CN117413321A - High-entropy ceramic inert matrix dispersion fuel pellet and preparation method thereof - Google Patents
High-entropy ceramic inert matrix dispersion fuel pellet and preparation method thereof Download PDFInfo
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- CN117413321A CN117413321A CN202180098407.0A CN202180098407A CN117413321A CN 117413321 A CN117413321 A CN 117413321A CN 202180098407 A CN202180098407 A CN 202180098407A CN 117413321 A CN117413321 A CN 117413321A
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- 239000000919 ceramic Substances 0.000 title claims abstract description 114
- 239000000446 fuel Substances 0.000 title claims abstract description 83
- 239000011159 matrix material Substances 0.000 title claims abstract description 55
- 239000006185 dispersion Substances 0.000 title claims abstract description 41
- 239000008188 pellet Substances 0.000 title claims abstract description 37
- 238000002360 preparation method Methods 0.000 title claims description 7
- 239000002245 particle Substances 0.000 claims abstract description 49
- 238000005245 sintering Methods 0.000 claims abstract description 27
- 239000000843 powder Substances 0.000 claims description 60
- 235000015895 biscuits Nutrition 0.000 claims description 51
- 239000011258 core-shell material Substances 0.000 claims description 32
- 241000013033 Triso Species 0.000 claims description 20
- 239000002270 dispersing agent Substances 0.000 claims description 17
- 239000002002 slurry Substances 0.000 claims description 17
- 238000000034 method Methods 0.000 claims description 16
- 150000004767 nitrides Chemical class 0.000 claims description 16
- 239000011812 mixed powder Substances 0.000 claims description 15
- 239000003960 organic solvent Substances 0.000 claims description 15
- 229910000711 U alloy Inorganic materials 0.000 claims description 12
- 238000003825 pressing Methods 0.000 claims description 10
- 238000002156 mixing Methods 0.000 claims description 9
- 238000005507 spraying Methods 0.000 claims description 8
- 239000011247 coating layer Substances 0.000 claims description 7
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 claims description 6
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical group [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 6
- 229910001066 Pu alloy Inorganic materials 0.000 claims description 6
- 238000000498 ball milling Methods 0.000 claims description 6
- 239000000463 material Substances 0.000 claims description 6
- 239000011224 oxide ceramic Substances 0.000 claims description 6
- 229910052574 oxide ceramic Inorganic materials 0.000 claims description 6
- 238000005096 rolling process Methods 0.000 claims description 6
- 229910021332 silicide Inorganic materials 0.000 claims description 6
- FVBUAEGBCNSCDD-UHFFFAOYSA-N silicide(4-) Chemical compound [Si-4] FVBUAEGBCNSCDD-UHFFFAOYSA-N 0.000 claims description 6
- WGTYBPLFGIVFAS-UHFFFAOYSA-M tetramethylammonium hydroxide Chemical compound [OH-].C[N+](C)(C)C WGTYBPLFGIVFAS-UHFFFAOYSA-M 0.000 claims description 6
- 229920002873 Polyethylenimine Polymers 0.000 claims description 5
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 claims description 5
- 238000001035 drying Methods 0.000 claims description 5
- 238000000227 grinding Methods 0.000 claims description 5
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 4
- 229910052581 Si3N4 Inorganic materials 0.000 claims description 4
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 claims description 4
- 229910052786 argon Inorganic materials 0.000 claims description 3
- 238000011049 filling Methods 0.000 claims description 3
- 238000001272 pressureless sintering Methods 0.000 claims description 3
- 238000002485 combustion reaction Methods 0.000 claims 1
- 230000008961 swelling Effects 0.000 abstract description 4
- 238000009776 industrial production Methods 0.000 abstract description 2
- 229910026551 ZrC Inorganic materials 0.000 description 11
- OTCHGXYCWNXDOA-UHFFFAOYSA-N [C].[Zr] Chemical compound [C].[Zr] OTCHGXYCWNXDOA-UHFFFAOYSA-N 0.000 description 11
- 239000003758 nuclear fuel Substances 0.000 description 9
- 239000002994 raw material Substances 0.000 description 7
- 238000005253 cladding Methods 0.000 description 6
- 238000010438 heat treatment Methods 0.000 description 6
- 230000007797 corrosion Effects 0.000 description 5
- 238000005260 corrosion Methods 0.000 description 5
- 239000011248 coating agent Substances 0.000 description 4
- 238000000576 coating method Methods 0.000 description 4
