CN116682582A - Hollow radioactive contained fuel containing burnable poison, preparation method and application - Google Patents
Hollow radioactive contained fuel containing burnable poison, preparation method and application Download PDFInfo
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- CN116682582A CN116682582A CN202310811318.7A CN202310811318A CN116682582A CN 116682582 A CN116682582 A CN 116682582A CN 202310811318 A CN202310811318 A CN 202310811318A CN 116682582 A CN116682582 A CN 116682582A
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- 239000000446 fuel Substances 0.000 title claims abstract description 183
- 239000002574 poison Substances 0.000 title claims abstract description 109
- 231100000614 poison Toxicity 0.000 title claims abstract description 109
- 230000002285 radioactive effect Effects 0.000 title claims abstract description 48
- 238000002360 preparation method Methods 0.000 title claims abstract description 17
- 239000002245 particle Substances 0.000 claims abstract description 88
- 239000011241 protective layer Substances 0.000 claims abstract description 26
- 239000011159 matrix material Substances 0.000 claims abstract description 17
- 239000003758 nuclear fuel Substances 0.000 claims abstract description 12
- 235000015895 biscuits Nutrition 0.000 claims description 65
- 239000010410 layer Substances 0.000 claims description 41
- 238000003825 pressing Methods 0.000 claims description 31
- 239000011812 mixed powder Substances 0.000 claims description 23
- 239000011268 mixed slurry Substances 0.000 claims description 22
- 238000000034 method Methods 0.000 claims description 20
- 239000008188 pellet Substances 0.000 claims description 19
- 239000002296 pyrolytic carbon Substances 0.000 claims description 19
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 13
- 238000000498 ball milling Methods 0.000 claims description 13
- 238000000227 grinding Methods 0.000 claims description 13
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 12
- 229910052799 carbon Inorganic materials 0.000 claims description 12
- 239000011248 coating agent Substances 0.000 claims description 12
- 238000000576 coating method Methods 0.000 claims description 12
- 238000001272 pressureless sintering Methods 0.000 claims description 11
- 238000000748 compression moulding Methods 0.000 claims description 10
- 229920002873 Polyethylenimine Polymers 0.000 claims description 9
- 229910004298 SiO 2 Inorganic materials 0.000 claims description 8
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 8
- 238000009718 spray deposition Methods 0.000 claims description 8
- 239000004677 Nylon Substances 0.000 claims description 7
- 229920001778 nylon Polymers 0.000 claims description 7
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 6
- 230000006835 compression Effects 0.000 claims description 6
- 238000007906 compression Methods 0.000 claims description 6
- 238000002156 mixing Methods 0.000 claims description 6
- 239000006185 dispersion Substances 0.000 claims description 5
- 230000005855 radiation Effects 0.000 claims description 5
- 239000002131 composite material Substances 0.000 claims description 4
- 238000000465 moulding Methods 0.000 claims description 4
- 239000002270 dispersing agent Substances 0.000 claims description 3
- 238000001035 drying Methods 0.000 claims description 3
- 230000004992 fission Effects 0.000 abstract description 10
- PEDCQBHIVMGVHV-UHFFFAOYSA-N glycerol group Chemical group OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 description 18
- 239000002002 slurry Substances 0.000 description 16
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 12
- 239000000843 powder Substances 0.000 description 12
- 239000007921 spray Substances 0.000 description 12
- 238000013461 design Methods 0.000 description 10
- 238000010438 heat treatment Methods 0.000 description 9
- 238000007723 die pressing method Methods 0.000 description 7
- 238000004519 manufacturing process Methods 0.000 description 7
- 239000000203 mixture Substances 0.000 description 7
- 229910000711 U alloy Inorganic materials 0.000 description 6
- 229910052786 argon Inorganic materials 0.000 description 6
- 239000011230 binding agent Substances 0.000 description 6
- 238000001816 cooling Methods 0.000 description 6
- 238000005238 degreasing Methods 0.000 description 6
- 235000019441 ethanol Nutrition 0.000 description 6
- 238000013329 compounding Methods 0.000 description 5
- 239000007789 gas Substances 0.000 description 5
- 238000011166 aliquoting Methods 0.000 description 4
- 238000000889 atomisation Methods 0.000 description 4
- 238000000151 deposition Methods 0.000 description 4
- 230000000694 effects Effects 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- 239000003595 mist Substances 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- 238000005303 weighing Methods 0.000 description 4
- 229910001093 Zr alloy Inorganic materials 0.000 description 3
- 238000000280 densification Methods 0.000 description 3
- 238000012986 modification Methods 0.000 description 3
- 230000004048 modification Effects 0.000 description 3
- 238000012545 processing Methods 0.000 description 2
- 239000000941 radioactive substance Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 239000000758 substrate Substances 0.000 description 2
- 238000000429 assembly Methods 0.000 description 1
- 230000000712 assembly Effects 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 238000005336 cracking Methods 0.000 description 1
- 238000004132 cross linking Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 238000010297 mechanical methods and process Methods 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 230000001681 protective effect Effects 0.000 description 1
- 238000012827 research and development Methods 0.000 description 1
- 238000012552 review Methods 0.000 description 1
- 230000000630 rising effect Effects 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
Classifications
-
- 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
- G21C3/02—Fuel elements
- G21C3/04—Constructional details
- G21C3/045—Pellets
-
