CN108249925B - Preparation method of all-ceramic micro-packaging fuel pellet - Google Patents
Preparation method of all-ceramic micro-packaging fuel pellet Download PDFInfo
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- CN108249925B CN108249925B CN201711384305.7A CN201711384305A CN108249925B CN 108249925 B CN108249925 B CN 108249925B CN 201711384305 A CN201711384305 A CN 201711384305A CN 108249925 B CN108249925 B CN 108249925B
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- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/515—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics
- C04B35/56—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides
- C04B35/565—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides based on silicon carbide
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- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/626—Preparing or treating the powders individually or as batches ; preparing or treating macroscopic reinforcing agents for ceramic products, e.g. fibres; mechanical aspects section B
- C04B35/628—Coating the powders or the macroscopic reinforcing agents
- C04B35/62892—Coating the powders or the macroscopic reinforcing agents with a coating layer consisting of particles
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- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/64—Burning or sintering processes
- C04B35/645—Pressure sintering
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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
- G21C3/62—Ceramic fuel
- G21C3/64—Ceramic dispersion fuel, e.g. cermet
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3217—Aluminum oxide or oxide forming salts thereof, e.g. bauxite, alpha-alumina
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3224—Rare earth oxide or oxide forming salts thereof, e.g. scandium oxide
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3224—Rare earth oxide or oxide forming salts thereof, e.g. scandium oxide
- C04B2235/3225—Yttrium oxide or oxide-forming salts thereof
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
- C04B2235/74—Physical characteristics
- C04B2235/77—Density
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- 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 fuel pellet preparation, and particularly relates to a preparation method of an all-ceramic micro-packaging fuel pellet, which comprises the following steps: step 1, adding silicon carbide powder and a sintering aid; step 2, coating silicon carbide powder on the surface of the TRISO particles; step 3, performing fuel pellet; and 4, hot-pressing and sintering the fuel pellets. The all-ceramic micro-packaging fuel pellet prepared by the invention is cylindrical, and the density of the pellet is more than or equal to 3.1g/cm3And the structure of the TRISO particles in the core block is kept complete and is uniformly distributed in the silicon carbide matrix.
Description
Technical Field
The invention belongs to the technical field of fuel pellet preparation, and particularly relates to a preparation method of an all-ceramic micro-packaging fuel pellet.
Background
At present, the commercial nuclear fuel adopts a uranium dioxide ceramic pellet, and the main preparation method is to prepare the ceramic pellet from uranium dioxide with a certain enrichment degree by powder metallurgy methods such as pressing, sintering, shape grinding and the like. Although the nuclear fuel can be developed for more mature application in many years, certain defects still exist under specific use conditions, mainly manifested by low thermal conductivity of a matrix, poor fault tolerance in case of accidents, and poor safety guarantee of the nuclear fuel.
As an important measure for improving the safety performance of a nuclear power station, research and development of an fault Tolerant Fuel (ATF) is becoming a new direction of international development in the nuclear Fuel field, i.e., a Fuel capable of accommodating accidents and having inherent safety to a certain extent.
The all-ceramic micro-packaging fuel pellet is designed for high fuel consumption U used in a light water reactor, uranium dioxide fuel particles are packaged in a silicon carbide matrix, and the silicon carbide matrix is high in stability, high in thermal conductivity and good in compatibility with a coolant. The fuel coated by the full ceramic matrix releases few fission gases and corrosive fission products, so that the fault tolerance is high when an accident occurs, and the safety is ensured.
Disclosure of Invention
The invention aims to solve the technical problem that TRISO (TRISO) Coated Fuel Particles and silicon carbide powder are used as raw materials, and the TRISO Particles are uniformly dispersed and distributed in a silicon carbide substrate through a powder metallurgy process to prepare the all-ceramic micro-encapsulated Fuel pellet.
In order to realize the purpose, the invention adopts the technical scheme that:
a preparation method of an all-ceramic micro-packaging fuel pellet comprises the following steps:
step 1, adding silicon carbide powder and sintering aid
Step 1.1, determining the raw materials
The average grain diameter of the silicon carbide powder is less than or equal to 1 mu m, and the specific surface area is more than or equal to 20m2/g；
The sintering aid is a mixture of aluminum oxide and rare earth element oxide, and the average grain diameter is 0.9-1.1 mu m;
step 1.2, adding combustion aid
Adding a sintering aid into the silicon carbide powder, wherein the addition amount of the sintering aid is 6-10% of the mass of the silicon carbide powder;
mixing a sintering aid and silicon carbide powder by adopting a wet ball milling process, wherein a dispersing agent is an organic solvent;
drying and screening the mixture after wet ball milling to obtain a silicon carbide powder matrix raw material;
step 2, coating silicon carbide powder on the surface of TRISO particles
Step 2.1, uniformly coating a bonding system on the surface of the TRISO particles and soaking for a set time, wherein the bonding system is a viscous organic solvent;
2.2, bonding a layer of the silicon carbide powder matrix raw material obtained in the step 1 on the surface of the particles by adopting a surface bonding technology;
step 2.3, uniformly mixing the TRISO particles with the silicon carbide powder;
step 3, preforming of fuel pellets
The fuel pellet preforming adopts compression molding, the green compact pellet is cylindrical, zinc stearate mixed carbon tetrachloride is used as a forming lubricant, the pellet forming pressure is 10-50 MPa, and the pressure maintaining time is 5-20 s;
step 4, hot-pressing and sintering the fuel pellets
The sintering of the fuel pellet belongs to liquid phase sintering, the sintering mode is hot pressing sintering, high-density graphite is used as a hot pressing die, the hot pressing temperature is controlled to be 1850-2000 ℃, the heat preservation time is controlled to be 30-100 min, and the hot pressing pressure is 15-50 MPa.