- 238000004321 preservation Methods 0.000 description 4
- 230000000694 effects Effects 0.000 description 2
- 230000004992 fission Effects 0.000 description 2
- 238000002844 melting Methods 0.000 description 2
- 230000008018 melting Effects 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 150000007513 acids Chemical class 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 229910052797 bismuth Inorganic materials 0.000 description 1
- JCXGWMGPZLAOME-UHFFFAOYSA-N bismuth atom Chemical compound [Bi] JCXGWMGPZLAOME-UHFFFAOYSA-N 0.000 description 1
- 125000001153 fluoro group Chemical class F* 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 229910052573 porcelain Inorganic materials 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 238000009385 rock melting Methods 0.000 description 1
- 238000002390 rotary evaporation Methods 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 239000002915 spent fuel radioactive waste Substances 0.000 description 1
- 238000009718 spray deposition Methods 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- 239000011215 ultra-high-temperature ceramic Substances 0.000 description 1
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
-
- 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
- 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
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
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- Engineering & Computer Science (AREA)
- Physics & Mathematics (AREA)
- Plasma & Fusion (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Manufacturing & Machinery (AREA)
- Chemical & Material Sciences (AREA)
- Ceramic Engineering (AREA)
- Dispersion Chemistry (AREA)
- Ceramic Products (AREA)
Abstract
The high-entropy ceramic inert matrix dispersion fuel pellet comprises a cylindrical fuel-free zone (20) and a cylindrical fuel zone (10) arranged in the fuel-free zone (20); the fuel zone (10) comprises a high-entropy ceramic matrix (11) and fuel particles (12) dispersed in the high-entropy ceramic matrix (11); the high-entropy ceramic matrix (11) and the fuel-free area (20) are both made of high-entropy ceramic through sintering. The high-entropy ceramic is used as a matrix of the inert base dispersion fuel pellet, so that the pellet has high thermal conductivity, low swelling and easy post-treatment, and is suitable for industrial production.
Description
The invention relates to the technical field of nuclear fuel, in particular to a high-entropy ceramic inert matrix dispersion fuel pellet and a preparation method thereof.
With the development of industry, the demand for energy is also increasing, and nuclear energy is favored by various industries as a clean energy source. With the rapid increase in nuclear energy utilization, the consequent safety issues are also not negligible. Wherein, the core fuel is not melted or leaked under the extreme accident environment, which is an important guarantee for the safety of the nuclear reactor. Currently, cladding is mainly adopted to ensure that nuclear fuel does not leak, but the cladding still has the possibility of being damaged. The full ceramic coated Fuel (FCM) proposed in the united states provides a significant improvement in safety by employing an inert matrix of SiC. However, the heat conductivity of the SiC inert matrix after irradiation is lower than 10W/m.K, so that the temperature of the fuel center is easy to rise, meanwhile, the SiC inert matrix of the FCM can be eroded by fission products Pd, ag, cs and the like, and the safe allowable temperature is lower than 1600 ℃.
Zirconium carbide (ZrC) is used as ultrahigh-temperature ceramic, has excellent high-temperature stability (the melting point is 3530 ℃ and high-temperature phase transition does not occur), has small absorption cross section, is resistant to corrosion of nuclear fission products, has high heat conductivity after irradiation, is resistant to corrosion of lead bismuth and molten salt, and has great prospect as an inert matrix of novel reactor dispersion fuel. However, the sintering temperature of ZrC is up to about 2200 ℃, and the high-temperature sintering is easy to cause serious coarsening of the microstructure of the material. In addition, a sintering aid is usually required to be added in the ZrC sintering process, and the use of the sintering aid not only reduces the high-temperature performance of the ZrC, but also reduces the comprehensive performances of corrosion resistance, radiation resistance and the like.