- 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
- G21C21/10—Manufacture of fuel elements or breeder elements contained in non-active casings by extrusion, drawing, or stretching by rolling, e.g. "picture frame" technique
-
- 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
-
- 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
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C7/00—Control of nuclear reaction
- G21C7/02—Control of nuclear reaction by using self-regulating properties of reactor materials, e.g. Doppler effect
- G21C7/04—Control of nuclear reaction by using self-regulating properties of reactor materials, e.g. Doppler effect of burnable poisons
-
- 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
Landscapes
- 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)
- Chemical Kinetics & Catalysis (AREA)
- Monitoring And Testing Of Nuclear Reactors (AREA)
Abstract
The invention provides a hollow radioactive contained fuel containing burnable poison, a preparation method and application thereof, comprising the following steps: a hollow fuel zone and a fuel-free protective layer coated on the periphery of the fuel zone; the hollow fuel zone comprises a matrix and fuel elements and burnable poison distributed in the matrix; the fuel element is isotropically coated fuel particles and the burnable poison is isotropically coated burnable poison particles. The invention can realize the radioactive containment of the reactor fuel with high compactness and high safety, ensures that radioactive products, especially fission gas, are not released into the environment under accidents, provides fission sites for the long-period stability of the core of the miniature nuclear power supply, effectively restricts the radioactive fission products in the fuel and provides guarantee for the safe and stable operation of the reactor.
Description
Technical Field
The invention relates to fuel, in particular to hollow radioactive inclusion fuel containing burnable poison, a preparation method and application thereof.
Background
The miniature nuclear power supply is an energy device facing to remote areas of sea, space and land, can meet energy supply requirements in civil, military and other aspects, and has the advantages of high energy density, strong continuous high power output capability, large power adjustable range, low dependence on external substances (no need of oxidizing agents, nuclear fuel storage and the like) and the like compared with the conventional power supply.
The high safety of the reactor is an essential element of the safety review and commercial operation of the micro nuclear power source, which requires the fuel to have high inclusion of radioactive substances under accident conditions. Because the conventional UO2+Zr alloy nuclear fuel system is used in the pressurized water reactor at present, potential nuclear leakage risks exist under accident working conditions, fuel elements are exposed to high-temperature, high-pressure and strong-corrosion environments and undergo rapid temperature and pressure rising and falling, performances such as performance degradation, cracking and the like can occur, and a protective barrier is damaged to cause radioactive substance leakage; meanwhile, the arrangement mode of the non-uniform arrangement of the fuel rods and the burnable poison rods makes the reactor core of the reactor huge in volume, and cannot meet the requirement of high compactness of the miniature nuclear power supply. Therefore, the development of the accident fault-tolerant fuel design suitable for the micro nuclear power system has very important significance.
The fuel research and development in the field of micro nuclear power sources in China is late, and most of current designs are still traditional UO 2 The accident fault tolerance capability of the structural design of the +Zr alloy fuel system is weak, and the avoidance of the leakage risk of reflective substances cannot be ensured. For the pressureless sintering scheme adopted by accident-resistant fuel suitable for miniature nuclear power supply, the method is different from the traditional UO 2 Fuel pellets, need to be filledThe requirements of the core body, the distribution of burnable poison and the safety are met, and the special use scene of the miniature nuclear power supply is considered, so that a high-safety fuel preparation scheme is provided. Therefore, the design and preparation scheme of the hollow radioactive inclusion fuel containing the burnable poison are formed by combining various factors such as radiation shielding, thermodynamic performance, manufacturing process and the like.
Disclosure of Invention
Aiming at the defects in the prior art, the invention aims to provide a hollow radioactive containing fuel containing a burnable poison, which has the characteristics of excellent anti-irradiation performance, good fissile gas containing performance, high heat conductivity and excellent safety performance; meanwhile, a preparation method of the hollow radioactive-contained fuel containing the burnable poison is also provided, and the preparation method adopts a pressureless sintering method to prepare the dispersion type fuel pellets containing the burnable poison, so that the preparation and production efficiency are greatly improved while densification is realized, and the purpose of industrialized mass production is realized.
The invention provides a hollow radioactive containment fuel containing a burnable poison, which comprises a hollow fuel zone and a fuel-free protective layer coated on the periphery of the fuel zone;
the hollow fuel zone comprises a matrix and fuel elements and burnable poison uniformly distributed in the matrix;
the substrate is a SiC substrate, the fuel element is three layers of isotropic coated fuel particles (TRISO), the burnable poison is double layers of isotropic coated burnable poison particles (BISO), and the fuel-free zone protective layer is made of SiC.
Further, the density of the matrix and the fuel-free protective layer is not less than 95%.
