CN112820431A - Metal wall microcapsule nuclear fuel pellet added with oxide and preparation method thereof - Google Patents
Metal wall microcapsule nuclear fuel pellet added with oxide and preparation method thereof Download PDFInfo
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- CN112820431A CN112820431A CN202011620314.3A CN202011620314A CN112820431A CN 112820431 A CN112820431 A CN 112820431A CN 202011620314 A CN202011620314 A CN 202011620314A CN 112820431 A CN112820431 A CN 112820431A
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- 229910052751 metal Inorganic materials 0.000 title claims abstract description 74
- 239000002184 metal Substances 0.000 title claims abstract description 74
- 239000008188 pellet Substances 0.000 title claims abstract description 39
- 239000003094 microcapsule Substances 0.000 title claims abstract description 37
- 239000003758 nuclear fuel Substances 0.000 title claims abstract description 37
- 238000002360 preparation method Methods 0.000 title claims abstract description 20
- 239000002245 particle Substances 0.000 claims abstract description 64
- 239000011148 porous material Substances 0.000 claims abstract description 8
- 238000005245 sintering Methods 0.000 claims description 41
- 239000000843 powder Substances 0.000 claims description 28
- 238000002156 mixing Methods 0.000 claims description 19
- 238000000034 method Methods 0.000 claims description 16
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 14
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 12
- 238000000465 moulding Methods 0.000 claims description 11
- 229910052721 tungsten Inorganic materials 0.000 claims description 11
- 239000000463 material Substances 0.000 claims description 10
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 claims description 10
- 239000010937 tungsten Substances 0.000 claims description 10
- 229910045601 alloy Inorganic materials 0.000 claims description 8
- 239000000956 alloy Substances 0.000 claims description 8
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 8
- 239000011651 chromium Substances 0.000 claims description 8
- 229910052681 coesite Inorganic materials 0.000 claims description 8
- 229910052593 corundum Inorganic materials 0.000 claims description 8
- 229910052906 cristobalite Inorganic materials 0.000 claims description 8
- 230000009467 reduction Effects 0.000 claims description 8
- 239000000377 silicon dioxide Substances 0.000 claims description 8
- 229910052682 stishovite Inorganic materials 0.000 claims description 8
- 229910052905 tridymite Inorganic materials 0.000 claims description 8
- 229910001845 yogo sapphire Inorganic materials 0.000 claims description 8
- 239000011812 mixed powder Substances 0.000 claims description 7
- 239000000203 mixture Substances 0.000 claims description 7
- 239000000126 substance Substances 0.000 claims description 6
- 229910052804 chromium Inorganic materials 0.000 claims description 5
- 238000010907 mechanical stirring Methods 0.000 claims description 5
- 229910052750 molybdenum Inorganic materials 0.000 claims description 5
- 230000001590 oxidative effect Effects 0.000 claims description 5
- 230000008569 process Effects 0.000 claims description 5
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 claims description 4
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims description 4
- 238000000498 ball milling Methods 0.000 claims description 4
- 150000001875 compounds Chemical class 0.000 claims description 4
- 238000000748 compression moulding Methods 0.000 claims description 4
- 238000000462 isostatic pressing Methods 0.000 claims description 4
- 239000011733 molybdenum Substances 0.000 claims description 4
- 230000003647 oxidation Effects 0.000 claims description 4
- 238000007254 oxidation reaction Methods 0.000 claims description 4
- 238000001132 ultrasonic dispersion Methods 0.000 claims description 4
- 239000008187 granular material Substances 0.000 claims description 2
- 230000004992 fission Effects 0.000 abstract description 15
- 239000000919 ceramic Substances 0.000 abstract description 7
- 230000014759 maintenance of location Effects 0.000 abstract description 5
- 238000004519 manufacturing process Methods 0.000 abstract description 3
- 230000002285 radioactive effect Effects 0.000 description 8
- 239000000446 fuel Substances 0.000 description 4
- 230000006872 improvement Effects 0.000 description 3
- 230000004888 barrier function Effects 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- 230000005012 migration Effects 0.000 description 2
- 238000013508 migration Methods 0.000 description 2
- 239000003870 refractory metal Substances 0.000 description 2
- 238000003980 solgel method Methods 0.000 description 2
- 229910018516 Al—O Inorganic materials 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 230000000274 adsorptive effect Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000001413 cellular effect Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 238000012216 screening Methods 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- 238000003805 vibration mixing Methods 0.000 description 1
- 230000003313 weakening effect Effects 0.000 description 1
- 238000009736 wetting Methods 0.000 description 1
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Classifications
-
- 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
-
- 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
Abstract
The invention belongs to the technical field of nuclear fuel pellet design and manufacture, and particularly relates to a metal wall microcapsule nuclear fuel pellet added with oxides and a preparation method thereof. Including UO2Particles, metal walls and inert oxide inclusions, wherein the metal walls form a honeycomb-shaped continuous network structure, and each honeycomb-shaped pore has UO2Particles, metal walls encasing UO2Particulate, inert oxide inclusions are present within the metal wall. The invention combines the advantages of the metal microcapsule core block and the ceramic microcapsule core block, and compared with the traditional UO2Nuclear fuel pellets, while achieving improved thermal conductivity and retention of fission products.