The invention aims to solve the technical problem of providing a high-entropy ceramic inert matrix dispersion fuel pellet with low sintering temperature, high thermal conductivity and low swelling rate and a preparation method thereof.
The technical scheme adopted for solving the technical problems is as follows: providing a high-entropy ceramic inert matrix dispersion fuel pellet, comprising a cylindrical fuel-free zone and a fuel zone of a cylinder arranged in the fuel-free zone; the fuel zone comprises a high-entropy ceramic matrix and fuel particles dispersed in the high-entropy ceramic matrix; the high-entropy ceramic matrix and the fuel-free area are both manufactured by sintering high-entropy ceramic.
Preferably, the high-entropy ceramic includes at least one of a high-entropy carbide ceramic, a high-entropy nitride ceramic, a high-entropy oxide ceramic, and a high-entropy silicide ceramic.
Preferably, the high entropy carbide ceramic comprises at least five of SiC, zrC, tiC, nbC, taC, VC, crC, moC and WC; the grain diameter of the powder of the high-entropy carbide ceramic is 10 nm-200 mu m.
Preferably, the high entropy nitride ceramic comprises Si 3 N 4 At least five of ZrN, tiN, nbN, taN, VN, crN, moN, WN; the grain size of the powder of the high-entropy nitride ceramic is 10 nm-200 mu m.
Preferably, the fuel particles comprise TRISO particles, UO 2 、UC、UC 2 、UN、UCN、UCO、U 3 Si 2 U alloy and PuO 2 At least one of PuC, puN, pu alloy.
Preferably, the core of the TRISO particles comprises UO 2 、UC、UC 2 、UN、UCN、UCO、U 3 Si 2 At least one of U alloy. The invention also provides a preparation method of the high-entropy ceramic inert matrix dispersion fuel pellet, which comprises the following steps:
s1, mixing high-entropy ceramic powder with a dispersing agent and an organic solvent to form slurry;
a part of slurry is dried to form mixed powder, or the high-entropy ceramic powder is mixed with a dispersing agent to form mixed powder;
s2, spraying the slurry on the surfaces of rolling fuel particles, and drying to form a coating layer adhered to the surfaces of the fuel particles;
s3, mixing a part of the mixed powder with fuel particles with a coating layer according to a proportion, and pressing to form a columnar core biscuit; pressing the other part of the mixed powder to form a cylindrical core-shell biscuit;
and S4, filling the core biscuit into the core-shell biscuit, and carrying out pressurized or pressureless sintering at the sintering temperature of 1600-1950 ℃ to form a densified high-entropy ceramic inert matrix dispersion fuel pellet.
Preferably, the high-entropy ceramic powder comprises at least one of high-entropy carbide ceramic powder, high-entropy nitride ceramic powder, high-entropy oxide ceramic powder and high-entropy silicide ceramic powder.
Preferably, the high-entropy carbide ceramic powder comprises at least five of SiC, zrC, tiC, nbC, taC, VC, crC, moC and WC, and the grain size is 10 nm-200 mu m;
the high-entropy nitride ceramic powder comprises Si 3 N 4 、ZrN、TiN、NbN、TaN、VN、CrN、MoN、At least five WN particles with the particle size of 10 nm-200 μm.
Preferably, the fuel particles comprise TRISO particles, UO 2 、UC、UC 2 、UN、UCN、UCO、U 3 Si 2 U alloy and PuO 2 At least one of PuC, puN, pu alloy;
the core of the TRISO particles comprises UO 2 、UC、UC 2 、UN、UCN、UCO、U 3 Si 2 At least one of U alloy.
Preferably, in the slurry, the mass ratio of the organic solvent to the high-entropy ceramic powder is 1:1 to 3:1, a step of; the dispersing agent accounts for 0.5-4% of the high-entropy ceramic powder by mass.
Preferably, the dispersing agent is at least one of polyethyleneimine and tetramethylammonium hydroxide; the organic solvent is at least one of absolute ethyl alcohol and acetone.