Further, the coated fuel particles comprise a fuel core and four protective layers coated outside the fuel core;
the four protective layers are a loose carbon layer (Buffer), an inner pyrolytic carbon (IPyC) layer, a SiC layer and an outer pyrolytic carbon (OPyC) layer from inside to outside in sequence;
the fuel core is UO 2 、UC、UN、U 3 Si 2 In U-alloy or other arbitrary nuclear fuelOne or more of (C) and (U) O 2 、UC、UN、U 3 Si 2 In U alloys or other nuclear fuels 235 The U enrichment degree is 2-20%;
the density of the loose carbon layer is 1.1g/cm 3 The thickness is 95 mu m;
the density of the inner pyrolytic carbon layer is 1.9g/cm 3 The thickness is 30-60 mu m;
the density of the SiC layer is 3.18g/cm 3 The thickness is 25-55 mu m;
the density of the outer pyrolytic carbon layer is 1.9g/cm 3 The thickness is 30-60 mu m;
the coated fuel particles have a diameter of 400-800 μm.
Further, the coated burnable poison particles comprise burnable poison cores and two protective layers coated outside the burnable poison cores;
the two protective layers are a loose carbon layer and a compact pyrolytic carbon layer from inside to outside in sequence;
the core of the burnable poison is B 4 C、Gd 2 O 3 Or one or more of other burnable poisons;
the density of the loose carbon layer is 1.1g/cm 3 The thickness is 80-100 mu m;
the density of the dense pyrolytic carbon layer is 1.9g/cm 3 The thickness is 80-100 mu m;
the diameter of the coated burnable poison particles is 200-400 mu m.
Further, the coated fuel particles account for 30-50% of the volume of the pellet fuel;
the BISO coated burnable poison particles account for 5-15% of the volume of the pellet fuel;
the thickness of the fuel-free area protective layer is 0.2-2mm.
The invention provides a preparation method of a hollow radioactive inclusion fuel containing a burnable poison, which comprises the following steps:
step S1: preparing SiC mixed slurry and SiC mixed powder;
step S2: coating the SiC mixed slurry on fuel particles and burnable poison particles by a spray deposition method, wherein the binder is glycerol which is diluted by absolute ethyl alcohol and has the concentration of 10-15%;
step S3: carrying out compression molding on the fuel particles coated with SiC and the burnable poison particles to obtain a biscuit of a fuel area;
step S4: molding the SiC mixed powder to obtain a biscuit without a fuel area;
step S5: the fuel zone biscuit and the non-fuel zone biscuit are compositely pressed into a radioactive containing dispersion core block fuel biscuit containing combustible poison;
step S6: carrying out pressureless sintering on the radioactive containing dispersion core block fuel biscuit containing the burnable poison in a vacuum furnace;
step S7: the sintered compact is machine-added to the final size pellet fuel.
Further, the SiC mixed slurry contains 85-95% of SiC and 1-10% of Al by weight percent 2 O 3 1-10% of Y 2 O 3 0.5-10% of SiO 2 And 0.5 to 5% of polyethyleneimine as dispersant.
Further, placing each component of the SiC mixed slurry into a nylon ball milling tank, adding 1-2 times of alcohol of the total mass to mix, adding 3 times of zirconia grinding balls or alumina grinding balls of the total mass to ball mill for 24 hours to obtain the SiC mixed slurry;
and drying the SiC mixed slurry to obtain SiC mixed powder.
Further, the operation temperature of the step S2 is 70-100 ℃;
the compression pressure of the mould pressing in the step S3 is 20-60 MPa, and the obtained fuel zone biscuit is hollow columnar;
the compression pressure of the mould pressing in the step S4 is 20-60 MPa, the obtained fuel-free zone biscuit comprises an upper cover, a lower cover and an annular cylinder, the thickness is 2-4mm, and the fit clearance between the fuel-free zone biscuit and the fuel-free zone biscuit is 0.1-0.25mm;
the pressure of the composite pressing in the step S5 is higher than the pressing pressure of the pressing in the step S3 and the pressing pressure of the pressing in the step S4.
Further, the pressure of the composite pressing in the step S5 is 60-80 MPa.
Further, in the step S6, firstly, the temperature is raised to 600 ℃ at the speed of 5-10 ℃/min and is kept for 0.5-2h, degreasing treatment is carried out, the vacuum degree is 10 < -2 > -10Pa, then argon is introduced for protection, the pressure is 10-50kPa, the temperature is raised to 1700-1900 ℃ at the speed of 2-10 ℃/min, and the temperature is kept for 1-5h, and the furnace is cooled.
The invention also provides the application of the hollow radioactive containment fuel containing the burnable poison in processing nuclear fuel pellets according to the size of a fuel assembly in a microminiature nuclear reactor.
Compared with the prior art, the invention has the following beneficial effects:
the hollow radioactive containment fuel containing the burnable poison can realize high-compactness and high-safety radioactive containment of the reactor fuel, ensure that radioactive products, particularly fission gas, are not released into the environment in the event of an accident, stably provide a fission field for the long-period of a miniature nuclear power reactor core, effectively restrict the radioactive fission products in the fuel and provide a guarantee for safe and stable operation of the reactor.