Description
Technical Field
The invention belongs to the technical field of nuclear fuel pellet design and manufacture, and particularly relates to a metal wall microcapsule nuclear fuel pellet added with oxides and a preparation method thereof.
Background
Future nuclear power plants and nuclear power plants have a strong demand for accident-resistant fuels. The accident-resistant fuel can enhance retention of radioactive fission products compared to conventional nuclear fuels. The fuel pellets are both a source of radioactive fission products and a first barrier to the release of radioactive fission products to the environment. Therefore, the novel fuel pellet which has excellent physical and chemical properties and nuclear properties and can retain radioactive fission products has wide application prospect.
A concept of microcapsule core block is proposed abroad, migration of radioactive fission products such as Cs and I is limited by a method of increasing multiple chemical traps or weakening diffusivity, and retention capacity of the radioactive fission products and corrosive fission products with strong radioactivity is enhanced. The structure is that all UO is coated with thin-walled metal or oxide2The particles are packaged, and the thin wall can play a role in chemical trap and physical barrier to the migration of fission products and can play a role in improving the thermal conductivity.
According to the difference of thin-wall materials, the microcapsule core block developed abroad is divided into two types of metal microcapsule core block and ceramic microcapsule core block, the metal microcapsule core block uses W, Mo, Cr or their alloy as thin wall, and the ceramic microcapsule core block uses SiO2、TiO2、Al2O3Or an oxide of Si-Ti-Al-O series as a thin wall.
Disclosure of Invention
The metal microcapsule core block and the ceramic microcapsule core block respectively have the following defects: the metal microcapsule core has weak absorption capacity to fission products Cs and I, and the ceramic microcapsule core has limited improvement of thermal conductivity. In order to exert the advantages of the metal wall microcapsule nuclear fuel pellet and overcome the defects of the metal wall microcapsule nuclear fuel pellet and the metal wall microcapsule nuclear fuel pellet, the metal wall microcapsule nuclear fuel pellet added with the oxide and the preparation method thereof are designed.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
an oxide-added metal-walled microencapsulated nuclear fuel pellet comprising UO2Particles, metal walls, inert oxide inclusions, the metal walls forming a cellular continuous network structure, each cellularAll pores have UO2Particles, metal walls encasing UO2Particulate, inert oxide inclusions are present within the metal wall.
UO2The particle size of the particles is 1-1000 μm.
The particle size of the inert oxide inclusion is less than 1 μm.
The metal wall is tungsten, molybdenum, chromium, and alloys thereof.
The inert oxide inclusion being SiO2、TiO2、Al2O3Or compounds or mixtures consisting of Si, Ti, Al, O.
A method for preparing a metal wall microcapsule nuclear fuel pellet added with oxide,
(1)UO2preparing particles;
(2) mixing materials: mixing UO2Uniformly mixing the particles, the inert oxide powder and the metal powder to wrap the UO with the inert oxide powder and the metal powder2Particles;
(3) molding: forming the mixed powder into a green body;
(4) primary sintering: subjecting the shaped green body to a treatment of pure H2Or H2/N2Mixed gas or H2Mixed gas of/Ar or H2Sintering at a temperature lower than 1200 ℃ in the atmosphere of the mixed gas of the/He;
(5) when the metal wall adopts a tungsten simple substance or a tungsten-containing alloy, carrying out oxidation sintering: in an oxidizing atmosphere O2Or CO2Sintering at a temperature of less than 1800 ℃ for 0.5-10 hours;
(6) reduction and sintering: in pure H2Or H2/N2Mixed gas or H2Mixed gas of/Ar or H2Sintering at a temperature lower than 1800 ℃ in an atmosphere of a mixed gas/He.