Preferably, in the step S1, high-entropy ceramic powder, a dispersing agent and an organic solvent are ball-milled and mixed on a roller ball mill, and ball milling is carried out for 1-10 hours at a rotating speed of 50-200 r/min, wherein the adopted grinding balls are silicon nitride, and the ball-to-material ratio is 1:1 to 4:1.
preferably, in step S2, the fuel particles are heated to 50 ℃ to 100 ℃ while being rolled; and spraying the slurry on the surfaces of the fuel particles by adopting an air pressure spraying device.
Preferably, in the step S3, the core biscuit is molded under the pressure of 10MPa to 100 MPa; the core-shell biscuit is molded under the pressure of 30MPa to 400 MPa.
Preferably, in the step S3, the diameter of the core biscuit is 6 mm-8 mm, and the height is 8 mm-24 mm;
the inner diameter of the core-shell biscuit is 6.2 mm-8.2 mm, the outer diameter is 8.5 mm-10 mm, and the height is 8-24 mm.
Preferably, in step S4, the sintering atmosphere is argon or vacuum.
The invention has the beneficial effects that: the high-entropy ceramic with high temperature resistance, high corrosion resistance and irradiation resistance is used as the matrix of the inert base dispersion fuel pellet, so that the characteristics of high thermal conductivity, low swelling, easy post-treatment, suitability for industrial production and the like of the pellet are realized; the nuclear fuel containment under the condition of the nuclear reactor cladding damage is improved, and the leakage of the nuclear fuel is prevented; improving the high temperature resistance of the nuclear fuel and promoting the application of the nuclear fuel in a high-temperature reactor.
The invention will be further described with reference to the accompanying drawings and examples, in which:
FIG. 1 is a schematic cross-sectional view of a high entropy ceramic inert matrix dispersion fuel pellet of the present invention.
For a clearer understanding of technical features, objects and effects of the present invention, a detailed description of embodiments of the present invention will be made with reference to the accompanying drawings.
As shown in FIG. 1, the high entropy ceramic inert matrix dispersion fuel pellet of the present invention comprises a columnar fuel zone 10 and a columnar fuel-free zone 20. The fuel zone 10 is disposed in the fuel-free zone 20 and the two are tightly coupled.
Wherein the fuel zone 10 comprises a high entropy ceramic matrix 11 and fuel particles 12 dispersed in the high entropy ceramic matrix 11. The high-entropy ceramic matrix 11 and the fuel-free area 20 are all made of high-entropy ceramic by sintering; the high-entropy ceramic comprises at least one of high-entropy carbide ceramic, high-entropy nitride ceramic, high-entropy oxide ceramic and high-entropy silicide ceramic. The high-entropy carbide ceramic comprises at least five of SiC, zrC, tiC, nbC, taC, VC, crC, moC and WC, the purity is 99-99.99%, and the proportion of the dosage of each is 1:1, a step of; the powder particle size of the high-entropy carbide ceramic is preferably 10nm to 200 mu m. High entropy nitride ceramicsThe porcelain comprises Si 3 N 4 At least five of ZrN, tiN, nbN, taN, VN, crN, moN and WN, the purity is 99-99.99%, and the proportion of the dosage of each is 1:1, a step of; the grain size of the high entropy nitride ceramics is 10 nm-200 mu m.
The fuel particles may include TRISO particles, UO 2 、UC、UC 2 、UN、UCN、UCO、U 3 Si 2 U alloy and PuO 2 At least one of PuC, puN, pu alloy. Wherein the core of the TRISO particles comprises UO 2 、UC、UC 2 、UN、UCN、UCO、U 3 Si 2 At least one of U alloy.
The high-entropy ceramic inert matrix dispersion fuel pellet is used for fuel rods, is arranged in cladding tubes of fuel plates and is arranged along the axial direction of the fuel rods.
