CN108417278B - Preparation method of metal type fuel pellet with high irradiation stability - Google Patents

Preparation method of metal type fuel pellet with high irradiation stability Download PDF

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Publication number
CN108417278B
CN108417278B CN201810100350.3A CN201810100350A CN108417278B CN 108417278 B CN108417278 B CN 108417278B CN 201810100350 A CN201810100350 A CN 201810100350A CN 108417278 B CN108417278 B CN 108417278B
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sintering
fuel pellet
metal type
type fuel
mixed powder
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CN108417278A (en
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高瑞
杨振亮
李冰清
张鹏程
褚明福
唐浩
钟毅
刘徐徐
段丽美
黄奇奇
王志毅
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    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21C—NUCLEAR REACTORS
    • G21C3/00—Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
    • G21C3/42—Selection of substances for use as reactor fuel
    • G21C3/58—Solid reactor fuel Pellets made of fissile material
    • G21C3/60—Metallic fuel; Intermetallic dispersions
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21C—NUCLEAR REACTORS
    • G21C21/00—Apparatus or processes specially adapted to the manufacture of reactors or parts thereof
    • G21C21/02—Manufacture of fuel elements or breeder elements contained in non-active casings
    • G21C21/16—Manufacture of fuel elements or breeder elements contained in non-active casings by casting or dipping techniques
    • 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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  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • Plasma & Fusion (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical & Material Sciences (AREA)
  • Dispersion Chemistry (AREA)
  • Powder Metallurgy (AREA)

Abstract

The invention discloses a preparation method of a metal type fuel pellet with high irradiation stability, which comprises the following steps: mixing uranium-based alloy powder and a carbon-based nano material according to a volume ratio of 99.9-99:1-0.1, placing the mixture in a nylon ball milling tank, adding 3 times of zirconia grinding balls by mass, and mixing for 24 hours to obtain mixed powder; step two: and carrying out pressureless sintering, hot-pressing sintering, spark plasma sintering or flash firing on the mixed powder, cooling along with the furnace after the heat preservation and pressure preservation are finished, taking out, and carrying out machining forming to obtain the metal type fuel pellet. The metallic fuel pellet prepared by the method has the advantages of high uranium loading, high heat conduction, good irradiation resistance, strong fission gas containing capacity and excellent mechanical property, and can be used as a novel nuclear fuel of a nuclear reactor.