Further, a method of preparing an all ceramic micro encapsulated fuel pellet as described above, step 1.1, the sintering aid is alumina and Y2O3Mixture of (2), alumina and Y2O3The mass ratio of (A) to (B) is 2: 8. 4: 6. 3: 7.
Further, a method for preparing the all-ceramic micro-encapsulated fuel pellet as described above, step 1.1, the sintering aid is alumina and Gd2O3Mixture of (a), alumina and Gd2O3The mass ratio of (A) to (B) is 2: 8. 4: 6. 3: 7.
Further, in the above method for preparing the all-ceramic micro-encapsulated fuel pellet, in step 1.2, the dispersant is one of absolute ethyl alcohol and carbon tetrachloride.
Further, in the preparation method of the all-ceramic micro-packaging fuel pellet, in step 2.1, a bonding system is glycerol ethanol solution with the mass concentration of 5-30%, glycerol is used as a bonding agent, and absolute ethyl alcohol is used as a diluent.
Further, in the preparation method of the all-ceramic micro-packaging fuel pellet, in step 2.2, the mass of the TRISO particles is 20-50 wt% of the mass of the silicon carbide powder matrix raw material.
Further, in the above method for preparing the all-ceramic micro-encapsulated fuel pellet, in step 4, the sintering atmosphere is one of vacuum and argon atmosphere.
The technical scheme of the invention has the beneficial effects that: prepared by the inventionThe full ceramic micro-packaging fuel pellet is in a cylindrical shape, and the density of the pellet is more than or equal to 3.1g/cm3And the structure of the TRISO particles in the core block is kept complete and is uniformly distributed in the silicon carbide matrix.
Detailed Description
The technical solution of the present invention will be described in detail with reference to the following specific examples.
The invention relates to a preparation method of a full-ceramic micro-packaging fuel pellet, which comprises the following steps:
step 1, adding silicon carbide powder and sintering aid
Step 1.1, determining the raw materials
The average grain diameter of the silicon carbide powder is less than or equal to 1 mu m, and the specific surface area is more than or equal to 20m2/g；
The sintering aid is a mixture of aluminum oxide and rare earth element oxide, and the average grain diameter is 0.9-1.1 mu m;
specifically, the scheme of the sintering aid comprises the following two schemes: (ii) alumina and Y2O3Mixture of (2), alumina and Y2O3The mass ratio of (A) to (B) is 2: 8. 4: 6. 3: 7; ② the sintering aid is alumina and Gd2O3Mixture of (a), alumina and Gd2O3The mass ratio of (A) to (B) is 2: 8. 4: 6. 3: 7;
step 1.2, adding combustion aid
Adding a sintering aid into the silicon carbide powder, wherein the addition amount of the sintering aid is 6-10% of the mass of the silicon carbide powder;
mixing a sintering aid and silicon carbide powder by adopting a wet ball milling process, wherein a dispersing agent is an organic solvent such as absolute ethyl alcohol, carbon tetrachloride and the like;
drying and screening the mixture after wet ball milling to obtain a silicon carbide powder matrix raw material;
step 2, coating silicon carbide powder on the surface of TRISO particles
Step 2.1, uniformly coating a bonding system on the surface of the TRISO particles and soaking for a set time, wherein the bonding system is a viscous organic solvent; specifically, the bonding system is a glycerol ethanol solution with the mass concentration of 5-30%, glycerol is used as a bonding agent, and absolute ethyl alcohol is used as a diluent;
2.2, bonding a layer of the silicon carbide powder matrix raw material obtained in the step 1 on the surface of the particles by adopting a surface bonding technology; the mass of the TRISO particles is 20-50 wt% of the mass of the silicon carbide powder matrix raw material;
step 2.3, uniformly mixing the TRISO particles with the silicon carbide powder;
step 3, preforming of fuel pellets
The fuel pellet preforming adopts compression molding, the green compact pellet is cylindrical, zinc stearate mixed carbon tetrachloride is used as a forming lubricant, the pellet forming pressure is 10-50 MPa, and the pressure maintaining time is 5-20 s;
step 4, hot-pressing and sintering the fuel pellets
The fuel pellet sintering belongs to liquid phase sintering, the sintering mode is hot-pressing sintering, high-density graphite is used as a hot-pressing die, the sintering atmosphere is vacuum or argon atmosphere, the hot-pressing temperature is controlled to be 1850-2000 ℃, the heat preservation time is controlled to be 30-100 min, and the hot-pressing pressure is 15-50 MPa.