Compared with the SiC inert base, the high-entropy ceramic matrix 11 has higher high-temperature resistance, corrosion resistance and irradiation resistance, can improve the high-temperature stability and the heat conductivity after irradiation of nuclear fuel, reduces the melting risk of the reactor core and improves the safety. After irradiation and at high temperature, the thermal conductivity of the high-entropy ceramic matrix 11 of the fuel can be maintained above 15W/mK. As the irradiation dose increases and the temperature increases, the swelling rate of the high-entropy ceramic matrix 11 of the fuel can be kept below 0.3%. In the post-treatment of spent fuel, wet or dry separation can be performed using strong acids or fluorine salts.
The preparation method of the high-entropy ceramic inert matrix dispersion fuel pellet can comprise the following steps:
s1, mixing high-entropy ceramic powder with a dispersing agent and an organic solvent to form slurry; and (3) drying a part of the slurry to form mixed powder, or mixing the high-entropy ceramic powder with a dispersing agent to form mixed powder.
Specifically, high-entropy ceramic powder, a dispersing agent and an organic solvent are subjected to ball milling and mixing on a roller ball mill, and ball milling is carried out for 1-10 hours at a rotating speed of 50-200 r/min, wherein the adopted grinding balls are silicon nitride, and the ball-to-material ratio (the mass ratio of the grinding balls to the mixed materials) is 1:1 to 4:1.
in the slurry, the mass ratio of the organic solvent to the high-entropy ceramic powder is 1:1 to 3:1.
the dispersing agent accounts for 0.5 to 4 percent of the mass of the high-entropy ceramic powder.
The high-entropy ceramic powder comprises at least one of high-entropy carbide ceramic powder, high-entropy nitride ceramic powder, high-entropy oxide ceramic powder and high-entropy silicide ceramic powder. The high-entropy carbide ceramic powder comprises at least five of ZrC, tiC, nbC, taC, VC, crC, moC with purity of 99-99.99%, and the proportion of the dosage of each is 1:1, a step of; the grain size of the carbide ceramic powder is 10 nm-200 mu m. The high entropy nitride ceramic powder comprises Si 3 N 4 At least five of ZrN, tiN, nbN, taN, VN, crN, moN and WN, the purity is 99-99.99%, and the proportion of the dosage of each is 1:1, a step of; the grain diameter of the high entropy nitride ceramic powder is 10 nm-200 mu m.
The dispersing agent is at least one of polyethyleneimine and tetramethyl ammonium hydroxide. The organic solvent is at least one of absolute ethyl alcohol and acetone.
S2, spraying the slurry on the surfaces of the rolling fuel particles by adopting an air pressure spraying device, and drying to form a coating layer adhered to the surfaces of the fuel particles.
The fuel particles are heated to 50-100 ℃ while rolling.
Wherein the fuel particles may comprise TRISO particles, UO 2 、UC、UC 2 、UN、UCN、UCO、U 3 Si 2 U alloy and PuO 2 At least one of PuC, puN, pu alloy. The core of TRISO particles comprises UO 2 、UC、UC 2 、UN、UCN、UCO、U 3 Si 2 At least one of U alloy.
S3, mixing a part of mixed powder with fuel particles with a coating layer according to a proportion, and pressing to form a columnar core biscuit; pressing the other part of mixed powder to form a cylindrical core-shell biscuit.
The core biscuit is molded under the pressure of 10MPa to 100 MPa. The diameter of the core biscuit is 6 mm-8 mm, and the height is 8 mm-24 mm.
The core-shell biscuit is molded under the pressure of 30MPa to 400 MPa. The inner diameter of the core-shell biscuit is 6.2 mm-8.2 mm, the outer diameter is 8.5 mm-10 mm, and the height is 8 mm-24 mm.
S4, filling the core biscuit into the core-shell biscuit, and carrying out pressurized or pressureless sintering at the sintering temperature of 1600-1950 ℃ to form a densified high-entropy ceramic inert matrix dispersion fuel pellet, wherein the density is higher than 92%.
During sintering, the sintering atmosphere is argon or vacuum. And preserving the temperature for 0.5-5 h after sintering.
Referring to fig. 1, a high entropy ceramic inert matrix dispersion fuel pellet is produced in which a fuel zone 10 is formed from a core green body and a fuel-free zone 20 is formed from a core-shell green body.