Description

Preparation method of metal type fuel pellet with high irradiation stability
Technical Field
The invention relates to a preparation method of a metal type fuel pellet with high irradiation stability.
Background
Relative to the UO most commonly used in commercial reactors2The fuel, metal type nuclear fuel based on uranium-based alloy has the advantages of high uranium content and high heat conductivity, but the metal type nuclear fuel has larger swelling under irradiation conditionDeformation, thus limiting the application of this type of core block in nuclear reactors.
Disclosure of Invention
The invention aims to solve the technical problems and provides a preparation method of a metal type fuel pellet, which improves the thermal physical property, the mechanical property and the irradiation stability of the metal type fuel pellet so as to enable the core pellet to have the conditions applied in a nuclear reactor.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
a method for preparing a metal type fuel pellet with high irradiation stability comprises the following steps,
the method comprises the following steps: mixing uranium-based alloy powder and a carbon-based nano material according to a volume ratio of 99.9-99:1-0.1, placing the mixture in a nylon ball milling tank, adding 3 times of zirconia grinding balls by mass, and mixing for 24 hours to obtain mixed powder;
step two: and carrying out pressureless sintering, hot-pressing sintering, spark plasma sintering or flash firing on the mixed powder, cooling along with the furnace after the heat preservation and pressure preservation are finished, taking out, and carrying out machining forming to obtain the metal type fuel pellet.
Specifically, the uranium-based alloy is U-Mo, U-Zr or U3Si2The grain diameter is 5-100 μm,235the U enrichment degree is 1-5%.
Specifically, the carbon-based nano material is any one or more of the following materials: SiC particles with the particle size of 20nm-2 mu m, SiC whiskers with the diameter of 20nm-200nm and the length of 5-20 mu m, carbon nanotubes with the diameter of 5nm-100nm and the length of 1-20 mu m, and graphene with the plane length of 100nm-200 mu m.
Further, in the second step, when the sintering mode is pressureless sintering, the steps are as follows: the mixed powder is molded under the condition of 100-400MPa to obtain a fuel pellet biscuit, the fuel pellet biscuit is placed in an atmosphere sintering furnace, the temperature is raised to a certain temperature at the speed of 1-10 ℃/min, the temperature is preserved for 30-60min, the temperature is raised to 800-1200 ℃ at the speed of 1-10 ℃/min, and the temperature is preserved for 1-5 h; the atmosphere is vacuum or argon atmosphere protection.
As another sintering method, the stepsIn the second step, when the sintering mode is hot-pressing sintering, the steps are as follows: placing the mixed powder in a graphite mold, and vacuumizing to 5 × 10-2-5×10-1Pa, heating to 800-1200 ℃ at the speed of 1-20 ℃/min under the condition of sintering pressure of 20-100MPa, and preserving heat for 1-4 h; the sintering atmosphere is argon atmosphere.
As another sintering method, in the second step, when the sintering method is spark plasma sintering, the steps are as follows: placing the mixed powder in a graphite mold, and vacuumizing to 5 × 10-2-5×10-1Pa, then filling argon to 10-60 kPa; heating to 700-1200 ℃ at the speed of 50-1000 ℃/min under the sintering pressure condition of 20-100MPa, and preserving the heat for 1-30 min.
As another sintering method, in the second step, when the sintering method is flash firing, the steps are as follows: placing the mixed powder in graphite or metal mold, and vacuumizing to 5 × 10-2-5×10-1Pa, then filling argon to 10-60 kPa; heating to 700-1200 ℃ at the speed of 400-2000 ℃/min, and keeping the temperature for 10s-5 min.
Compared with the prior art, the invention has the following beneficial effects:
according to the invention, the dispersed carbon-based nano material is added into the metal type fuel pellet to be compounded with the uranium-based alloy powder, and the carbon-based nano material is dispersed in the metal fuel, takes the carbon-based nano material as a core, can form abundant structural defects at the periphery, and can effectively resist irradiation deformation and contain fission gas. In addition, because the nano dispersion is enhanced, the tensile stress and the bending stress can be better resisted, and better mechanical properties can be obtained.
Therefore, the method can prepare the metal type fuel pellet with high uranium loading, high heat conduction, good radiation resistance, strong fission gas containing capacity and excellent mechanical property, so that the type of pellet has the condition of being applied in a nuclear reactor and can be used as novel nuclear fuel of the nuclear reactor.
Detailed Description
The present invention is further illustrated by the following examples, which include, but are not limited to, the following examples.
The following examples illustrate the method of making the metallic fuel pellet of the present invention.
Example 1
Step one, raw materials are proportioned according to the following mode:
U-10M alloy powder, 5-100 μ M,2351-5% of U enrichment degree, 99 vol% of silicon carbide particles with the particle size of 10-100 nm, 1 vol% of the silicon carbide particles, placing the powder in a nylon ball milling tank, adding 3 times of zirconia grinding balls by mass, and mixing for 24 hours.
Step two, sintering is carried out according to the following mode:
and carrying out die pressing forming on the mixed powder to obtain a fuel pellet biscuit, wherein the forming pressure is 100Mpa, the biscuit is placed in an atmosphere sintering furnace for pressureless sintering, the temperature is firstly increased to about 600 ℃ at the speed of 5-10 ℃/min and is preserved for 0.5h, the temperature is increased to 1100 ℃ at the speed of 1 ℃/min and is preserved for 2h, the furnace is cooled, the atmosphere is argon atmosphere, and the pressure is 10-50 kPa.
And step three, taking out the sample after furnace cooling, and processing the sample to the required shape and size.
Example 2
Step one, raw materials are proportioned according to the following mode:
5-100 mu m of U-10Zr alloy powder,2351-5% of U enrichment, 99.9 vol%, SiC whiskers with the diameter of 20-200 nm and the length of 5-20 mu m and 0.1 vol%, placing the powder in a nylon ball milling tank, adding 3 times of zirconia grinding balls by mass, and mixing for 24 hours.
Step two, sintering is carried out according to the following mode:
and (3) carrying out die pressing forming on the mixed powder to obtain a fuel pellet biscuit, wherein the forming pressure is 300Mpa, placing the biscuit in an atmosphere sintering furnace for pressureless sintering, firstly heating to about 500 ℃ at the speed of 5-10 ℃/min, and preserving heat for 0.5 h. Heating to 850 deg.C at a rate of 1 deg.C/min, maintaining for 1 hr, cooling in a vacuum atmosphere at a pressure of 5 × 10-2～5×10-1Pa。
