the furnace to finally obtain the gamma-U uranium-molybdenum-niobium alloy fuel pellet.
6. The method according to claim 5, wherein step S3 includes: and (3) putting the blank into a high-temperature heating furnace in an argon atmosphere, heating to 1300 ℃ at the speed of 7 ℃/min, preserving heat for 2 hours, cooling to 1000 ℃ at the speed of 7 ℃/min, preserving heat for 3 hours, and then cooling to room temperature along with the furnace to finally obtain the gamma-U uranium-molybdenum-niobium alloy fuel pellet.
7. A uranium molybdenum niobium alloy fuel pellet prepared by the preparation method according to any one of claims 1 to 6, wherein the uranium molybdenum niobium alloy fuel pellet comprises: 6-8wt.% molybdenum, 1-2wt.% niobium, balance uranium and unavoidable impurities; the uranium molybdenum niobium alloy fuel pellets contain complete gamma phase uranium.
8. Use of a method according to any one of claims 1 to 6 in the field of nuclear fuels.
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Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103466568A (en) * | 2013-09-09 | 2013-12-25 | 中国原子能科学研究院 | Preparation method of uranium nitride fuel powder and pellet |
| CN107723554A (en) * | 2017-11-10 | 2018-02-23 | 中国工程物理研究院材料研究所 | A kind of preparation method of uranium niobium molybdenum alloy |
| CN113005372A (en) * | 2019-12-20 | 2021-06-22 | 中核北方核燃料元件有限公司 | Preparation process of pellet with high uranium content |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103466568A (en) * | 2013-09-09 | 2013-12-25 | 中国原子能科学研究院 | Preparation method of uranium nitride fuel powder and pellet |
| CN107723554A (en) * | 2017-11-10 | 2018-02-23 | 中国工程物理研究院材料研究所 | A kind of preparation method of uranium niobium molybdenum alloy |
| CN113005372A (en) * | 2019-12-20 | 2021-06-22 | 中核北方核燃料元件有限公司 | Preparation process of pellet with high uranium content |
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