The invention is further illustrated by the following examples.
Example 1
ZrC, tiC, nbC, taC and MoC are used as raw material powder, the purity of the powder is 99.9%, the particle size is 20nm, and the proportion of the powder is 1:1:1:1:1, a step of; the polyethyleneimine is taken as a dispersing agent, the content of polyethyleneimine is 2wt% of the raw material powder, absolute ethyl alcohol is taken as an organic solvent, and the mass of the organic solvent and the comprehensive proportion of the raw material powder and the dispersing agent are 2:1. mixing in a roller ball mill according to the proportion, wherein the grinding balls are silicon nitride, the revolution is 100r/min, the ball milling time is 12h, the slurry is prepared after ball milling, and part of the slurry is subjected to rotary evaporation and drying to prepare mixed powder.
Heating TRISO particles to 90 ℃ in a rolling state, coating the slurry on the TRISO particles through spray deposition, removing an organic solvent from the TRISO particles subjected to coating at the temperature of 90 ℃ to obtain TRISO particles subjected to coating (i.e. a coating layer), and then carrying out dry pressing on the TRISO particles subjected to coating and the prepared mixed powder at the proportion content of 40wt%, wherein the mechanical pressing pressure is 100MPa, and the cylindrical core biscuit with the diameter of 8mm and the height of 8mm is obtained through pressing.
Pressing the mixed powder without TRISO particles into a core-shell biscuit with the inner diameter of 8.2mm, the outer diameter of 10mm and the height of 8mm under the pressure of 80MPa, and loading the core-shell biscuit into the core-shell biscuit; heating to 1900 ℃ at 20 ℃/min in a pressureless furnace, preserving heat for 1h, and obtaining the high-entropy inert base dispersion fuel (IMDP) with the sintering atmosphere of Ar, wherein the density of the high-entropy ceramic matrix reaches 96%.
The resulting high entropy inert based dispersion fuel structure is shown in FIG. 1. Wherein TRISO particles 12 are dispersed in an inert-based nuclear fuel core (i.e., in the high-entropy ceramic matrix 11 of the fuel zone 10), and the edge fuel-free zone 20 further prevents leakage of nuclear fuel due to TRISO particle breakage. The IMDP fuel pellets are filled into cladding tubes to complete assembly, and the assembled and sealed cladding can be used for high-temperature gas cooled piles, rock melting piles and other pile types.
Example 2
ZrC, crC, nbC, taC and MoC powder were mixed according to 1:1:1:1:1 proportion is used as raw material powder, the purity of the powder is 99.99 percent, the grain diameter is 100nm, a core-shell biscuit and a core biscuit are respectively prepared according to the method of the embodiment 1, and the core biscuit is molded under the pressure of 50MPa, and the size is 7mm in diameter and 10mm in height; the core-shell biscuit is pressed and formed under the pressure of 200MPa, and the inner diameter is 7.2mm, the outer diameter is 9mm and the height is 10mm. The core-shell biscuit is sintered in a pressureless furnace after being filled into the core-shell biscuit, the temperature is raised to 1800 ℃ at the heating rate of 15 ℃/min, the heat preservation time is 2 hours, the sintering atmosphere is vacuum, and the density of the high-entropy inert base dispersion fuel prepared by sintering is 98%.
Example 3
ZrC, crC, nbC, VC, taC and MoC powder were mixed according to 1:1:1:1:1:1 proportion is used as raw material powder, the purity of the powder is 99.99 percent, the grain diameter is 100 mu m, a core-shell biscuit and a core biscuit are respectively prepared according to the method of the embodiment 1, and the core biscuit is molded under the pressure of 100MPa, and the size is 8mm in diameter and 20mm in height; the core-shell biscuit is pressed and formed under 400MPa, and the inner diameter is 8.2mm, the outer diameter is 10mm and the height is 20mm. The core-shell biscuit is sintered in a pressureless furnace after being filled into the core-shell biscuit, the temperature is raised to 1950 ℃ at a heating rate of 5 ℃/min, the heat preservation time is 4 hours, the sintering atmosphere is vacuum, and the density of the high-entropy inert base dispersion fuel prepared by sintering is 97%.