Drawings
Other features, objects and advantages of the present invention will become more apparent upon reading of the detailed description of non-limiting embodiments, given with reference to the accompanying drawings in which:
FIG. 1 is a schematic view of a hollow radioactive package fuel containing a burnable poison in one direction according to an embodiment of the present invention;
FIG. 2 is a schematic view of another direction of a hollow radioactive package fuel containing a burnable poison according to an embodiment of the present invention;
FIG. 3 is a flow chart of a method of preparing a hollow, radiation-containing fuel containing a burnable poison according to an embodiment of the present invention.
In the figure:
1 is a SiC fuel-free zone; 2 is TRISO fuel particles; 3 is BISO burnable poison particle; 4 is a hollow area; and 5 is a compact SiC matrix.
Detailed Description
The present invention will be described in detail with reference to specific examples. The following examples will assist those skilled in the art in further understanding the present invention, but are not intended to limit the invention in any way. It should be noted that variations and modifications could be made by those skilled in the art without departing from the inventive concept. These are all within the scope of the present invention.
The invention aims to provide a hollow radioactive containment fuel containing burnable poison, which can realize high-compactness and high-safety radioactive containment of reactor fuel, ensure that radioactive products, particularly fission gas, are not released into the environment in case of accidents, stably provide fission sites for the long-period of a miniature nuclear power reactor core, effectively restrict the radioactive fission products in the fuel and provide guarantee for safe and stable operation of the reactor.
As shown in fig. 1, the hollow radioactive containment fuel containing the burnable poison comprises an annular fuel zone and a fuel-free protective layer coated on the periphery of the fuel zone, wherein the annular fuel zone comprises a matrix, fuel elements and the burnable poison uniformly distributed in the matrix, the matrix is compact SiC, the fuel elements are three layers of isotropically coated fuel particles, particularly TRISO particles, the burnable poison is two layers of isotropically coated burnable poison particles, particularly BISO particles, and the fuel-free protective layer is made of SiC.
The density of the matrix and the protective layer of the fuel-free area is not less than 95%, the TRISO coated fuel particles comprise a fuel core and four protective layers coated outside the fuel core, and the four protective layers comprise a loose carbon layer, an inner pyrolytic carbon layer, a SiC layer and an outer pyrolytic carbon layer from inside to outside in sequence; the fuel core is UO 2 、UC、UN、U 3 Si 2 One or more of U alloy or other nuclear fuel, and the fuel core is UO 2 、UC、UN、U 3 Si 2 One or more of U alloy or other nuclear fuel, and said UO 2 、UC、UN、U 3 Si 2 In U alloys or other nuclear fuels 235 The U enrichment degree is 2-20%, and the density of the loose carbon layer is 1.1g/cm 3 A thickness of 95 μm, the density of the inner pyrolytic carbon layer is 1.9g/cm 3 A thickness of 30-60 μm, the SiC layer having a density of 3.18g/cm 3 The thickness of the outer pyrolytic carbon layer is 25-55 mu m, and the density of the outer pyrolytic carbon layer is 1.9g/cm 3 The thickness is 30-60 mu m; the TRISO coated fuel particles have a diameter of 400-600 μm. The BISO coated burnable poison particles comprise burnable poison cores and two protective layers coated outside the burnable poison cores, wherein the two protective layers are a loose carbon layer and a compact pyrolytic carbon layer in sequence from inside to outside; the core of the burnable poison is B 4 C、Gd 2 O 3 Or one or more of other burnable poison, the loose carbon layer having a density of 1.1g/cm 3 A thickness of 80-100 μm, the density of the dense pyrolytic carbon layer is 1.9g/cm 3 The thickness is 80-100 mu m; the diameter of the BISO coated fuel particles is 200-240 mu m.
The volume fractions of the TRISO coated fuel particles and the BISO coated burnable poison particles in the pellet fuel are respectively 30-50% and 5-15%, and the thickness of the protective layer of the fuel-free area is 0.2-2mm.
The main components of the hollow radioactive-containing fuel containing the burnable poison comprise 30-50 vol.% of TRISO particles, 5-15 vol.% of BISO particles, a compact SiC matrix and a fuel-zone-free protective layer, wherein the TRISO particles are made of UO 2 、UC、UN、U 3 Si 2 One or more of U alloy or other nuclear fuels are fuel cores, and sequentially comprise a loose carbon layer, an inner pyrolytic carbon layer, a SiC layer and an outer pyrolytic carbon layer from inside to outside; BISO particles as B 4 C、Gd 2 O 3 Or one or more of other burnable poison is burnable poison core, which is composed of loose carbon layer and compact pyrolytic carbon layer from inside to outside; the density of the compact SiC matrix and the protective layer of the SiC fuel-free area is higher than 95%, the integrity of fuel particles and burnable poison particles is kept good, the compact SiC matrix is tightly combined with the interface of TRISO and BISO, the hollow radioactive contained fuel containing burnable poison has good heat conducting property and irradiation resistance, and has enough mechanical strength and excellent fissile gas inclusion, and compared with the fuel assembly of the traditional UO2 pellet+Zr alloy, the hollow radioactive contained fuel containing burnable poison is safeThe fuel assembly has the advantages of remarkably improved performance, capability of being used for fuel assemblies of ultra-compact reactors in micro nuclear power sources, and wide industrial prospect.