UO2Preparing particles: preparation of UO by sol-gel or plasma spheroidizing method2Particles are screened and vibrated to obtain UO with the particle size of 1-1000 mu m2And (3) granules.
Mixing materials: adopting mechanical stirring, vibration, ultrasonic dispersion or ball milling powder mixing process to mix UO2Granular, inert oxide powderThe powder and the metal powder are mixed uniformly.
Molding: and forming the mixed powder into a green body by compression molding or isostatic pressing.
Primary sintering: sintering at a temperature of less than 1200 ℃ for 0.5-20 hours; reduction and sintering: sintering at a temperature of less than 1800 ℃ for 0.5-10 hours.
The beneficial effects obtained by the invention are as follows:
the invention combines the advantages of the metal microcapsule core block and the ceramic microcapsule core block, and compared with the traditional UO2Nuclear fuel pellets, while achieving improved thermal conductivity and retention of fission products.
An oxide-added metal-wall microcapsule nuclear fuel pellet comprises UO2Particles, metal walls, inert oxide inclusions, wherein the metal walls form a honeycomb-like continuous network structure with UO in each honeycomb-like pore2Particles, metal walls encasing UO2Particulate, inert oxide inclusions exist within the metal wall in the form of small size inclusions.
The metal wall is made of refractory metals such as tungsten, molybdenum, chromium and the like and alloys thereof, has the advantages of high melting point and good heat conductivity, enhances the heat conductivity of the core block, and improves the safety of the core block.
The inert oxide inclusion being SiO2、TiO2、Al2O3Or compounds or mixtures composed of Si, Ti, Al, O, have a strong adsorptive effect on the radioactive fission products Cs, I, etc., thereby reducing the release of the radioactive fission products.
A process for preparing the oxide-added nuclear fuel pellet with metal wall and microcapsules includes UO2The method comprises the steps of particle preparation, material mixing, molding, primary sintering, oxidation sintering, reduction sintering and the like, and has the following effects: metal capable of wetting UO2The particles form a honeycomb-shaped continuous network structure, inert oxide inclusions can be added, and the metal-wall micro-capsule nuclear fuel pellet added with the oxide, which can simultaneously realize the improvement of the thermal conductivity and the fission product retention capacity, can be prepared.
Drawings
FIG. 1 is a schematic of the microstructure of an oxide-doped metal-walled microencapsulated nuclear fuel pellet;
FIG. 2 is a flow chart of a method for preparing metal-wall microcapsule nuclear fuel pellets with added oxides;
in the figure: 1-UO2Particles, 2-metal walls, 3-inert oxide inclusions.
Detailed Description
The invention is described in detail below with reference to the figures and specific embodiments.
The structure of a metal wall microcapsule nuclear fuel pellet added with oxide comprises three parts-UO2Particles, metal walls, inert oxide inclusions, wherein the metal walls form a honeycomb-like continuous network structure with UO in each honeycomb-like pore2Particles, metal walls encasing UO2Particles, UO2The particle size of the particles is within the range of 1-1000 mu m, and the inert oxide inclusion exists in the metal wall in the form of small-size inclusion with the particle size of less than 1 mu m; the metal wall is made of refractory metals such as tungsten, molybdenum, chromium and the like and alloys thereof; the inert oxide inclusion being SiO2、TiO2、Al2O3Or compounds or mixtures consisting of Si, Ti, Al, O.