And step three, taking out the sample after furnace cooling, and processing the sample to the required shape and size.
Example 3
Step one, raw materials are proportioned according to the following mode:
U3Si25-100 mu m of alloy powder,235the U enrichment degree is 1-5%, 95 vol%, the diameter is 5nm-100nm, the length is 1-20 mu m, 5 vol%, the powder is placed in a nylon ball milling tank, 3 times of the mass of zirconia grinding balls are added, and the mixture is mixed for 24 hours.
Step two, sintering is carried out according to the following mode:
putting the powder into a designed graphite die, and carrying out hot-pressing sintering, wherein the sintering process comprises the following steps: heating to 800 ℃ at the speed of 1-20 ℃/min, preserving heat for 1h, applying sintering pressure of 20MPa, cooling the furnace after heat preservation and pressure maintaining are finished, and adopting argon as sintering atmosphere.
And step three, taking out the sample after furnace cooling, and processing the sample to the required shape and size.
Example 4
Step one, raw materials are proportioned according to the following mode:
u-10Mo alloy powder, 5-100 μm,235the U enrichment degree is 1-5%, 99 vol%, the planar length of graphene is 100nm-200 mu m, and 1 vol%, the powder is placed in a nylon ball milling tank, zirconium oxide grinding balls with the mass being 3 times that of the powder are added, and the mixture is mixed for 24 hours.
Step two, sintering is carried out according to the following mode:
putting the powder into a designed graphite die, and carrying out hot-pressing sintering, wherein the sintering process comprises the following steps: heating to 1100 ℃ at the speed of 1-20 ℃/min, preserving heat for 2h, applying sintering pressure of 40MPa, and cooling in a furnace after heat preservation and pressure maintaining are finished, wherein the sintering atmosphere is argon.
And step three, taking out the sample after furnace cooling, and processing the sample to the required shape and size.
Example 5
Step one, raw materials are proportioned according to the following mode:
5-100 mu m of U-10Zr alloy powder,235the U enrichment degree is 1-5%, 99.9 vol%, the diameter is 5nm-100nm, the length is 1-20 mu m carbon nano tube, 0.1 vol%, the powder is placed in a nylon ball milling tank, 3 times of the mass of zirconia grinding balls are added, and the mixture is mixed for 24 hours.
Step two, sintering is carried out according to the following mode:
placing the powder in a designed graphite die, and performing spark plasma sintering, wherein the sintering process comprises the following steps: vacuum-pumping to 5 × 10-2～5×10-1Pa, and then filling argon to 10-60 kPa; heating to 700 deg.C at a rate of 50 deg.C/min, sintering at 20MPa for 30min, cooling
And step three, taking out the sample after furnace cooling, and processing the sample to the required shape and size.
Example 6
Step one, raw materials are proportioned according to the following mode:
U3Si25-100 mu m of alloy powder,235the U enrichment degree is 1-5%, 95 vol%, the planar length of graphene is 100nm-200 mu m, and 5 vol%, the powder is placed in a nylon ball milling tank, zirconium oxide grinding balls with the mass being 3 times that of the powder are added, and the mixture is mixed for 24 hours.
Step two, sintering is carried out according to the following mode:
placing the powder in a designed graphite die, and performing spark plasma sintering, wherein the sintering process comprises the following steps: vacuum-pumping to 5 × 10-2～5×10-1Pa, and then filling argon to 10-60 kPa; heating to 1200 ℃ at the speed of 1000 ℃/min, keeping the sintering pressure at 100MPa, keeping the temperature for 1min, and cooling the furnace after the heat preservation and pressure keeping are finished.
And step three, taking out the sample after furnace cooling, and processing the sample to the required shape and size.
Example 7
Step one, raw materials are proportioned according to the following mode:
u-10Mo alloy powder, 5-100 μm,235the U enrichment degree is 1-5%, 99.9 vol%, SiC particles with the particle size of 20nm-2 mu m and 0.1 vol%, the powder is placed in a nylon ball milling tank, zirconium oxide grinding balls with the mass being 3 times that of the powder are added, and the mixture is mixed for 24 hours.
Step two, sintering is carried out according to the following mode:
placing the powder in a designed graphite or metal die, and carrying out flash sintering, wherein the sintering process is as follows: vacuum-pumping to 5 × 10-2～5×10-1Pa, and then filling argon to 10-60 kPa; heating to 800 deg.C at a rate of 400 deg.C/min, sintering at 20MPa, maintaining the temperature for 0.1min, and cooling
And step three, taking out the sample after furnace cooling, and processing the sample to the required shape and size.
Example 8
Step one, raw materials are proportioned according to the following mode:
u-10Mo alloy powder, 5-100 μm,2351-5% of U enrichment, 95 vol%, SiC whiskers with the diameter of 20-200 nm and the length of 5-20 mu m and 5 vol%, placing the powder in a nylon ball milling tank, adding 3 times of zirconia grinding balls by mass, and mixing for 24 hours.
Step two, sintering is carried out according to the following mode:
placing the powder in a designed graphite or metal die, and carrying out flash sintering, wherein the sintering process is as follows: vacuum-pumping to 5 × 10-2～5×10-1Pa, and then filling argon to 10-60 kPa; heating to 1200 ℃ at a speed of 2000 ℃/min, keeping the sintering pressure at 100MPa for 2min, and cooling the furnace after the heat preservation and pressure maintaining are finished.
And step three, taking out the sample after furnace cooling, and processing the sample to the required shape and size.
Example 9
Step one, raw materials are proportioned according to the following mode:
u-10Mo alloy powder, 5-100 μm,235the U enrichment degree is 1-5%, 99 vol%, the planar length of graphene is 100nm-200 mu m, and 1 vol%, the powder is placed in a nylon ball milling tank, zirconium oxide grinding balls with the mass being 3 times that of the powder are added, and the mixture is mixed for 24 hours.
Step two, sintering is carried out according to the following mode:
placing the powder in a designed graphite or metal die, and carrying out flash sintering, wherein the sintering process is as follows: vacuum-pumping to 5 × 10-2～5×10-1Pa, and then filling argon to 10-60 kPa; heating to 1100 deg.C at 1000 deg.C/min, sintering under 40MPa, maintaining the temperature for 0.5min, and cooling.
And step three, taking out the sample after furnace cooling, and processing the sample to the required shape and size.
The above-mentioned embodiment is only one of the preferred embodiments of the present invention, and should not be used to limit the scope of the present invention, but all the insubstantial modifications or changes made within the spirit and scope of the main design of the present invention, which still solve the technical problems consistent with the present invention, should be included in the scope of the present invention.