As shown in fig. 2, the preparation method of the hollow radioactive package fuel containing the burnable poison comprises the following steps:
step 1: preparing SiC mixed slurry and SiC mixed powder;
step 2: coating the SiC mixed slurry on fuel particles and burnable poison particles by a spray deposition method, wherein the binder is glycerol which is diluted by absolute ethyl alcohol and has the concentration of 10-15%;
step 3: carrying out compression molding on the fuel particles coated with SiC and the burnable poison particles to obtain a biscuit of a fuel area;
step 4: molding the SiC mixed powder to obtain a biscuit without a fuel area;
step 5: the fuel zone biscuit and the fuel-free zone biscuit are compositely pressed into a hollow radioactive fuel-containing biscuit containing combustible poison;
step 6: the hollow radioactive inclusion fuel biscuit containing the burnable poison is sintered in a vacuum furnace in a pressureless way;
step 7: the sintered compact is machine-added to the final size pellet fuel.
The SiC mixed slurry comprises 85-95% of SiC and 1-10% of Al by weight percent 2 O 3 1-10% of Y 2 O 3 0.5-10% of SiO 2 And 0.5 to 5% of polyethyleneimine as dispersant.
Placing the components in a nylon ball milling tank, adding 1-2 times of alcohol with the total mass of the components, mixing, adding 2-3 times of zirconia grinding balls or alumina grinding balls with the total mass, ball milling for 6-24 hours to obtain SiC mixed slurry, and drying to obtain SiC mixed powder.
The operation temperature of the step 2 is 70-100 ℃; the pressing pressure of the die pressing in the step 3 is 10-60 MPa, the dwell time is 10-20s,
the obtained fuel zone biscuit is hollow columnar; the compression pressure of the die pressing in the step 4 is 10-60 MPa, the obtained fuel-free zone biscuit comprises an upper cover, a lower cover and an annular cylinder, the thickness is 2-4mm, and the fit clearance between the fuel-free zone biscuit and the fuel-free zone biscuit is 0.1-0.25mm; the pressure of the compound pressing in the step 5 is higher than the pressing pressure of the pressing in the step 3 and the pressing pressure of the pressing in the step 4.
The pressure of the composite pressing in the step 5 is 60-80 MPa, in the step 6, firstly, the temperature is raised to 600 ℃ at the speed of 5-10 ℃/min, the temperature is kept for 0.5-2h, degreasing treatment is carried out, and the vacuum degree is 10 -2 And (3) introducing argon for protection, heating to 1600-2000 ℃ at the speed of 2-10 ℃/min under the pressure of 20-60kPa, and preserving heat for 1-5h, and cooling.
The invention adopts SiC and Y 2 O 3 、SiO 2 Preparing SiC mixed slurry and SiC mixed powder from polyethylenimine, coating the SiC mixed slurry on fuel particles and burnable poison particles by a spray deposition method to form a compact SiC matrix so as to prepare a fuel zone biscuit, molding the SiC mixed powder into a fuel-free zone biscuit, compounding and pressing the fuel zone biscuit and the fuel-free zone biscuit into a hollow radioactive-contained fuel biscuit containing burnable poison, carrying out pressureless sintering on the hollow radioactive-contained fuel biscuit containing burnable poison in a vacuum furnace at high temperature, and mechanically processing the sintered biscuit into a fuel assembly in a water pile according to the required size after cooling; the invention adopts a pressureless sintering method to prepare the hollow radioactive-containing fuel containing the burnable poison, thereby realizing densification and simultaneously greatly improving the preparation and production efficiency and effectively realizing the purpose of industrialized mass production.
The hollow radioactive contained fuel containing the burnable poison prepared by the preparation method can be finally processed into the fuel assembly of the water reactor by adopting a pure mechanical method according to the size of the fuel assembly of the water reactor in the nuclear reactor.
For the purpose of further illustrating the invention, several preferred embodiments are provided below.
Example 1:
step 1: weighing the powder according to the following specification and proportion: siC,85wt.%; al (Al) 2 O 3 ，5wt.％；Y 2 O 3 ，5wt.％；SiO 2 3wt%; a Polyethyleneimine (PEI) having a cross-linking group,molecular weight 800,2wt.%. Mixing the powder with alcohol with equal mass, placing the mixture into a nylon ball milling tank, wherein the grinding balls adopt zirconia balls, the ball-to-material ratio is 3:1, and ball milling for 24 hours to obtain SiC slurry. Aliquoting the slurry, one serving for coating the fuel particles and the burnable poison particles; the other part is dried for 16-24 hours at the temperature of 60-100 ℃ and sieved to obtain SiC mixed powder.
Step 2: the SiC mixed slurry is coated on fuel particles and burnable poison particles by a spray deposition method, and the binder is glycerol which is diluted by absolute ethyl alcohol and has the concentration of 12 percent. The fuel particles and the burnable poison particles were placed on a shaker and subjected to a temperature of 70 ℃. And (3) forming mist slurry by using the SiC slurry prepared in the step (I) through a spray generator, and depositing SiC powder on the surfaces of the fuel particles and the burnable poison particles. The proper atomization effect is modulated by adjusting parameters such as the angle, the opening size, the spray pressure, the flow speed and the like of the spray generator. Different TRISO and BISO volume fractions can be obtained by coating SiC mixed powders of different masses.