Example 4
ZrC, tiC, nbC, taC and MoC powder were mixed according to 1:1:1:1:1 proportion is used as raw material powder, the purity of the powder is 99.99 percent, the grain diameter is 50nm, a core-shell biscuit and a core biscuit are respectively prepared according to the method of the embodiment 1, and the core biscuit is molded under the pressure of 10MPa, and the size is 8mm in diameter and 24mm in height; the core-shell biscuit is pressed and formed under the pressure of 300MPa, and the inner diameter is 8.2mm, the outer diameter is 10mm and the height is 24mm. The core-shell biscuit is sintered in a pressureless furnace after being filled into the core-shell biscuit, the temperature is raised to 1850 ℃ at the heating rate of 10 ℃/min, the heat preservation time is 1h, the sintering atmosphere is vacuum, and the density of the high-entropy inert base dispersion fuel prepared by sintering is 98%.
Example 5
ZrC, crC, nbC, taC and VC powder are mixed according to the following ratio of 1:1:1:1:1 proportion is used as raw material powder, the purity of the powder is 99.99 percent, the grain diameter is 200 mu m, a core-shell biscuit and a core biscuit are respectively prepared according to the method of the embodiment 1, and the core biscuit is molded under the pressure of 100MPa, and the size is 6mm in diameter and 8mm in height; the core-shell biscuit is pressed and formed under 400MPa, and has an inner diameter of 6.2mm, an outer diameter of 8mm and a height of 8mm. The core-shell biscuit is sintered in a pressureless furnace after being filled into the core-shell biscuit, the temperature is raised to 1950 ℃ at the heating rate of 10 ℃/min, the heat preservation time is 5 hours, the sintering atmosphere is vacuum, and the density of the high-entropy inert base dispersion fuel prepared by sintering is 94%.
The foregoing description is only illustrative of the present invention and is not intended to limit the scope of the invention, and all equivalent structures or equivalent processes or direct or indirect application in other related technical fields are included in the scope of the present invention.
Claims (17)
- The high-entropy ceramic inert matrix dispersion fuel pellet is characterized by comprising a cylindrical fuel-free zone and a fuel zone of a cylinder arranged in the fuel-free zone; the fuel zone comprises a high-entropy ceramic matrix and fuel particles dispersed in the high-entropy ceramic matrix; the high-entropy ceramic matrix and the fuel-free area are both manufactured by sintering high-entropy ceramic.
- The high entropy ceramic inert matrix dispersion fuel pellet of claim 1, wherein the high entropy ceramic comprises at least one of a high entropy carbide ceramic, a high entropy nitride ceramic, a high entropy oxide ceramic, and a high entropy silicide ceramic.
- The high entropy ceramic inert matrix dispersion fuel pellet of claim 2, wherein the high entropy carbide ceramic comprises at least five of SiC, zrC, tiC, nbC, taC, VC, crC, moC and WC; the grain diameter of the powder of the high-entropy carbide ceramic is 10 nm-200 mu m.
- The high entropy ceramic inert matrix dispersion fuel pellet of claim 2, wherein the high entropy nitride ceramic comprises Si 3 N 4 At least five of ZrN, tiN, nbN, taN, VN, crN, moN, WN; the grain size of the powder of the high-entropy nitride ceramic is 10 nm-200 mu m.
- The high entropy ceramic inert matrix dispersion fuel pellet of claim 1, wherein the fuel particles comprise TRISO particles, UO 2 、UC、UC 2 、UN、UCN、UCO、U 3 Si 2 U alloy and PuO 2 At least one of PuC, puN, pu alloy.
- The high entropy ceramic inert matrix dispersion fuel pellet of claim 5, wherein the core of TRISO particles comprises UO 2 、UC、UC 2 、UN、UCN、UCO、U 3 Si 2 At least one of U alloy.