The preparation method of the metal wall microcapsule nuclear fuel pellet added with the oxide comprises the following steps:
(1)UO2preparing particles: preparing UO by sol-gel or plasma spheroidizing method2Particles are screened and vibrated to obtain UO with the particle size of 1-1000 mu m2Particles;
(2) mixing materials: adopting powder mixing process of mechanical stirring, vibration, ultrasonic dispersion or ball milling, etc. to mix UO2Uniformly mixing the particles, the inert oxide powder and the metal powder to wrap the UO with the inert oxide powder and the metal powder2Particles;
(3) molding: molding the mixed powder into a green body by compression molding or isostatic pressing;
(4) primary sintering: subjecting the shaped green body to a treatment of pure H2Or H2/N2Mixed gas or H2Mixed gas of/Ar or H2Sintering for 0.5-20 hours at the temperature lower than 1200 ℃ in the atmosphere of the/He mixed gas;
(5) when the metal wall adopts a tungsten simple substance or a tungsten-containing alloy, carrying out oxidation sintering: in an oxidizing atmosphere O2Or CO2Sintering at a temperature of less than 1800 ℃ for 0.5-10 hours;
(6) reduction and sintering: in pure H2Or H2/N2Mixed gas or H2Mixed gas of/Ar or H2Sintering for 0.5-10 hours at the temperature lower than 1800 ℃ in the atmosphere of the/He mixed gas.
Example 1:
a metal-wall microcapsule nuclear fuel pellet added with oxide has a phase composition including UO2Particles, metal walls, inert oxide inclusions, wherein the metal walls form a continuous network structure and each honeycomb has UO in its pores2Particles, metal walls encasing UO2Particles, inert oxide inclusions present within the metal wall;
in this example, the metal wall is W and the inert oxide inclusion is SiO2。
The preparation method of the metal wall microcapsule nuclear fuel pellet added with the oxide comprises the following steps:
(1)UO2preparing particles: preparation of UO by sol-gel method2Particles are obtained by screening and vibration separation to obtain UO with the particle size of 300-400 mu m2Particles;
(2) mixing materials: adopting mechanical stirring and vibration mixing process to mix UO2Particles, SiO2Mixing the powder and W powder uniformly to obtain SiO2Powder and W powder are uniformly coated with UO2Particles;
(3) molding: molding the mixed powder into a green body by adopting a compression molding mode;
(4) primary sintering: subjecting the shaped green body to a treatment of pure H2Sintering at 900 ℃ for 8 hours in the atmosphere of (2);
(5) oxidizing and sintering: in CO2Sintering at 1400 deg.C for 4 hr;
(6) reduction and sintering: in pure H2Is sintered at a temperature of 1550 c for 2 hours.
Example 2:
a metal-wall microcapsule nuclear fuel pellet added with oxide has a phase composition including UO2Particles, metal walls, inert oxide inclusions, wherein the metal walls form a continuous network structure and each honeycomb has UO in its pores2Particles, metal walls encasing UO2Particles, inert oxide inclusions present within the metal wall;
in this example, the metal wall is Cr and the inert oxide inclusion is TiO2And Al2O3The mixture of (1: 1 by mass).
The preparation method of the metal wall microcapsule nuclear fuel pellet added with the oxide comprises the following steps:
(1)UO2preparing particles: preparation of UO by sol-gel method2Particles are screened and vibrated to obtain UO with the particle size of 200-300 mu m2Particles;
(2) mixing materials: adopting the processes of mechanical stirring, ultrasonic dispersion and ball milling to mix UO2Particles, TiO2And Al2O3Mixing the powder with Cr powder to obtain TiO powder2And Al2O3Powder and Cr powder are evenly coated on UO2Particles;
(3) molding: forming the mixed powder into a green body by adopting an isostatic pressing forming mode;
(4) primary sintering: subjecting the shaped green body to H2Sintering for 10 hours at the temperature of 800 ℃ in the atmosphere of/Ar mixed gas;
(5) reduction and sintering: at H2Sintering at 1750 ℃ for 4 hours in an atmosphere of/Ar mixed gas.
An oxide-added metal-wall microcapsule nuclear fuel pellet and a preparation method thereof are characterized in that the microstructure of the pellet comprises UO2Particles, metal walls, inert oxide inclusions, wherein the metal walls form a honeycomb-like continuous network structure with UO in each honeycomb-like pore2Particles, metal walls encasing UO2Particle, inert oxide inclusion storageWithin the metal wall. The preparation method comprises the steps of UO2Preparing particles, mixing materials, molding, primarily sintering, oxidizing sintering, reducing sintering and the like. The invention combines the advantages of the metal microcapsule core block and the ceramic microcapsule core block, and simultaneously realizes the improvement of the thermal conductivity and the capability of retaining fission products.