Step 3: and (3) carrying out compression molding on the fuel particles coated with SiC and the burnable poison particles to obtain a biscuit in the fuel area. And designing a hollow columnar die according to the size requirement of the fuel area, and performing compression molding under the pressure of 20 MPa.
Step 4: and (3) carrying out mould pressing forming on the SiC mixed powder to obtain the biscuit in the fuel-free area. The biscuit in the fuel-free zone comprises an upper cover, a lower cover and an annular cylinder, the thickness of the biscuit is 2mm, and the fit clearance between the biscuit and the fuel zone is 0.1mm. And (3) carrying out die design according to the specific fuel-free area size requirement, and carrying out die pressing forming under the pressure of 40 MPa.
Step 5: and (3) compounding and pressing the fuel zone biscuit and the fuel-free zone to form a hollow radioactive-containing fuel biscuit containing the burnable poison. The mold is designed according to the specific size, and the mold is molded under the pressure of 60 MPa.
Step 6: pressureless sintering is performed in a vacuum furnace. Firstly, heating to 600 ℃ at a rate of 5/min, preserving heat for 0.5h, degreasing, and carrying out vacuum degree of 10 -2 Pa. Then argon is introduced for protection, and the pressure is 50kPa. Heating to 1700 ℃ at the speed of 10 ℃/min, preserving heat for 1h, and cooling in a furnace.
Step 7: and grinding redundant fuel-free areas according to the pellet size requirement to obtain the final-size pellet fuel.
Example 2:
the method comprises the following steps: weighing the powder according to the following specification and proportion: siC,86wt.%; al (Al) 2 O 3 ，2wt.％；Y 2 O 3 ，4wt.％；SiO 2 3wt.%; polyethyleneimine, molecular weight 1800,5wt.%. Mixing the powder with alcohol with twice the mass, putting the mixture into a nylon ball milling tank, and ball milling the mixture for 24 hours by adopting alumina balls with the ball-to-material ratio of 3:1 to obtain SiC slurry. Aliquoting the slurry, one serving for coating the fuel particles and the burnable poison particles; the other part is dried for 24 hours at 80 ℃ and sieved to obtain SiC mixed powder.
Step 2: the SiC mixed slurry is coated on fuel particles and burnable poison particles by a spray deposition method, and the binder is glycerol which is diluted by absolute ethyl alcohol and has the concentration of 10 percent. The fuel particles and the burnable poison particles were placed on a shaker and subjected to a temperature of 100 ℃. And (3) forming mist slurry by using the SiC slurry prepared in the step (I) through a spray generator, and depositing SiC powder on the surfaces of the fuel particles and the burnable poison particles. The proper atomization effect is modulated by adjusting parameters such as the angle, the opening size, the spray pressure, the flow speed and the like of the spray generator. Different TRISO and BISO volume fractions can be obtained by coating SiC mixed powders of different masses.
Step 3: and (3) carrying out compression molding on the fuel particles coated with SiC and the burnable poison particles to obtain a biscuit in the fuel area. And designing a hollow columnar die according to the size requirement of the fuel area, and performing compression molding under the pressure of 60 MPa.
Step 4: and (3) carrying out mould pressing forming on the SiC mixed powder to obtain the biscuit in the fuel-free area. The biscuit in the fuel-free zone comprises an upper cover, a lower cover and an annular cylinder, the thickness of the biscuit is 4mm, and the fit clearance between the biscuit and the fuel zone is 0.25mm. And (3) carrying out die design according to the specific fuel-free area size requirement, and carrying out die pressing forming under the pressure of 30 MPa.
Step 5: and (3) compounding and pressing the fuel zone biscuit and the fuel-free zone to form a hollow radioactive-containing fuel biscuit containing the burnable poison. The mold is designed according to the specific size, and the mold is molded under the pressure of 60 MPa.
Step 6: pressureless sintering is performed in a vacuum furnace. Firstly, heating to 600 ℃ at a speed of 10 ℃/min, preserving heat for 2 hours, degreasing, and carrying out vacuum degree of 1Pa. Then argon is introduced for protection, and the pressure is 10kPa. Heating to 1900 ℃ at a speed of 2 ℃/min, preserving heat for 5 hours, and cooling in a furnace.
Step 7: and grinding redundant fuel-free areas according to the pellet size requirement to obtain the final-size pellet fuel.
Example 3:
the method comprises the following steps: weighing the powder according to the following specification and proportion: siC,92wt.%; al (Al) 2 O 3 ，1wt.％；Y 2 O 3 ，1wt.％；SiO 2 5wt.%; polyethyleneimine, molecular weight 1800,1wt.%. Mixing the powder with 1.5 times of alcohol by mass, placing the mixture into a nylon ball milling tank, and ball milling the mixture for 24 hours to obtain SiC slurry, wherein the grinding balls are alumina balls with a ball-to-material ratio of 3:1. Aliquoting the slurry, one serving for coating the fuel particles and the burnable poison particles; the other part is dried for 24 hours at 80 ℃ and sieved to obtain SiC mixed powder.