- The preparation method of the high-entropy ceramic inert matrix dispersion fuel pellet is characterized by comprising the following steps of:s1, mixing high-entropy ceramic powder with a dispersing agent and an organic solvent to form slurry;a part of slurry is dried to form mixed powder, or the high-entropy ceramic powder is mixed with a dispersing agent to form mixed powder;s2, spraying the slurry on the surfaces of rolling fuel particles, and drying to form a coating layer adhered to the surfaces of the fuel particles;s3, mixing a part of the mixed powder with fuel particles with a coating layer according to a proportion, and pressing to form a columnar core biscuit; pressing the other part of the mixed powder to form a cylindrical core-shell biscuit;and S4, filling the core biscuit into the core-shell biscuit, and carrying out pressurized or pressureless sintering at the sintering temperature of 1600-1950 ℃ to form a densified high-entropy ceramic inert matrix dispersion fuel pellet.
- The method for preparing a high-entropy ceramic inert matrix dispersion fuel pellet according to claim 7, wherein the high-entropy ceramic powder comprises at least one of high-entropy carbide ceramic powder, high-entropy nitride ceramic powder, high-entropy oxide ceramic powder and high-entropy silicide ceramic powder.
- The method for preparing the high-entropy ceramic inert matrix dispersion fuel pellet according to claim 8, wherein the high-entropy carbide ceramic powder comprises at least five of SiC, zrC, tiC, nbC, taC, VC, crC, moC and WC, and has a particle size of 10 nm-200 μm;the high-entropy nitride ceramic powder comprises Si 3 N 4 At least five of ZrN, tiN, nbN, taN, VN, crN, moN, WN, the grain diameter is 10 nm-200 μm.
- The method for preparing high-entropy ceramic inert matrix dispersion fuel pellets according to claim 7, wherein the combustion is performed byThe material particles comprise TRISO particles and UO 2 、UC、UC 2 、UN、UCN、UCO、U 3 Si 2 U alloy and PuO 2 At least one of PuC, puN, pu alloy;the core of the TRISO particles comprises UO 2 、UC、UC 2 、UN、UCN、UCO、U 3 Si 2 At least one of U alloy.
- The method for preparing the high-entropy ceramic inert matrix dispersion fuel pellet according to claim 7, wherein a mass ratio of the organic solvent to the high-entropy ceramic powder in the slurry is 1:1 to 3:1, a step of; the dispersing agent accounts for 0.5-4% of the high-entropy ceramic powder by mass.
- The method for preparing the high-entropy ceramic inert matrix dispersion fuel pellets according to claim 7, wherein the dispersing agent is at least one of polyethylenimine and tetramethylammonium hydroxide; the organic solvent is at least one of absolute ethyl alcohol and acetone.
- The method for preparing the high-entropy ceramic inert matrix dispersion fuel pellet as claimed in claim 7, wherein in the step S1, high-entropy ceramic powder, a dispersing agent and an organic solvent are ball-milled and mixed on a roller ball mill, ball milling is carried out for 1-10 h at a rotating speed of 50-200 r/min, the adopted grinding balls are silicon nitride, and the ball-to-material ratio is 1:1 to 4:1.
- the method for preparing high-entropy ceramic inert matrix dispersion fuel pellets according to claim 7, wherein in step S2, the fuel particles are heated to 50 ℃ to 100 ℃ while rolling; and spraying the slurry on the surfaces of the fuel particles by adopting an air pressure spraying device.
- The method for preparing high-entropy ceramic inert matrix dispersion fuel pellets according to claim 7, wherein in step S3, the core green body is molded under a pressure of 10MPa to 100 MPa; the core-shell biscuit is molded under the pressure of 30MPa to 400 MPa.
- The method for preparing high-entropy ceramic inert matrix dispersion fuel pellets according to claim 7, wherein in step S3, the diameter of the core biscuit is 6 mm-8 mm, and the height is 8 mm-24 mm;the inner diameter of the core-shell biscuit is 6.2 mm-8.2 mm, the outer diameter is 8.5 mm-10 mm, and the height is 8 mm-24 mm.
- The method for preparing high-entropy ceramic inert matrix dispersion fuel pellets according to claim 7, wherein in step S4, the sintering atmosphere is argon or vacuum.
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