Claims (1)
1. The preparation method of the all-ceramic micro-packaging fuel pellet is characterized by comprising the following steps of:
step 1, adding silicon carbide powder and sintering aid
Step 1.1, determining the raw materials
The average grain diameter of the silicon carbide powder is less than or equal to 1 mu m, and the specific surface area is more than or equal to 20m2/g；
The sintering aid is a mixture of aluminum oxide and rare earth element oxide, and the average grain diameter is 0.9-1.1 mu m;
step 1.2, adding combustion aid
Adding a sintering aid into the silicon carbide powder, wherein the addition amount of the sintering aid is 6-10% of the mass of the silicon carbide powder;
mixing a sintering aid and silicon carbide powder by adopting a wet ball milling process, wherein a dispersing agent is an organic solvent;
drying and screening the mixture after wet ball milling to obtain a silicon carbide powder matrix raw material;
step 2, coating silicon carbide powder on the surface of TRISO particles
Step 2.1, uniformly coating a bonding system on the surface of the TRISO particles and soaking for a set time, wherein the bonding system is a viscous organic solvent;
2.2, bonding a layer of the silicon carbide powder matrix raw material obtained in the step 1 on the surface of the particles by adopting a surface bonding technology;
step 2.3, uniformly mixing the TRISO particles with the silicon carbide powder;
step 3, preforming of fuel pellets
The fuel pellet preforming adopts compression molding, the green compact pellet is cylindrical, zinc stearate mixed carbon tetrachloride is used as a forming lubricant, the pellet forming pressure is 10-50 MPa, and the pressure maintaining time is 5-20 s;
step 4, hot-pressing and sintering the fuel pellets
The sintering of the fuel pellet belongs to liquid phase sintering, the sintering mode is hot pressing sintering, high-density graphite is used as a hot pressing die, the hot pressing temperature is controlled to be 1850-2000 ℃, the heat preservation time is controlled to be 30-100 min, and the hot pressing pressure is 15-50 MPa;
in step 1.1, the scheme of the sintering aid comprises the following two schemes: (ii) alumina and Y2O3Mixture of (2), alumina and Y2O3The mass ratio of (A) to (B) is 2: 8. 4: 6. 3: 7; ② the sintering aid is alumina and Gd2O3Mixture of (a), alumina and Gd2O3The mass ratio of (A) to (B) is 2: 8. 4: 6. 3: 7;
in the step 1.2, the dispersant is one of absolute ethyl alcohol and carbon tetrachloride;
in the step 2.1, a bonding system is a glycerol ethanol solution with the mass concentration of 5-30%, glycerol is used as a bonding agent, and absolute ethyl alcohol is used as a diluent;
in step 2.2, the mass of the TRISO particles is 20-50 wt% of the mass of the silicon carbide powder matrix raw material;
in the step 4, the sintering atmosphere is one of vacuum and argon atmosphere.
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Families Citing this family (6)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN112739664B (en) * | 2018-09-28 | 2023-07-21 | 福吉米株式会社 | Coated silicon carbide particle powder |
| CN110729064B (en) * | 2019-10-24 | 2021-04-13 | 中国核动力研究设计院 | Al for nuclear power2O3-Gd2O3Burnable poison ceramic material and preparation method thereof |
| WO2022241733A1 (en) * | 2021-05-20 | 2022-11-24 | 中广核研究院有限公司 | High-entropy ceramic inert matrix dispersion fuel pellet and preparation method therefor |
| CN113611435B (en) * | 2021-08-17 | 2023-06-02 | 西北工业大学 | Ceramic composite fuel pellet and preparation method and application thereof |
| CN115295198B (en) * | 2022-08-04 | 2024-03-19 | 中国核动力研究设计院 | Method for preparing full ceramic micro-package dispersion fuel by oscillation sintering |
| CN116926399B (en) * | 2023-07-05 | 2024-04-09 | 湖南昕昱科技有限公司 | Special ceramic material and preparation method and application thereof |
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| WO2017019620A1 (en) * | 2015-07-25 | 2017-02-02 | Ultra Safe Nuclear Corporation | Method for fabrication of fully ceramic microencapsulated nuclear fuel |
| CN106935297A (en) * | 2015-12-30 | 2017-07-07 | 中核北方核燃料元件有限公司 | A kind of preparation method of thorium anhydride paillon foil |
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