Claims (10)
1. An oxide-added metal-walled microencapsulated nuclear fuel pellet characterized by: including UO2Particles, metal walls and inert oxide inclusions, wherein the metal walls form a honeycomb-shaped continuous network structure, and each honeycomb-shaped pore has UO2Particles, metal walls encasing UO2Particulate, inert oxide inclusions are present within the metal wall.
2. An oxide-added metal-walled microencapsulated nuclear fuel pellet as claimed in claim 1 wherein: UO2The particle size of the particles is 1-1000 μm.
3. An oxide-added metal-walled microencapsulated nuclear fuel pellet as claimed in claim 1 wherein: the particle size of the inert oxide inclusion is less than 1 μm.
4. An oxide-added metal-walled microencapsulated nuclear fuel pellet as claimed in claim 1 wherein: the metal wall is tungsten, molybdenum, chromium, and alloys thereof.
5. An oxide-added metal-walled microencapsulated nuclear fuel pellet as claimed in claim 1 wherein: the inert oxide inclusion being SiO2、TiO2、Al2O3Or compounds or mixtures consisting of Si, Ti, Al, O.
6. A preparation method of a metal wall microcapsule nuclear fuel pellet added with oxide is characterized in that:
(1)UO2preparing particles;
(2) mixing materials: mixing UO2Granular, inert oxidationUniformly mixing the powder and the metal powder to coat UO with the inert oxide powder and the metal powder2Particles;
(3) molding: forming the mixed powder into a green body;
(4) primary sintering: subjecting the shaped green body to a treatment of pure H2Or H2/N2Mixed gas or H2Mixed gas of/Ar or H2Sintering at a temperature lower than 1200 ℃ in the atmosphere of the mixed gas of the/He;
(5) when the metal wall adopts a tungsten simple substance or a tungsten-containing alloy, carrying out oxidation sintering: in an oxidizing atmosphere O2Or CO2Sintering at a temperature of less than 1800 ℃ for 0.5-10 hours;
(6) reduction and sintering: in pure H2Or H2/N2Mixed gas or H2Mixed gas of/Ar or H2Sintering at a temperature lower than 1800 ℃ in an atmosphere of a mixed gas/He.
7. A method for the preparation of metal-walled microencapsulated nuclear fuel pellets with added oxides according to claim 6, characterized in that: UO2Preparing particles: preparation of UO by sol-gel or plasma spheroidizing method2Particles are screened and vibrated to obtain UO with the particle size of 1-1000 mu m2And (3) granules.
8. A method for the preparation of metal-walled microencapsulated nuclear fuel pellets with added oxides according to claim 6, characterized in that: mixing materials: adopting mechanical stirring, vibration, ultrasonic dispersion or ball milling powder mixing process to mix UO2The particles, inert oxide powder and metal powder are mixed homogeneously.
9. A method for the preparation of metal-walled microencapsulated nuclear fuel pellets with added oxides according to claim 6, characterized in that: molding: and forming the mixed powder into a green body by compression molding or isostatic pressing.
10. A method for the preparation of metal-walled microencapsulated nuclear fuel pellets with added oxides according to claim 6, characterized in that: primary sintering: sintering at a temperature of less than 1200 ℃ for 0.5-20 hours; reduction and sintering: sintering at a temperature of less than 1800 ℃ for 0.5-10 hours.
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CN109671511A (en) * | 2018-12-19 | 2019-04-23 | 中国工程物理研究院材料研究所 | A kind of preparation method of monocrystalline high thermal conductivity uranium dioxide fuel ball |
CN109741839A (en) * | 2018-12-24 | 2019-05-10 | 哈尔滨工程大学 | A kind of heat insulating metal and ceramic multilayer hollow sphere and preparation method thereof |
CN110156475A (en) * | 2019-07-02 | 2019-08-23 | 中国原子能科学研究院 | A kind of microwave synthesis method of uranium carbonitride zirconium powder |
CN112102968A (en) * | 2020-08-07 | 2020-12-18 | 中国科学院上海应用物理研究所 | High-thermal-conductivity fuel core block and preparation method thereof |
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