Claims (5)

1. A method for preparing a metal type fuel pellet with high irradiation stability is characterized by comprising the following steps,
the method comprises the following steps: mixing uranium-based alloy powder and a carbon-based nano material according to a volume ratio of 99.9-99:1-0.1, placing the mixture in a nylon ball milling tank, adding 3 times of zirconia grinding balls by mass, and mixing for 24 hours to obtain mixed powder; wherein the uranium-based alloy is U-Mo, U-Zr or U3Si2The grain diameter is 5-100 μm,235the U enrichment degree is 1-5%, and the carbon-based nano material is any one or more of the following materials: SiC particles with the particle size of 20nm-2 mu m, SiC whiskers with the diameter of 20nm-200nm and the length of 5-20 mu m, carbon nanotubes with the diameter of 5nm-100nm and the length of 1-20 mu m, and graphene with the plane length of 100nm-200 mu m;
step two: and carrying out pressureless sintering, hot-pressing sintering, spark plasma sintering or flash firing on the mixed powder, cooling along with the furnace after the heat preservation and pressure preservation are finished, taking out, and carrying out machining forming to obtain the metal type fuel pellet.
2. The method for preparing metal type fuel pellets with high radiation stability according to claim 1, wherein in the second step, when the sintering mode is pressureless sintering, the steps are as follows: the mixed powder is molded under the condition of 100-400MPa to obtain a fuel pellet biscuit, and then the fuel pellet biscuit is placed in an atmosphere sintering furnace, the temperature is raised to 800-1200 ℃ at the speed of 1-10 ℃/min, and the temperature is preserved for 1-5 h; the atmosphere is vacuum or argon atmosphere protection.
3. High irradiance according to claim 1The preparation method of the stable metal type fuel pellet is characterized in that in the second step, when the sintering mode is hot-pressing sintering, the steps are as follows: placing the mixed powder in a graphite mold, and vacuumizing to 5 × 10-2-5×10-1Pa, heating to 800-1200 ℃ at the speed of 1-20 ℃/min under the condition of sintering pressure of 20-100MPa, and preserving heat for 1-4 h; the sintering atmosphere is argon atmosphere.
4. The method for preparing metal type fuel pellets with high radiation stability according to claim 1, wherein in the second step, when the sintering mode is spark plasma sintering, the steps are as follows: placing the mixed powder in a graphite mold, and vacuumizing to 5 × 10-2-5×10-1Pa, then filling argon to 10-60 kPa; heating to 700-1200 ℃ at the speed of 50-1000 ℃/min under the sintering pressure condition of 20-100MPa, and preserving the heat for 1-30 min.
5. The method for preparing metal type fuel pellet with high radiation stability of claim 1, wherein in the second step, when the sintering mode is flash firing, the steps are as follows: placing the mixed powder in graphite or metal mold, and vacuumizing to 5 × 10-2-5×10-1Pa, then filling argon to 10-60 kPa; heating to 700-1200 ℃ at the speed of 400-2000 ℃/min, and keeping the temperature for 10s-5 min.
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CN112442174A (en) * 2019-08-29 2021-03-05 北京化工大学 Radiation-resistant phenyl silicone rubber and preparation method and application thereof
CN112863718A (en) * 2020-12-31 2021-05-28 中核北方核燃料元件有限公司 Preparation method of UMoZr dispersed fuel
CN113628767A (en) * 2021-09-03 2021-11-09 中国工程物理研究院材料研究所 UO with high irradiation stability2Ceramic fuel and preparation method and application thereof

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