Step 2: the SiC mixed slurry is coated on fuel particles and burnable poison particles by a spray deposition method, and the binder is glycerol which is diluted by absolute ethyl alcohol and has the concentration of 13 percent. The fuel particles and burnable poison particles were placed on a shaker and subjected to a temperature of 85 ℃. And (3) forming mist slurry by using the SiC slurry prepared in the step (I) through a spray generator, and depositing SiC powder on the surfaces of the fuel particles and the burnable poison particles. The proper atomization effect is modulated by adjusting parameters such as the angle, the opening size, the spray pressure, the flow speed and the like of the spray generator. Different TRISO and BISO volume fractions can be obtained by coating SiC mixed powders of different masses.
Step 3: and (3) carrying out compression molding on the fuel particles coated with SiC and the burnable poison particles to obtain a biscuit in the fuel area. And designing a hollow columnar die according to the size requirement of the fuel area, and performing compression molding under the pressure of 40 MPa.
Step 4: and (3) carrying out mould pressing forming on the SiC mixed powder to obtain the biscuit in the fuel-free area. The biscuit in the fuel-free zone comprises an upper cover, a lower cover and an annular cylinder, the thickness of the biscuit is 2mm, and the fit clearance between the biscuit and the fuel zone is 0.1mm. And (3) carrying out die design according to the specific fuel-free area size requirement, and carrying out die pressing forming under the pressure of 60 MPa.
Step 5: and (3) compounding and pressing the fuel zone biscuit and the fuel-free zone to form a hollow radioactive-containing fuel biscuit containing the burnable poison. The mold was designed according to the specific dimensions and was compression molded under a pressure of 40 MPa.
Step 6: pressureless sintering is performed in a vacuum furnace. Firstly, heating to 600 ℃ at the rate of 8/min, preserving heat for 1h, degreasing, and carrying out vacuum degree of 10Pa. Then argon is introduced for protection, and the pressure is 30kPa. Heating to 1800 ℃ at a speed of 5 ℃/min, preserving heat for 3 hours, and cooling in a furnace.
Step 7: and grinding redundant fuel-free areas according to the pellet size requirement to obtain the final-size pellet fuel.
Example 4:
the method comprises the following steps: weighing the powder according to the following specification and proportion: siC,95wt.%; al (Al) 2 O 3 ，1.5wt.％；Y 2 O 3 ，2wt.％；SiO 2 1wt.%; polyethyleneimine, molecular weight 1800,0.5wt.%. Mixing the powder with 1.8 times of alcohol by mass, placing the mixture into a nylon ball milling tank, and ball milling the mixture for 24 hours to obtain SiC slurry, wherein the grinding balls are alumina balls with a ball-to-material ratio of 3:1. Aliquoting the slurry, one serving for coating the fuel particles and the burnable poison particles; the other part is dried for 24 hours at 80 ℃ and sieved to obtain SiC mixed powder.
Step 2: the SiC mixed slurry is coated on fuel particles and burnable poison particles by a spray deposition method, and the binder is glycerol which is diluted by absolute ethyl alcohol and has the concentration of 15 percent. The fuel particles and the burnable poison particles were placed on a shaker and subjected to a temperature of 90 ℃. And (3) forming mist slurry by using the SiC slurry prepared in the step (I) through a spray generator, and depositing SiC powder on the surfaces of the fuel particles and the burnable poison particles. The proper atomization effect is modulated by adjusting parameters such as the angle, the opening size, the spray pressure, the flow speed and the like of the spray generator. Different TRISO and BISO volume fractions can be obtained by coating SiC mixed powders of different masses.
Step 3: and (3) carrying out compression molding on the fuel particles coated with SiC and the burnable poison particles to obtain a biscuit in the fuel area. And (3) carrying out die design according to the size requirement of the fuel area, and carrying out die pressing forming under the pressure of 45 MPa.
Step 4: and (3) carrying out mould pressing forming on the SiC mixed powder to obtain the biscuit in the fuel-free area. The biscuit in the fuel-free zone comprises an upper cover, a lower cover and an annular cylinder, the thickness of the biscuit is 3mm, and the fit clearance between the biscuit and the fuel zone is 0.15mm. And (3) carrying out die design according to the specific fuel-free area size requirement, and carrying out die pressing forming under the pressure of 55 MPa.
Step 5: and (3) compounding and pressing the fuel zone biscuit and the fuel-free zone to form a hollow radioactive-containing fuel biscuit containing the burnable poison. The hollow columnar mould is designed according to specific size, and is molded under the pressure of 70 MPa.
Step 6: pressureless sintering is performed in a vacuum furnace. Firstly, heating to 600 ℃ at the speed of 8 ℃/min, preserving heat for 1.5h, degreasing, and carrying out vacuum degree of 10Pa. Then argon is introduced for protection, and the pressure is 20kPa. Heating to 1850 ℃ at a speed of 5 ℃/min, preserving heat for 2 hours, and cooling in a furnace.
Step 7: and grinding redundant fuel-free areas according to the pellet size requirement to obtain the final-size pellet fuel.
The hollow radioactive inclusion fuel containing the burnable poison in the embodiment of the invention has the characteristics of excellent irradiation resistance, good inclusion of fission gas, high thermal conductivity and excellent safety performance, the preparation method is scientific, the process flow is simple, the hollow radioactive inclusion fuel containing the burnable poison is prepared by adopting a pressureless sintering method, the preparation and production efficiency are greatly improved while densification is realized, the purpose of industrialized mass production can be realized, and the preparation method has outstanding substantive characteristics and remarkable progress.
The above 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 color changes made in the main design concept and spirit of the present invention are still consistent with the present invention, and all the technical problems to be solved are included in the scope of the present invention.
The foregoing describes specific embodiments of the present invention. It is to be understood that the invention is not limited to the particular embodiments described above, and that various changes and modifications may be made by one skilled in the art within the scope of the claims without affecting the spirit of the invention.
Claims (10)
1. A hollow, radiation-containing fuel containing a burnable poison, comprising: a hollow fuel zone and a fuel-free protective layer coated on the periphery of the fuel zone;
the hollow fuel zone comprises a matrix and fuel elements and burnable poison distributed in the matrix;
the fuel element is isotropically coated fuel particles and the burnable poison is isotropically coated burnable poison particles.
2. The hollow, radiation-containing fuel containing burnable poison of claim 1, wherein the matrix and the fuel-free protective layer have a density of not less than 95%.
3. The burnable poison containing hollow radioactive package fuel of claim 1, wherein the coated fuel particles comprise a fuel core and a first protective layer coated over the fuel core;
the first protective layer at least comprises a loose carbon layer, an inner pyrolytic carbon layer, a SiC layer and an outer pyrolytic carbon layer from inside to outside.
4. The hollow, radiation-containing fuel containing a burnable poison of claim 1, wherein the coated burnable poison particles comprise a burnable poison core and a second protective layer coated over the burnable poison core;
the second protective layer is a loose carbon layer and a compact pyrolytic carbon layer from inside to outside in sequence.
5. The burnable poison containing hollow radioactive package fuel of claim 1 wherein the coated fuel particles have a diameter of 400-800 μm;
the diameter of the coated burnable poison particles is 200-400 mu m;
the thickness of the fuel-free area protective layer is 0.2-2mm.
6. A method for preparing a hollow radioactive containment fuel containing a burnable poison, which is characterized by comprising the following steps:
step S1: preparing SiC mixed slurry and SiC mixed powder;
step S2: coating the SiC mixed slurry on fuel particles and burnable poison particles by a spray deposition method;
step S3: carrying out compression molding on the fuel particles coated with SiC and the burnable poison particles to obtain a biscuit of a fuel area;
step S4: molding the SiC mixed powder to obtain a biscuit without a fuel area;
step S5: the fuel zone biscuit and the non-fuel zone biscuit are compositely pressed into a radioactive containing dispersion core block fuel biscuit containing combustible poison;
step S6: carrying out pressureless sintering on the radioactive containing dispersion core block fuel biscuit containing the burnable poison in a vacuum furnace;
step S7: the sintered compact is machine-added to the final size pellet fuel.
7. The method for preparing a hollow radioactive package fuel containing a burnable poison according to claim 6, wherein the SiC mixed slurry contains 85 to 95% of SiC and 1 to 10% of Al by weight 2 O 3 1-10% of Y 2 O 3， 0.5-10% SiO 2 And 0.5 to 5% of polyethyleneimine as dispersant.
8. The preparation method of the hollow radioactive-containing fuel containing the burnable poison according to claim 7, wherein each component of the SiC mixed slurry is placed in a nylon ball milling tank, alcohol with the total mass being 1-2 times of the total mass is added for mixing, and zirconia grinding balls or alumina grinding balls with the total mass being 2-5 times of the total mass are added for ball milling for 10-30 hours to obtain the SiC mixed slurry;
and drying the SiC mixed slurry to obtain the SiC mixed powder.
9. The method for preparing a hollow radioactive package fuel containing a burnable poison according to claim 6, wherein the operation temperature of the step S2 is 70 to 100 ℃;
the compression pressure of the mould pressing in the step S3 is 20-60 MPa, and the obtained fuel zone biscuit is hollow columnar;
the compression pressure of the mould pressing in the step S4 is 20-60 MPa, the obtained fuel-free zone biscuit comprises an upper cover, a lower cover and an annular cylinder, the thickness is 2-4mm, and the fit clearance between the fuel-free zone biscuit and the fuel-free zone biscuit is 0.1-0.25mm;
the pressure of the composite pressing in the step S5 is higher than the pressing pressure of the pressing in the step S3 and the pressing pressure of the pressing in the step S4.
10. A use of fuel, characterized in that the hollow, radioactive-containing fuel containing a burnable poison according to any one of claims 1 to 5 is processed into nuclear fuel pellets according to the size of the fuel assembly in a microminiature nuclear reactor.
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